EPA-600/2-78-024
March 1978
               Environmental Protection Technology Series
       SORBENTS
   FOR FLUORIDE,  METAL FINISHING,
AND  PETROLEUM SLUDGE  LEACHATE
              CONTAMINANT  CONTROL
                                Municipal Environmental Research Laboratory
                                      Office of Research and Development
                                     U.S. Environmental Protection Agency
                                             Cincinnati, Ohio 45268

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                                              EPA-600/2-78-024
                                              March  1978
SORBENTS FOR FLUORIDE, METAL FINISHING, AND PETROLEUM SLUDGE
                LEACHATE CONTAMINANT CONTROL
                             by
                        Paul  C. Chan
                      Robert Dresnack
                     John W.  Liskowitz
                        Angelo Perna
                      Richard Trattner
             New Jersey Institute of Technology
                 Newark, New Jersey  07102
                     Grant No.  R803717
                     Project Officer

                     Fred Ellerbusch
           Industrial  Pollution Control  Division
        Industrial  Environmental  Research Laboratory
                  Cincinnati, Ohio  45268
       MUNICIPAL ENVIRONMENTAL RESEARCH LABORATORY
            OFFICE OF RESEARCH AND DEVELOPMENT
           U.S.  ENVIRONMENTAL PROTECTION AGENCY
                 CINCINNATI,  OHIO  45268

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                                 DISCLAIMER

     This report has been reviewed by the Municipal Environmental Research
Laboratory, U.S. Environmental Protection Agency, and approved for publica-
tion.  Approval does not signify that the contents necessarily reflect the
views and policies of the U.S. Environmental Protection Agency, nor does
mention of trade names or commercial products constitute endorsement or
recommendation for use.
                                     ii

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                                   FOREWORD

     The Environmental Protection Agency was created because of increasing
public and government concern about the dangers of pollution to the health and
welfare of the American people.  Noxious air, foul water, and spoiled land are
tragic testimony to the deterioration of our natural environment.   The complex-
ity of that environment and the interplay between its components require a
concentrated and integrated attack on the problem.

     Research and development is that necessary first step in problem solution,
and it involves defining the problem, measuring its impact, and searching for
solutions.  The Municipal Environmental Research Laboratory develops new and
improved technology and systems for preventing, treating, and managing waste-
water and solid and hazardous waste pollutant discharges from municipal and
community sources, for preserving and treating public drinking water supplies,
and for minimizing the adverse economic, social, health, and aesthetic effects
of pollution.  This publication is one of the products of that research, a
most vital communication link between the researcher and the user community.

     This report deals with the investigation of leachate contaminant control
using sorbents.  Ashes, clays, and refined materials were tested to determine
their capacity to remove leachate contaminants produced from three industrial
sludges—calcium fluoride, metal hydroxide, and petroleum.  The report will
provide data to government and industry alike contemplating residue leachate
control from industrial sludge impoundment via sorbent contact.
                                       Francis T. Mayo
                                       Director
                                       Municipal Environmental
                                         Research Laboratory
                                     iii

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                                  ABSTRACT

      A  laboratory  evaluation of bottom ash, acidic and basic fly ashes, vermi-
 culite,  illite,  activated  carbon, kaolinite, natural zeolite, activated alumi-
 na,  and  cullite  for  the  removal of contaminants in the leachate and liquid
 portion  of  three industrial sludges  (calcium fluoride, metal finishing, and
 petroleum)  is  presented.   Batch and  lysimeter studies were carried out to
 evaluate the static  and  dynamic sorbent capacity for the constituents present
 in the  leachate.   Also,  permeability exhibited by these sorbents when con-
 tacted with the  above  industrial sludge leachate was studied.  The pH, con-
 ductivity,  chemical  oxygen demand (COD), total organic carbon (TOC), cationic
 and  anionic species  in the leachate  before and after contact with the sorbent
 materials,  and the coefficient of permeability were determined.

      The analysis  of the leachate showed that considerable variations exist in
 composition and  concentration of constituents in the leachate prepared from
 the  same industrial  sludge, which was collected over the period of this inves-
 tigation.  The results of the batch and lysimeter studies reveal that no
 single sorbent,  but  combinations of  two, three, or four sorbents, can be used
 to reduce the concentration of the constituents found in the leachate of a
 specific sludge.   These are acidic and basic fly ashes, kaolinite, and illite
 for  the  calcium  fluoride sludge leachate; verrniculite, kaolinite, and illite
 for  the  metal finishing sludge leachate; basic fly ash, vermiculite, and kao-
 linite for the petroleum sludge leachate.  The combination of the more expen-
 sive  activated carbon and activated alumina was found to be the more effective
 combination for  treating the calcium fluoride sludge leachate but less effec-
 tive  than the ash  and clay combinations in treating the metal finishing sludge
 leachate and petroleum sludge leachate.  The selection of a sorbent combina-
 tion  is  sludge leachate specific.   In some cases, the most effective sorbents
 for the  remoyal  of the same contaminant in the leachate from different sludges
 are not  the same.  Also, significantly greater sorbent capacities for the
 measured contaminants in the leachates are achieved by the sorbents under
 dynamic  conditions than are achieved under static conditions.  In addition,
 change in pH of  the  sorbent from acidic to alkaline, such as resulted when
 alkaline fluoride  sludge leachate and metal finishing sludge leachate were
 passed through the acidic fly ash and illite, was found to favor the removal
 of cations.

     This report was submitted in fulfillment of grant No. R803717 by New
Jersey Institute of Technology under partial sponsorship of the U.S. Environ-
mental Protection Agency.  This report covers the initial laboratory studies
carried out to identify the most promising sorbents that may be used to
 significantly reduce the concentration of measurable contaminant in calcium
fluoride sludge leachate, metal finishing sludge leachate, and petroleum
 sludge leachate.  The  study  covers the period  from June  1975  to May  1977.


                                     iv

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                                CONTENTS

Foreword	   in
Abstract	     iv
Figures	     yi
Tables	viii
Acknowledgment	     ix

   1.  Introduction 	      1
   2.  Conclusions	      4
   3.  Recommendations	      7
   4.  Materials Description	      9
            Sorbents	      9
            Sludge sources	     11
   5.  Experimental Procedures	     13
            Preparation of sorbent materials	     13
            Preparation of background leachates  from sorbents  ...     13
            Preparation of sludge leachates  	     13
            Static studies	     14
            Dynamic studies 	     14
            Analytical procedures 	     16
            Permeability studies	     17
            Grain size determination	     17
   6.  Results and Discussion	     20
            Results of static studies 	     20
            Results of lysimeter studies	     36

References	     82

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                                   FIGURES

Number                                                                  Page

   1     Laboratory arrangement  of lysimeters	  15

   2     Grain-size distribution of sorbents	  19

   3     Lysimeter studies  of pH in calcium  fluoride sludge leachate	  38

   4     Lysimeter studies  of calcium  ion  in> calcium fluoride sludge
          1 eachate	  40

   5     Lysimeter studies  of copper ion in  calcium fluoride sludge
          leachate	  42

   6     Lysimeter studies  of magnesium ion  in calcium fluoride
          sludge leachate	  44

   7     Lysimeter studies  of fluoride ion in calcium fluoride
          sludge leachate	  45

   8     Lysimeter studies  of COD in calcium fluoride sludge leachate....  47

   9     Lysimeter studies  of TOC in calcium fluoride sludge leachate	  48

  10     Permeability studies of sorbent materials with calcium
          f 1 uoride si udge  1 eachate	  51

  11     Lysimeter studies  of pH in metal  finishing sludge leachate	  52

  12     Lysimeter studies  of calcium  ion  in  metal finishing sludge
          1 eachate	  55

  13     Lysimeter studies  of copper ion in  metal finishing sludge
          1 eachate	  57

  14     Lysimeter studies  of magnesium ion  in metal finishing
          sludge leachate	  58

  15     Lysimeter studies  of nickel ion in  metal finishing sludge
          leachate	  60

  16     Lysimeter studies  of fluoride ion in metal finishing sludge
          1 eachate	  61
                                    VI

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Number                                                                  Page
  17    Lysimeter studies  of COD  in  metal  finishing sludge leachate	  62
  18    Lysimeter studies  of TOC  in  metal  finishing sludge leachate	  63
  19    Permeability studies of activated  carbon  	  64
  20    Permeability studies of sorbent  materials with metal
          finishing sludge leachate	  66
  21    Lysimeter studies  of pH in petroleum  sludge leachate	  68
  22    Lysimeter studies  of calcium ion in petroleum sludge
          1 eachate	  69
  23    Lysimeter studies  of copper  ion  in petroleum sludge leachate	  71
  24    Lysimeter studies  of magnesium ion in petroleum  sludge
          1 eachate	  73
  25    Lysimeter studies  of zinc ion in petroleum sludge leachate	  74
  26    Lysimeter studies  of fluoride ion  in  petroleum sludge
          1 eachate	  75
  27    Lysimeter studies  of cyanide ion in petroleum sludge
          1 eachate	  77
  28    Lysimeter studies  of COD  in  petroleum sludge leachate	  78
  29    Lysimeter studies  of TOC  in  petroleum sludge leachate	  79
  30    Permeability studies of sorbent materials with petroleum
          sludge leachate	  80
                                    vii

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                                    TABLES
Number                                                                   Page
   1     Static Study Results of Calcium Fluoride Sludge Leachate #1	   22
   2     Static Study Results of Calcium Fluoride Sludge Leachate #2	   23
   3     Static Study Results of Calcium Fluoride Sludge Leachate #3	   24
   4     Comparisons of Sorbent Capacities in Static and Lysimeter
          Tests (Calcium Fluoride Sludge Leachate)	   25
   5     Static Study Results of Metal  Finishing Sludge Leachate #1	   28
   6     Static Study Results of Metal  Finishing Sludge Leachate #2	   29
   7     Static Study Results of Metal  Finishing Sludge Leachate #3	   30
   8     Comparisons of Sorbent Capacities in Static and Lysimeter Tests
          (Metal  Finishing Sludge Leachate)	   31
   9     Static Study Results of Tank Bottom  Petroleum Sludge Leachate...   33
  10     Static Study Results for API Separator Petroleum Sludge
          Leachate	   34
  11     Comparisons of Sorbent Capacities in Static  and
          Lysimeter Tests  (Petroleum SIudge  Leachate)	   35
  12     Permeability Characteristics of Sorbent Materials	   54
                                    vi i i

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                               ACKNOWLEDGMENTS

     The authors are deeply indebted to Fred  Ellerbusch,  Sanitary  Engineer,
Industrial  Environmental  Research Laboratory, U.S.  Environmental Protection
Agency, Cincinnati, Ohio, for his guidance in this  project.

     We would further like to express our thanks  to the following  companies
for their cooperation in  supplying the sorbents  used in this  study:   Georgia
Kaolin Company, Elizabeth, New Jersey (kaolinite);  Double Eagle  Petroleum
and Mining Company, Casper, Wyoming (zeolite); Culligan International  Company,
Northbrook, Illinois (cullite); Public Service Electric & Gas Company, Hudson
Generating Station, Jersey City, New Jersey (fly  ash and  bottom  ash);  Alcoa,
Bauxite, Arkansas (activated alumina).  In addition, we thank the  Exxon Corpor-
ation, Linden, New Jersey, and Hoffman-LaRoche Corporation,  Nutley,  New Jersey,
for their assistance with the initial analysis of the leachates.

     We appreciate the efforts of Mung Shium Sheih, Richard  Trayer,  and Tak
Hoi Lee, graduate students in the Institute,  for their efforts in  conducting
the various experiments.   In particular, we thank Mr. Sheih  for  his  contribu-
tions in various phases of this project.

     The authors are especially appreciative of  Irene Mitchell and Diana Mul-
drow for their patience and skillful typing of  the entire manuscript.
                                      IX

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                                  SECTION  1

                                 INTRODUCTION


     As a result of the establishment under  the Federal  Water Pollution Con-
trol  Act of 1972 of a nonpollutant discharge policy to receiving waters by
1985, industry will be faced with finding  feasible techniques for  the  safe
disposal of hazardous and toxic sludges generated during the  treatment of
their waste streams.  Some progress has been made in the development of clos-
ed-loop type waste treatment.  However, this technology is  not expected to
significantly reduce the sludge volume in  the near future.  Currently, the
most often used sludge disposal technique  for industrial sludges  is the "sani-
tary" landfill.  Moreover, the disposal of industrial  sludge  in landfills can
lead to contamination of ground and surface  waters through  runoff and  percola-
tion.  Present-day sanitary landfills cannot be considered  a  panacea for  the
ultimate disposal of hazardous wastes.

     At present, means to accurately predict the leaching potential, direction
and rate of flow of the leachate through the soil surrounding the landfill
site is lacking.  These problems could be overcome by isolating the  landfill
site from its immediate soil surroundings.  By lining the base and sides  of
the landfill with compacted soil of low impermeablity, horizontal  groundwater
movement of the leachate is prevented.  Polyvinyl chloride and butyl  rubber
liners have also been used for this purpose.  This liner creates a "tub with-
out a drain" unless the rainwater that percolates down through the landfill is
provided a route of escape.  This could be accomplished by using gravity  out-
lets, such as drainage tiles, or perforated corrugated metal  pipe, installed
in the lowest portion or along the base of the landfill to remove and  collect
the leachate.  Further treatment of the collected leachate would be required
to reduce the pollutants to acceptable discharge levels, assuming that treat-
ment technology is available.  In any event, additional construction  and
operating costs would be required.

     It is the intent of this study to establish a design approach for the
removal of leachate components at the landfill site using relatively inexpen-
sive natural clays and other sorbents such as fly ash and bottom ash.

     This report deals with the results of a laboratory study which has  been
conducted to evaluate the effectiveness for contaminent removal of ten natural
and synthetic sorbent materials on the liquid portion and leachate generated
from three different industrial sludges.

     The sorbent materials that were  used were fly ash, bottom ash, illite,
kaolinite, vermiculite, natural zeolite, Ottawa  sand, cullite, activated car-
bon and activated  alumina.  Activated carbon and activated alumina were

                                       1

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 included in  this  study  even  though  they  are far more expensive than the other
 sorbents because  they are  generally known  to be effective sorbents for the
 removal  of organics,  cations  and  anions  from waste streams.  Their use may be
 warranted if the  above  inexpensive  sorbents are not effective in removing a
 specific component  from the  leachate.  Cullite, which is a synthetic zeolite,
 was  examined because  it is widely used in  water softening applications.
 Ottawa  sand  is  included because it  is mixed with some of the naturally occur-
 ring sorbents to  improve their permeabilities.  It was found in our prelimi-
 nary work prior to  this study to  be relatively inert to the experiments.

      Studies exploring  possible application of fly ash in this area of waste-
 water treatment have  been  investigated by  a number of investigators.  Deb
 et al.  (1) and  Nelson and Guarino (2} reported the use of fly ash for the re-
 moval of COD from wastewater.  They concluded that the unwashed fly ash added
 appreciable  COD but not BOD to the  solution.  Ballance et al. (3) investigated
 fly  ash  as a coagulant  aid in water treatment, reporting that fly ash has cer-
 tain properties which enhanced chemical  coagulation and settling of turbid
 water.

      Soil  chemists  have shown an  interest  in ion removal by clay soils for
 many years.  For a  complete discussion of  chemical reaction and clay mineral
 structures,  the reader  is referred  to standard works—for instance, Grim
 (4)  and  Brown (5).  Investigations  have  dealt, however, in the main, with
 selected  ions,  e.g., phosphorous  adsorption by Fried and Shapiro (6), Olson
 and  Watanable (7),  Ellis and Erickson (8), zinc adsorption by Tiller (9), and
 Sharpless, Wallihan, and Peterson (10).  For ion removal, Bittell and Miller
 (11)  investigated the removal of  lead, cadmium, and calcium by montmorillonite,
 illite,  and  kaolinite.   They found  that  the cations exhibited consistent pre-
 ferential  sorption  characteristics  for the three clays.  Calcium and cadmium
 competed  evenly, while  lead showed  favorable sorption over calcium by a factor
 of 2  to  3.   Recently, several investigators have examined the effectiveness of
 kaolinite, illite,  montmorillonite,  and  soil mixtures in removing pollutants
 such  as  heavy metals and organic  compounds.  Fuller et al. (12) examined
 eleven soil  mixtures, ranging from  sandy loam to clay mixtures, mixing with
 limestone  and hydrated  Fe2$04, for  developing a sanitary landfill liner.  Pre-
 liminary  results indicated both limestone  and dehydrated FepS04 nad a signifi-
 cant  retarding  influence on migration rate of the cations and anions studied.
 Another  investigation by Griffin et  al.  (13) examined the effect of pH on
 removal  of heavy metals  by kaolinite and montmorillonite.  They concluded
 that  both cationic  and  anionic adsorption  on these two clays were pH depen-
 dent.  Ihe adsorption of the cations was increased as the pH was raised.

      The above investigations, however, examined the effectiveness of clays
 for removing specific contaminant(s) from  leachates that were synthesized or
modified  in  the laboratory.  Early  laboratory work (14) on the chemical and
 physical reactions  of radioactive liquid waste with soils indicated that the
 removal  of radioisotopes from solutions by exchange with the soil is influ-
enced by the concentration of other  cations in solutions as well  as the total
 salt concentration.   These results  indicate that the composition of a leachate
could influence the removal of a specific  contaminant using a given sorbent.
Therefore, our studies were carried  out using leachates prepared directly from
the industrial sludges without modification to achieve a more realistic eval-

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uation of the sorbents for contaminant removal.

     The sludges chosen for this study were a calcium fluoride sludge (of the
type generated by the electronic and aircraft industries), a metal  finishing
sludge, and a petroleum sludge.  These sludges were selected because their
annual production is of a significant magnitude to present disposal problems.
Also, the leachate from these sludges contains a cross-section of hazardous
organic constituents, heavy metal hydroxides, anions such as cyanide, and sub-
stantial amounts of fairly soluble toxic salts such as calcium fluoride.
Analysis of the leachate generated from these sludges involved the determina-
tion of pH, conductivity, chemical oxygen demand (COD), total organic carbon
(TOC), anionic species, and cationic species, before and after contact with
sorbent materials.

     Static studies were initially conducted to evaluate the capacity of these
sorbent materials, using leachate with the maximum concentrations of contami-
nants that could be obtained from the sludge.  These studies were carried out
to define the most promising sorbent materials for removal of the constituents
in the sludge leachate.  The static studies were then followed by lysimeter
studies using the most promising sorbent materials to obtain information re-
garding the dynamic capacity and permeability characteristics of these mate-
rials.

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                                  SECTION 2

                                 CONCLUSIONS


     A number of sorbents have been identified as exhibiting a removal  capa-
city for leachate constituents under flowing conditions from the three  types
of sludges investigated.  No single sorbent material  was found to be effective
in removing all the objectionable ions from the leachates studied.   Two,
three, or four different sorbents could be collectively combined to reduce
sludge leachate contaminant levels. The combination of acidic  fly ash,  kaolinite,
illite and basic fly ash, respectively, in a layer system may be used for
treating the calcium fluoride sludge leachate under flowing conditions.  The
acidic and basic fly ashes are effective in reducing  the magnesium and  the
organics whereas kaolinite and illite are effective for the calcium, kaolinite
for copper and illite and kaolinite for fluoride based upon a comparison  of
their sorbent capacities.  The basic fly ash is recommended, even though  it is
not as effective as the acidic fly ash, for removal  of copper and magnesium
because it can retain the copper and magnesium ions that are initially  leached
from the acidic fly ash.  This leaching occurs until  the effluent from  the
acidic fly ash lysimeter becomes basic as a result of prolonged passage of the
alkaline fluoride sludge leachate through the column.

     Based upon a comparison of all sorbent capacities, the combined use  of
the relatively expensive sorbents, activated alumina  and activated  carbon,
may be more effective in reducing the above cations,  anions, and organics in
the calcium fluoride sludge leachate than the inexpensive ashes and clays.
The activated alumina reduces the levels of the calcium, copper, magnesium and
fluoride and the activated carbon is effective in reducing the organic  concen-
trations.  However, the usefulness of the activated alumina for treating  this
leachate is limited by the marked reduction observed  in its permeability  as
the calcium fluoride sludge leachate flows through this sorbent.  A point can
be reached where the activated alumina is impermeable to the flow of this
sludge leachate.

     The combination of illite, kaolinite, and vermiculite, respectively, in
a layered system may be used to treat the metal finishing sludge leachate
under flowing conditions.  Illite and vermiculite are effective for reducing
the concentrations of calcium, copper, magnesium, nickel, and the organics.
Vermiculite, although not as effective as the illite, is used to retain the
calcium and copper ions which are initially leached from the illite. This
occurs until the illite becomes alkaline due to prolonged passage of the  alka-
line metal  finishing sludge leachate through this sorbent.  The kaolinite is
effective for reducing the fluoride ion levels in this leachate.

     The combination of the activated alumina and activated carbon  can  also be

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used to treat the metal  finishing sludge  leachate.   The activated alumina is
found to be effective in reducing the calcium,  magnesium and  fluoride ions, and
the activated carbon is  effective in  reducing the  copper,  nickel and organics.
However, the clay sorbent combination, rather than the more expensive activa-
ted alumina and activated carbon combination, is more effective  in reducing
the contaminant levels measured in this leachate.

     The combination of  basic fly ash, vermiculite, and kaolinite may be used
to reduce the measurable contaminants present in the petroleum sludge lea-
chate.  Basic fly ash is effective in reducing  the copper  and the fluoride ion
concentrations based upon an examination  of the sorbent capacities.  Vermicu-
lite is effective for the calcium, zinc,  cyanide and the organics, and  kaoli-
nite is effective for the magnesium ions.   The  combination of activated alumi-
na and activated carbon  can again be  used to reduce the measurable contami-
nants in the petroleum sludge leachate.  The activated alumina is effective
for the calcium, copper, magnesium, and fluoride ions, and the activated carbon
is effective for the zinc and cyanide ions as well as the  organics.  However,
their sorbent capacities, as was the  case for the  metal finishing sludge lea-
chate, are again significantly lower  than the ash  and clay sorbent combina-
tions.

     In summary, the removal of organics  from the  calcium  fluoride leachate  is
best accomplished by the use of activated carbon.   However, with regard to the
metal finishing and petroleum sludge  leachates, illite and vermiculite, res-
pectively, are the most  effective for treating  the organics.

     The behavior of a sorbent with regard to the  removal  of  a particular  con-
taminant  varies with the type of leachate being  treated.   This  effect  may
result from the competitive ion exchange and sorption  processes  which exist
among the constituents of a leachate  and the sorbent and  cannot  be easily  pre-
dicted on the basis of results obtained from the  use of  synthetically consti-
tuted leachate.  This latter point serves to emphasize  the choice of an actual
industrial sludge leachate rather than a synthetically  constituted  leachate  if
one wishes to draw predictive conclusions regarding the  effectiveness of  sor-
bents in reducing the contaminants in an industrial sludge leachate.

     The experimental conditions, a 2.5 gram of concentrated  leachate mixed
with 1 gram of sorbent for 24 hours,  did not provide results  that were  in
agreement with some of the results obtained under flowing conditions but were
useful in indicating promising sorbents.   In general,  the sorption capacities
exhibited by a sorbent for a specific constituent in a  leachate, under  flowing
condition, was significantly higher than that achieved  under  non-flowing  con-
ditions.  In some cases  no removal of specific  constituents  by a sorbent was
observed under non-flowing conditions but significant removals were  observed
under flowing conditions.

     The pH of the leachate is a factor in the  leaching  and removal  of  consti-
tuents by a specific sorbent.  The pH of the effluent leachate,  after prolong-
ed passage through the lysimeter, approaches that of the  influent leachate.
Some sorbents are more effective in removing specific cations under alkaline
conditions than acidic conditions.  Acidic fly  ash leaches cations into the
leachate under acidic conditions,  but under alkaline conditions  it effectively

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 removes these constituents.  When this occurs, another sorbent, such as basic
 fly ash,  should be used in combination with the acidic fly ash in a layered
 system to remove the constituents being leached out.  This leaching will de-
 crease to insignificant levels when the effluent from the acidic fly ash be-
 comes alkaline.

     The  permeabilities exhibited by the sorbents are a significant factor in
 the removal of the contaminants from the three leachates studied.  The coeffi-
 cients of permeability for the clays were so low that mixtures of 20 percent
 clay and 80 percent sand were used to obtain adequate flows of leachate
 through the sorbents in the lysimeters.

     The coefficients of permeability for most of the sorbents, with the ex-
 ception of activated alumina, kaolinite, and bottom ash, remained fairly con-
 stant for both the calcium fluoride sludge leachate and petroleum sludge lea-
 chate.  The coefficient of permeability for kaolinite exhibited a decrease but
 it was not as marked as the decrease in the coefficient of permeability for
 the activated alumina and bottom ash upon the addition of these leachates.
 For the cases of the metal finishing sludge leachates, most of the sorbents
 exhibited a decrease in the coefficient of permeability with the exception of
 the activated carbon.  The coefficient of permeability for this sorbent re-
 mained fairly constant for all  three types of leachate.   The marked decreases
 in the coefficient of permeabilities may result in ponding when the mixtures
 containing these sorbents are used to treat the leachate studied unless pro-
 visions, such as the addition of inert materials to these sorbents, are made
 to minimize these decreases in  permeability.

     The composition and concentration of constituents in the industrial
sludges collected over a period of a year show considerable variations lead-
 ing, in some cases, to wide fluctuations within the leachate.  Thus, the
selection of sorbents to treat  these leachates must take into account the
changes in composition and concentrations that can be encountered.

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                                  SECTION 3

                               RECOMMENDATIONS


     A test, preferably under non-flowing conditions, must be devised for
predicting the effectiveness of the sorbents selected for removing specific
constituents from industrial sludge leachates.  This may be achieved by
identifying the desired properties such as clay type, inorganic composition
and carbon content in naturally occurring sorbents located in the vicinity of
the landfill.  Under flowing conditions, evaluation of a sorbent in a lysi-
meter is time consuming and requires analysis of a large number of samples.

     Means for handling suspended solids present in the leachate must be de-
vised to minimize the clogging of the sorbent bed in the field.  In this
study, the suspended solids in the leachates (generated from the industrial
sludges) were removed prior to treatment.

     Each sorbent was evaluated separately in the treatment of the various
types of industrial sludge leachates.  Since a combination of sorbents must be
used in a single bed for treating the leachate, the removal capacity of these
combinations in a single column must be evaluated.

     The influence of variations in weather conditions such as temperature, pH
of precipitations, etc., on the removal processes must be studied.  For exam-
ple, pH has been shown to be a factor in the leaching - removal process.
Since it is well known that the pH of precipitation can vary dramatically with
locality (15), process development must define and design for this effect.

     Since these naturally occurring sorbents show promise for removal of
cations, anions, and organics from the leachates studied, an investigation
should be carried out using these inexpensive natural sorbents rather than
refined sorbents such as activated carbon for tertiary treatment of waste
streams.  Fly ash has been studied extensively for this purpose, but its use
as part of a sorbent mixture has not been examined.  Also, the sorbents could
be used in sand beds or mixed media filters.  The low cost of these sorbents
warrants their being discarded rather than being regenerated, as in the case
with activated carbon.

     The application of sewage treatment effluents to agricultural soils has
been handicapped by the presence of trace amounts of toxic cations and anions
in this effluent.  The naturally occurring sorbents and waste products should
be tested with the agricultural soils to determine whether these sorbents can
provide an inexpensive means of tying up these toxic substances before they
can contaminate ground or surface waters or be incorporated within the vegeta-
tion.

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      The  selection of sorbents used in this study was limited by time and
 financial considerations.  Other sorbents should be looked at.  For example,
 in our study, alumina was shown to have a great affinity for a large number of
 cations and anions; however, its low permeability negated its usefulness as a
 sorbent.  By choosing a naturally occurring soil or waste materials such as
 red mud,  etc. with a high alumina oxide content or by admixing with sand, this
 permeability problem can be overcome.

      Likewise, the choice of industrially generated sludges used in this study
 led to a limited number of measurable contaminants being encountered in the
 leachate.   Sorbent combinations for the treatment of only calcium,  magnesium,
 copper, nickel, zinc, fluoride cyanide and organics have been defined.   Addi-
 tional industrial sludges whose leachate contains significant concentration of
 cadmium, chromium, lead, iron, mercury, arsenic, antimony, tin,  strontium,
 etc.  should be examined to define the sorbent combinations that  can be  used to
 treat these contaminants.

     The results of this additional  work could provide a list of promising  sor-
 bent combinations that may be recommended to industry for treating  the  heavy
metal, toxic anions and organics encountered in their sludge leachate.
                                     8

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                                  SECTION  4

                            MATERIALS DESCRIPTION
SORBENTS
     The sorbent materials that were selected for this  study  are  bottom  ash,
fly ash, zeolite, vermiculite, illite,  kaolinite, activated alumina,  cullite,
and activated carbon.   The selection of these materials was based on  the con-
sideration of three factors, namely, (1) economics,  (2) availability, and (3)
removal potential.

Fly Ash

     Fly ash is a waste product of fossil fueled power  generating plants and
is collected by electrostatic precipitators from the fuel  gases before they
enter the stacks.  This material is generally dark gray in color and  is  com-
posed of constituents  present in coal or their combustion products.   Physical-
ly, it is a fine gritty substance with  the individual particles ranging  from
0.5 to 100 microns.  The principal chemical constituents of fly ash  are
silica, alumina, iron  oxides, sulfur trioxides, and alkali and alkaline  earth
metals.  Approximately 30 million tons  of fly ash is produced annually in
this country; only 17.4% is eventually  utilized, and the balance is  disposed
of in landfills.  The samples, both acidic and basic, used for this  study were
supplied by Public Service Electric & Gas Company, Hudson Generating Station,
Jersey City, New Jersey.

Bottom Ash

     As in the case of fly ash, bottom ash is also a waste product of fossil
fueled power generating plants and is collected as a residue of the  furnace.
This material is generally dark gray in color and is also composed of consti-
tuents similar to those present in fly ash.  However, the individual  particle
is much larger than that of fly ash.  The samples used for this study were also
furnished by Public Service Electric & Gas Company, Hudson Generating Station,
Jersey City, New Jersey.  The material  as received contained grain sizes rang-
ing from 150 microns  to 1/2  inch. They were ground to pass a sieve size of 80
mesh before use.

Zeolite

     Any mineral belonging to the zeolite family of minerals and synthetic
compounds is characterized by an aluminosilicate tetrahedral  framework and
loosely held water molecules, permitting reversible dehydration.  Zeolites

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 have been extensively studied from theoretical  and  technical  standpoints be-
 cause of their potential  and actual  use  as  molecular  sieves,  catalysts, and
 water softeners.   Zeolites  are low temperature  and  low-pressure minerals found
 in aurygdaloidal  basalts  and also  as  authigenic minerals  in sandstones and
 other sediments.   These materials  are usually white in color.  After consider-
 ing potential  sorption characteristics,  as  well as  availability, zeolite was
 selected for the  present  study.  The  sample used was  from Brickhorn, New
 Mexico,  and was furnished by the Double  Eagle Petroleum and Mining Company,
 Casper,  Wyoming.   Physically, the  material  is light tannish-white in color
 and  has  a  powder-like  texture.  The sorbent was used as received.

 Kaolinite

      The structure of kaolinite is composed of  a single silica tetrahedral
 sheet and a single alumina  octahedral  sheet combined  in a unit.  It is the
 principal  mineral  of  the  kaolinite group of clay mineral.  The mineral kaoli-
 nite has a moderately low cation-exchange capacity  (5-15 milliequivalent per
 100 g).   Broken bonds  around the edges of the silica-alumina  units are the
 major cause of this exchange capacity.   Kaolinite may form under acid condi-
 tions at low temperatures and pressures.  It is a principal component of
 lateritic-type soils.   Kaolinite has  been used  extensively in the ceramics
 industry and in paper  products.  The  selection  of this sorbent material was
 principally due to its importance  in  clay family as well as its potential
 sorptive properties and availability.  This material was furnished by Georgia
 Kaolin Company, Elizabeth,  New Jersey.   Physically, it is tannish-white pow-
 der.   It was used  as  received.

 Vermiculite

      This  micaceous mineral  exfoliates when heated or subjected to certain
 chemical  reactions.   It is  a  hydrated magnesium aluminum iron silicate.  The
 structure  of vermiculite consists  of trioctahedral  mica sheets separated by
 double water layers and is  unbalanced by substitution of aluminum for tetra-
 hedral layer.   The resulting  charge deficiency is satisfied by exchangeable
 cations which  occur chiefly  between the mica layers.  Vermiculites have a high
 cation-exchange capacity  (150 mi Hi equivalents per 100 g).  They also adsorb
 certain organic molecules between  the mica  layers.   It is frequently listed as
 an alternate product of biolite mica in ancient sediments.  Vermiculite is ex-
 tensively  used  in many industries, including fireproofing, insulation, ferti-
 lizer conditioners, and packing materials.  This material was used as received
 and was obtained from W.R. Grace & Co., Trenton, New Jersey.

 mite

     The term illite is used to denote the aluminum, magnesium, and iron rich
mica found in the  clay fraction of weathered shale in Illinois.  The basic
structural unit is composed of two silica tetrahedral  sheets  with a central
octahedral sheet.   The size of naturally occurring  illite particles is very
small with well-defined edges.  The illites  have a  moderate cation-exchange
capacity (20-30 milliequivalent per 100 g).   It is  primarily  due to broken
bonds, but lattice substitution may also be  a cause in poorly crystallized
varieties.   Illite is  a common product of weathering and is  particularly


                                     10

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 abundant  in deep-sea clays.  The sample used for this study was obtained from
 A.P.  Green Refractory Co., Morris, Illinois.

      The  material  received was in rock form and was ground to powder that
 passed  through an  80-mesh screen before use.

Activated Alumina

     Activated alumina is a highly porous,  granular form of  aluminum oxide with
preferential  adsorptive capacity  for  moisture  and  odor.   Sizes  range from powder
to 1.5-inch diameter particles.   In  this  study,  particle sizes  less than
.045 mm and in the size range from 0.147  mm to 0.295 mm  were examined.   Acti-
vated alumina has been used as a  desiccant for gases and vapors in the  petro-
leum industry.  It is also used as a  catalyst  or catalyst carrier.  The sample
studied was furnished by Alcoa,  Bauxite,  Arkansas.

Activated Carbon

      Activated carbon is a manufactured form of carbon with high adsorptivity
 for  gases, vapors,  and  colloidal solids.   It is obtained by the destructive
 distillation  of  carbonaceous materials and activated by heating to 800-900°C
 with steam or carbon dioxide.  This  results in a porous internal honeycomb-
 like structure.  The specific area of air  activated  carbon  is  generally very
 large,  ranging from 600 to 2000 square meters per  gram.  Although capable of
 adsorbing large  amounts of water vapor, activated  carbon finds  its major use
 in solvent recovery, odor and taste  removal, and as  a catalyst  and catalyst
 carrier.  The sample  (Grade  718, Granular) was obtained from Witco Chemical,
 Activated Carbon Division, New York, New York.

Cullite

     Cull He is  a commercial  name of a synthetic zeolite.   It is a  chemically
bound mixture of oxides of sodium, aluminum, and silicon.   Physically,  it has
a white granular form, ranging from 16 to 40 mesh.   The  primary use  of this
material is in water softening.   This material  was selected primarily  due to
potential  capacity as a reference point of synthetic sorbent material.   The
sample used in this study is called "High Capacity Cullite", abbreviated
"Cullite"  hereafter.  The sample was  supplied by Culligan U.S.A.,  Northbrook,
Illinois.


SLUDGE SOURCES

     The calcium fluoride sludge used in  this  study is  the result of lime pre-
cipitation of fluoride in waste streams from etching processes  used  in  the
electronics and aircraft industries.   Three samples designated  as  #1,  #2, and
#3 were collected over a period of a year to determine  how changes  in  produc-
tion schedules and process influence the composition of  the leachate generated
from this  sludge.

     The metal finishing sludges designated as #1, #2,  and #3 were also collec-
ted over a year and are  the result of alkaline treatment of a waste stream from

                                     11

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a metal finishing plant.

     Storage tank bottoms and the API separator were the source of the petro-
leum sludge #1  and #2 generated by refineries.
                                     12

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                                  SECTION 5

                           EXPERIMENTAL  PROCEDURES
PREPARATION OF SORBENT MATERIALS

     All sorbent materials were used as received.   Sorbent materials which
were not obtained as a powder (illite,  bottom  ash,  and  vermiculite) were
ground in a laboratory hammer mill  (Weber Bros,  and White Metal  Works,  Inc.
Type 22) and passed through an eighty mesh A.S.T.M. standard sieve.  All  sor-
bents were dried to constant weight at 103°C (in accordance with "Standard
Method" procedures; 13th Ed., 1971, A.P.M.A.)  and stored in a desiccator  until
used.

PREPARATION OF  BACKGROUND  LEACHATES FROM SORBENTS

     Background leachates of all sorbents except vermiculite were prepared
using deionized water and dried sorbent material in the ratio of 2.5 ml water
per gram of sorbent material and agitated in a Burrell  Shaker for 24 hours  at
ambient temperature.  Our studies revealed that saturation of the mixture with
respect to total dissolved solids as measured by conductance was achieved in
24 hours.  The vermiculite leachate was prepared in ratio of 10 ml of  water to
one gram of sorbent material because all the water was  taken up by the vermi-
culite and none was available for analysis when the 2.5 to 1 ratio was used.
The resultant mixture was then filtered using a glass fiber filter (Reeve
Angel Type 934A; 1.6 microns pore size) in order to remove all undissolved  and
non-filterable solids.  The filtrates (leachates) were  then analyzed according
to procedures described later.

PREPARATION OF SLUDGE LEACHATES

     A sample of each type of sludge was dried at 103°C to constant weight  in
order to determine its moisture content.  In the case of the calcium  fluoride
and metal finishing sludges, the unaltered sludge was then mixed with  deion-
ized water in a ratio of 2.5 ml water per gram of dried sludge (as defined  by
the above moisture content determination) and mechanically stirred for 24
hours.  The above ratio used in the test was arrived at after a series of
trial ratios were carried out.  This involved decreasing the quantity  of water
in the mixture until maximum sludge leachate concentrations were achieved.

     The petroleum sludge leachates presented a filtration problem because  of
the extremely high concentration of oils and greases present in the sludge.
Thus, a higher mixture ratio (i.e. 10 to 1) of water to sludge was employed.
Ratios less than this were extremely difficult to filter.  All suspensions,


                                     13

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 with  the  exception  of  the metal finishing sludge leachate, were filtered
 through a glass  fiber  filter  (Reeve Angle Type 934A) after stirring.  The
 resultant filtrates were analyzed, stored in screw-capped plastic bottles or
 carboys at ambient  temperatures until used.

      The  metal finishing sludge leachate was prepared by filtering the suspen-
 sion  with a Trommel Rotary Vacuum Laboratory Filter  (Fabricators, Inc., of
 Piscataway, New  Jersey) using newsprint paper, because of the slow rate of
 settling  of the  solid  encountered with this sludge.  This leachate was then
 passed through a glass fiber filter to remove any nonfilterable residue, ana-
 lyzed and stored in plastic carboys at ambient temperature until used.

      All  leachates  were analyzed again just before use, even though stored
 leachate  samples failed to exhibit any significant changes in contaminant
 concentration.

 STATIC STUDIES

      Into a tared, one liter screw-capped, polypropylene Erlenmeyer flask was
 placed  100 grams of dried sorbent material.  To this was added 250 ml of
 sludge leachate.  To the vermiculite, 1000 ml of sludge leachate was added
 because the 250  ml amount of leachate initially added was absorbed by this
 sorbent and none was left for analysis after filtration.  The flask was sealed
 and agitated for 24 hours at ambient temperature.  At the end of this time,
 the mixture was  filtered through a glass fiber filtered the filtrate was
 analyzed.   Vermiculite, illite and kaolim'te were used as a mixture containing
 80 grams  of inert Ottawa sand and 20 grams of sorbent (see Tables 3,7, and
 10).  These mixtures were required in the dynamic studies to increase the
 permeability of  these sorbents to acceptable levels (see the following sec-
 tion).  Thus, these mixtures were used in the static studies to provide a
 basis for comparing the static results with the lysimeter results.

 DYNAMIC STUDIES

      In order to simulate dynamic conditions, lysimeter studies were conducted
 using 500 g of sorbent material, except for activated carbon where 250 g pro-
 vided approximately the same column height.   The sorbents, vermiculite, il-
 lite, and kaolim'te, were prepared as a mixture consisting of 80 percent inert
 Ottawa sand and  20 percent clay.  This ratio was arrived at after a series of
 studies established that this would permit adequate flows of leachate through
 these sorbents.  "Pure" clay lysimeters did not exhibit adequate permeability
 characteristics.

     Lysimeters were constructed of plexiglass tubing (6.2 cm i.d.; 0.6 cm
wall thickness;  90 cm length), supported in a vertical  position.  The labora-
tory arrangement of the lysimeters are shown in Figure 1.  A 164 micron pore
size corundum disc (6.10 cm diameter; 0.6 cm thickness) was placed in each
column,  directly over the drain hole in order to prevent clogging of the out-
let and also to support the sorbent material.   The column was packed with the
preweighed sorbent,  placing 3 to 4 cm of Ottawa sand below and above the sor-
bent to prevent disturbing the geometry of the sorbent column during addition
of leachate or water.   The packed column was then slowly wetted with leachate

                                     14

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              Figure  1.   Laboratory Arrangement of  Lysimeters
to allow total saturation and to force all entrapped air in the soil voids
out of the column packing.  After a saturation period of at least 24 hours,
the column was then filled with leachate to the level of an overflow drain,
which had been trapped into the top side of the column, to permit a constant
head condition.  Leachate was fed to the top of the column through a valved
manifold that distributed the leachate to 10 lysimeters simultaneously,
from a central reservoir.  The central reservoir, a 100-liter polyethylene
carboy, delivered the leachate to the manifold system by means of a gravity
syphon feed arrangement.  Any overflow from the constant head drains was col-
lected and pumped back up to the central reservoir.  All tubing in the system
was made of Tygon tubing (3/8" i.d.).  A constant hydraulic head was main-
tained in the lysimeters at all times, and the volume of leachate passing
through the columns was continuously monitored.  Samples of leachate effluent
were collected at intervals and analyzed to determine the concentration of
all measurable constituents remaining in the effluent after a known volume of
leachate had passed through the column.  This was continued until break-
through for all measurable contaminates had occurred or excessively low
permeabilities were encountered.  Break-through is defined as that condition
when the concentration of the species of concern in the collected effluent
sample approached or exceeded that in the influent.
                                     15

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 ANALYTICAL  PROCEDURES

     The  constituents in the leachate generated from each sludge were initial-
 ly  identified using emission spectroscopy and x-ray fluorescence.  Their con-
 centration was then determined using atomic absorption and specific ion
 probes.   The concentration of organics was determined using total organic
 carbon and chemical oxygen demand measurements.  pH and conductivity measure-
 ments were also carried out on the leachate to further characterize the sam-
 ples.

 pH  Measurements--
     The  pH of the samples was measured by means of an Orion Model 701 Digital
 pH/mv Meter using an Orion combination pH electrode, Model 91-02.

 Conduct! vi ty~
     Measured,using a Beckman conductivity bridge (Model RC16B2) together with
 a specific conductance cell having a cell constant of 1.

 Chemical  Oxygen Demand (COD)«
     An automated procedure based on the manual method described in "Standard
 Methods"  was employed in the determination of COD.  The sample was digested
 with a potassium dichromate - sulfuric acid digestion mixture, and the deple-
 tion of the hexavalent chromium (due to the oxidation reaction with the sam-
 ples) was measured colorimetrically.  This automated analysis was performed
 using a Technicon Autoanalyzer II (Industrial Method Number 137-71W).

 Total Organic Carbon (TOC) —
     Measured by use of the Dohrmann Envirotech DC-52D Carbon Analyzer.

 Determination of Anionic Species--
     The  analysis for the anions Cl~, F", CN~ were as follows:

     Chloride ion analysis—Analysis of chloride ion was conducted using a
 chloride  ion electrode (Orion Model  No. 94-17) in combination with a single
 junction  reference electrode (Orion  Model No. 90-01) connected to an Orion
 Model 701 digital/mv meter.  This electrode responds directly to chloride ion.
 The chloride ion concentration of a  sample solution was determined directly by
 comparing the electrode potentials obtained using standards of known chloride
 ion content.  Straight-line calibration curves were obtained over the range of
 1 to 1000 ppm using reagent grade sodium chloride.

     Fluoride ion analysis—Analysis of fluoride ion was carried out using a
 fluoride  ion electrode (Orion Model  94-09) in combination with a single junc-
 tion reference electrode (Orion Model 90-01) connected to an Orion Model 701
 digital  pH/mv meter.   The fluoride content of a sample solution was determined
directly by comparing the electrode  potential reading in the sample solution
to electrode potentials  obtained in  standards of known fluoride content.
Straight-line calibration curves were obtained over the range of 0.1  ppm to
 1000 ppm using reagent grade sodium  fluoride.  A total ionic strength adjuster
 buffer containing 1,2-cyclohexylenedinitrilotetraacetic acid (Orion Cat. No.
 94-09-09A) was used in the ratio of  one part reagent to one part sample for
 all  fluoride ion measurement.   This  reagent will  "swamp out" variations in the

                                     16

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levels of other ions present in the solution as well  as  destroy  polyvalent
cation complexes of fluoride by preferentially complexing these  cations.
Therefore, total fluoride was measured.

     Analysis of cyanide ion—Analysis of cyanide ion was conducted  using a
cyanide ion electrode (Orion Model  900100) connected  to  an Orion Model  701
digital pH/mv meter.  This electrode responds directly to cyanide ion activi-
ty, without regard to sample ionic composition, total ionic strength, pH or
complexing species.  The free cyanide ion content of  a sample solution  was
determined directly by comparing the electrode potentials obtained using stan-
dards of known free cyanide ion content.  Semi-logarithmic calibration curves
were obtained over the range of 0.01 to 10 ppm using  reagent grade socnum
cyanide.   All solutions were adjusted with 10M NaOH to concentrations of 0.1M
in NaOH.

Determination of'Metals--
     The concentrations of the various metals reported (i.e.  Ca, Cd, Cr, Cu,
Fe, Mg, Ni, Pb, Zn) were determined using a Varian Techtron Atomic Absorption
Spectrometer (Model 1200) according to E.P.A. procedures (16).  The reference
solutions used to construct calibration curves in these  determinations  were
made up using deionized water with a specific resistence of 18 Megohm-cm
(25°C).

PERMEABILITY STUDIES

     After a steady flow condition through the column was established,  volume
throughput per second was recorded.  The permeability coefficient, k,  was  then
calculated by means of the following equation  (17):

                                k = (QL)/(aht)

where a = Cross-sectional area of soil column

      Q = Total quantity of water which flowed through the soil column in
          elapsed time, t.

      h = Total hydraulic head, i.e., distance from  the bottom drain to the
          top of the leachate level corresponding to the level of the top
          overflow drain.

      1 = Length of soil sample in the lysimeter.

      t = Total elapsed time in seconds for quantity collected, Q.

     Permeability tests were conducted each day, until break-through had been
achieved.  In certain cases, where the flow through  the lysimeters ceased, the
studies were discontinued even though leachate analysis  indicated that the
sorbtive capacity of the soil column was not yet exhausted.

GRAIN SIZE DETERMINATION

     The test procedure for grain size determination  follows:   For  large grain


                                     17

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 sorbents  (i.e.  >200 mesh)  sieve  analysis was  performed.   For  those sorbents of
 a fine particle size (<200 mesh)  the  hydrometer  test was  used to  determine
 grain size.   For mixed  size composition a  combined  analysis was used.

 Sieve Analysis--
      A sieve  analysis consists of passing  a sample  through a  set  of sieves and
 weighing  the  amount of  material  retained on each sieve.   The  sieves used were
 specified according to  ASTM.

 Hydrometer Analysis--
      The  hydrometer analysis  is  based upon Stokes'  law, which relates the ter-
 minal  velocity  of a sphere falling freely  through a fluid to  the  diameter.  It
 is  assumed that Stokes1  law is valid to a mass of dispersed solid particles of
 various diameter and shapes.  The hydrometer  is  used to determine the percen-
 tage  of dispersed particles  remaining in suspension at a  given time.  The
 grain  size equivalent to a spherical particle is computed for each hydrometer
 reading using Stokes1 law.

      The  results  of both sieve and hydrometer analysis were plotted in the
 form  of a  grain-size distribution curve on a semi-logarithmic chart (see
 Figure 2).  The grain size distribution curve was obtained by plotting parti-
 cle diameter on the  logarithmic abscissa and the percent  finer by weight on
 the arithmetic  ordinate.   The grain diameter whose size is greater than that
 of  10  percent of the particles by weight is called the effective  diameter be-
 cause  of  the influence  of  the smaller grain sizes on soil properties.  In
 order  to  demonstrate the characteristics of gradation, the two most commonly
 used  indices are  the uniformity coefficient and the coefficient of curvature.
 The uniformity  coefficient  is defined as the ratio of the size of the 60 per-
 cent particle diameter, by weight, to the effective diameter, i.e.,

                              Cu= (D60)/(D1Q).

 The coefficient of curvature,

                          Cz - [(D30)2]/[(D6())(D10)],

 is a value that can be used to identify such samples of poorly graded mater-
 ials.   The reader is referred to standard texts of soil  mechanics for a more
detailed explanation (17).
                                      18

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       100
        80
        60
    m
—j   en
vo   ac
        20
                 10
1.0
  0.1             0.01

GRAIN SIZE (mm)
                                                   Activated Alumina
                                                   Activated Carbon
                                                   Bottom Ash
                                                   Cullite
                                                   Fly Ash (Acidic)
                                                   Fly Ash (Basic)
                                                   Illite
                                                   Kaolinite
                                                   Vermiculite
                                                   Zeolite
0.001
                                 Figure 2.  Grain-Size Distribution of Sorbents.

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                                  SECTION 6

                            RESULTS AND DISCUSSION


      Three  calcium fluoride sludges and three metal finishing sludges were
 collected over a one-year period in order to determine the magnitude of
 changes  in  the concentration of the constituents due to changes in production
 schedules and manufacturing processes.  Comprehensive analyses were performed
 in  accordance with "Standard Methods" on leachates generated from these'
 sludges.  Petroleum sludges were collected from two separate sources, a stor-
 age tank bottom and API gravity separator, to determine the effect of two
 different sources of petroleum sludge on the composition and concentration of
 the constituents in their respective leachates.

      The heavy metals present in the leachates from the different sludges
 were  found  to be copper, chromium, cadmium, iron, nickel, lead, and zinc.
 Their concentrations are listed in the first column of Tables 1 to 3, 5 to 7,
 9,  and 10.  The concentrations of calcium and magnesium were also measured
 because they contribute to the hardness in water.  The concentrations of
 chloride, fluoride, and cyanide ions were also determined because their pre-
 sence in water in sufficient concentrations can lead to its rejection as
 potential drinking water.  As described earlier, this study is divided into
 two phases; namely, the static study and dynamic study.

 RESULTS OF  STATIC STUDIES

 Calcium Fluoride Sludge Leachate

      Analysis of the leachate prepared from the three calcium fluoride sludge
 samples collected over a period of one year indicated that most variations in
 concentrations of the measured constituents are within a factor of two with
 the exception of cyanide (see Tables 1  to 3).   Cyanide was not found in sig-
 nificant quantities in sludge sample #3 (see Table 3), the most recent one
 collected, because the use of cyanide in the production processes was discon-
 tinued during the study year period.   This was established through discus-
 sions with plant personnel  at the place where  the sludge was obtained after
 it was determined that amounts of cyanide found in the leachate prepared  from
 sludge sample #3 were significantly lower than those encountered in sludge
 leachates #1 and #2.

     Further examinations of the concentration levels of the constituents in
the leachate prepared from the fluoride sludges reveal  that the calcium,  mag-
nesium,  copper,  nickel,  fluoride,  and cyanide  and organic concentrations  (as
 indicated by COD and  TOC) are significant.   However,  cadmium (with the


                                     20

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 exception  of sludge  #1  leachate)  Iron, lead, chromium, and zinc are found at
 concentration levels that  do  not  differ significantly from the minimum concen-
 tration  levels that  can be readily measured using the atomic absorption
 spectrometer  and specific  ion probes.


      The sorbent capacity  of  eleven natural and refined sorbents for the re-
 moval  of constituents  in the  leachate is represented in Tables 1 to 3 for each
 of the constituents  that exist in the leachate at measurable levels.  This
 data  was obtained  by subtracting  the amount of each constituent remaining in
 the leachate  after treatment  with sorbent, from its initial concentration and
 dividing by  the amount  of  sorbent used.  Both acidic fly ash and activated
 carbon were  not evaluated  using leachate #1 (see Table 1) and leachate #2 (see
 Table 2) but  were  examined using  leachate #3.  During our static studies on
 leachate #1 and leachate #2,  only the basic fly ash was available.  Also, our
 limited  supply of  activated carbon was depleted due to the unanticipated large
 amounts  required for these studies.  Since we had collected a limited amount
 of sludge, we were unable  to  prepare leachate #1 and leachate #2 to evaluate
 the activated carbon and acidic fly ash once we obtained sufficient supplies
 of these sorbents.

      An  examination  of  the static study data (see Table 1, Table 2, and Table
 3)  resulting  from  the mixing  of eleven sorbents with three types of leachate
 suggests the  following  observations:  The sorbent exhibits a capacity for a
 specific contaminant and may  be used to remove this contaminant from the
 leachate.  The sorbent  exhibits no capacity for a contaminant in the leachate
 but the  amount of  t^his  contaminant that is leached from the sorbent when it is
 mixed  with the leachate is significantly less than the amount obtained when it
 is  mixed with water  (see sorbent capacities designated as L).  Finally, the
 sorbent  exhibits no  capacity  for the contaminant and no reduction in leaching
 is  observed when it  is mixed with the leachate.  For example, the acidic fly
 ash (see Table 3)  exhibits a  sorbent capacity of 105 mg of COD removed per
 gram of  acidic fly ash  used.  For the case of the calcium, copper and fluoride
 ions,  this sorbent exhibits no removal capacity but the concentration of these
 ions after treatment 1s significantly less than the mathematical sum of the
 concentration of these  ions in the influent sludge leachate and that which is
 leached  from  the sorbent with water.  Perhaps, the addition of a slightly
 alkaline leachate or the presence of contaminants in the leachate reduces the
 leaching potential  of the calcium, copper, and fluoride ions from the sorbent.
 me acidic fly ash exhibited  no removal  capacity for the nickel ion since the
 sum of the nickel  ion concentration in the sludge leachate and that which can
 oe  leached from the  sorbent is equal to the effluent concentration level of
 mckel ion after treatment.

    . The sorbent capacities are listed in Table 4 for both the static and the
 lysimeter tests.   The sorbent .capacities  are considered to include the removal
ctnH   ies related to such processes as  ion exchange, adsorption, etc.   A
rana-2- the sPecific removal  processes  such as the determination of exchange
 im/  1-  s °r 9enerat1on of sorption isotherms was not carried out in this
 investigation because it would be necessary to modify the sludge leachate by
altering the contaminant concentration to obtain this data.
                                     21

-------
                                                         TABLE I :  STATIC STUDY RESULTS OF CALCIUM FLUORIDE  SLUDGE  LEACHATE II
ro
ro
                                      Initial
                                     Condition                        Fly
                           Measured      of                  Bottom   Ash                                           Activated   Activated
                                                                                                                         Minimum
                                                                                                                        Detectable
parameters L
pH
Conductivity
Ca (mg/1)
Cd (mg/1)
Cr (mg/1)
Cu (mg/1)
Fe (mg/1)
Hg (rag/1)
N1 (mg/1)
Pb (mg/1)
Zn (mg/1)
f (rag/1)
Cl" (mg/1)
CtT (mg/1)
COO (mg/1)
TOC (mg/1)
eachate Description* Ash
fi , 1) 7.2
6'3 ?| 6.0
2680 }1
400 2
3
1
0.08 2
3
0.25 J2
3
1
0.22 2
3
0.10 2
{?
11.0 li
3
0.22 2
3
<0.20 2
3
0.02 2
3
6.1 2
3
58.5 2
3
0.60 2
3
76.0 2
3
) 2780
5200
20.0
385
37.5
<0.01
<0.01
0.18
<0.20
0.25
0
0.25
0.10
0.30
<0.05
0.10
0
93.2
52.0
A
<0.05
0.15
0.18
<0.20
<0.20
<0.01
0.10
0
0.31
2.5
9.0
500
470
L
0.07
0.48
0.30
40.3
79.8
L
16.5 (2) 16.3
(3) 0
(Basic)
8.5
10.0
2500
2990
300
485
L**
<0.01
<0.01
0.18
0.50
0.80
0
0.06
<0.03
0.48
<0.05
<0.05
0.13
3.2
1.0
25.0
<0.05
0.10
0.30
0.28
0.28
L
<0.01
0.02
0
1.7
2.2
9.8
9.5
60.0
L
0.04
0.56
0.10
4.8
36.8
93.5
4.1
0
41.3
Zeolite
7.8
7.4
81 50""
7000
6.0
135
663
<0.01
0.03
0.13
0.30
0.30
L
0.07
0.05
0.43
<0.05
0.15
0
169
6C.O
<0.05
0.15
0.18
0.28
0.25
L
0.03
C.04
L
0.51
1.7
11.0
12.6
180
0
0.04
0.54
0.15
'26.6
76.0
L
0
16.4
0
Verraiculite
8.1
7.3
182
2800
1.5
400
0
<0.01
<0.01
0.70
<0.20
<0.20
0.50
<0.03
0.07
0.15
<0.05
0.10
0
4.7
20.2
L
<0.05
0.13
0.09
<0.20
<0.20
<0.01
0.03
0
1.2
5.9
0.20
2.9
56.0
2.5
<0.03
0.50
0.10
13.0
53,2
22.8
2.1
10.9
5.6
Illite
3.0
3.0
4" 60
4400
' 2.S
335
163
0.06
0.06
0.05
0.70
0.80
L
3.6
3.7
L
2.2
2.3
0
' 70.0
48.0
L
0.65
0.75
L
0.33
0.29
L
1.5
1.7
0
0.33
0.64
13.7
'2!7 '
40.0
46.3
<0.03
0.15
1.1
15. '8
48.0
70.0
0
0
41.3
Kaolin He
5.1
4.2
295
1980
""42.0
355
113
<0.01
<0.01
0.18
0.30
0.25
L
" 0.16
0.29
L
<0.05
0.10
0
4.9
14.0
L
<0.05
0.25
0
<0.20
<0.20
0.27
0.06
L
2.3
3.1
7.5
6.8
50.0
21.3
1.2
1.6
L
7.0
140
0
IS. 5
26.0
0
Aluraina(I)
9.8
8.6
1790
3590

-------
                                                           TABLE 2 :  STATIC STUDY RESULTS OF CALCIUM FLUORIDE SLUDGE LEACHATE K
ro
CO
Initial
Condition
Measured of Bottom
Parameters Leachate Description* Ash
PH
Conductivity
Ca (mg/1)
Cd (mg/T)
Cr (mg/1)
Cu (mg/1)
Fe (mg/1)
Hg (mg/1)
N1 (mg/1)
Pb (mg/i;
Zn (mg/1)
r (mg/1)
el' (rag/1)
CfT (mg/1)
COD (mg/1)
TOC (mg/1)
75 S1 7>1
7'5 (2 7.2
3080
365
<0.01
0.30
0.49
1 Z780
2 5950
1 20.0
2 2.61
3 260
1 <0.01
2 <0.01
3
1 <0.20
2 0.30
3 0
[]) O.Z5
2) 0.20
3) 0.73
(1) <0.05
<0.05 (2 <0.05
(3
5.0
0.10
0.38
0.02
5.9
78.0
0.42
88.5
8.5
1 93.2
2 96.6
3) L
1) <0.05
2) <0.05
3 0.13
1 I <0.20
2) 0.33
3) 0.13
V <0.01
2) 0.04
3) 0
Vi 0.31
2) 2.5
3) 8.5
1) 500
2) 482
3) L
1 0.07
2 0.47
3 0
) 40.3
2) 89.3
3 L
1 0
2) 8.5
3) 0
Fly
Ash
(Basic)
8.5
8.9
2500
3410
300
365
L
<0.01
<0.01
0.50
0.70
L
0.06
0.16
0.83
<0.05
<0.05
3.2
3.3
4.3
<0.0'»
<0.05
0.13
0.28
0.28
0.25
<0.01
<0.01
0.03
1.7
2.3
9.0
9.5
88.0
0
0.04
0.50
0
4.8
52.1
91.0
4.1
0
21.3
Zeolite
7.8
7.6
8150
11550
6.0
88.0
693
<0.01
<0.01
0.30
0.40
L
0.07
0.20
0.73
<0.05
<0.05
169
174
0
<0.05
<0.05
0.13
0.28
0.38
L
0.03
0.05
0
0.51
2.1
9.5
126
195
0
0.04
0.44
0
26.8
93.8
L
0
8.3
0
Venn1cul1te
8.1
7.3
182
3200
1.5
318
47
<0.01
<0.01
<0.20
<0.20
1.0
<0.03
0.29
0.20
<0.05
<0.05
4.7
9.7
0
<0.05
<0.05
0.05
<0.20
<0.20
1.8
<0.01
0.02
0
1.2 '
5.4
0.50
"• 2.9
80.0
0
<0.03
0.43
0
13.0
67.0
21.5
2.7
8.0
0.5
mite
3.0
3.2
4460
4150
2.5
300
163
0.05
0.07
0
0.70
0.70
L
3.6
3.8
L
2.2
2.2
0
70.0
55.0
L
0.65
0.69
L
0.33
0.38
L
1.5
1.6
0
"0.33
0.91
12.5
2.7
70.0
20.0
<0.03
0.16
0.65
15.8 '
40.0
121
1 0
0
21.3
Kaollnlte
5.1
4.3
295
2680
4Z.O
231
335
<0.01
<0.01
0.25
0.30
L
0.16
0.60
0
<0.05
<0.05
4.9
9.9
0
<0.0b
<0.05
0.13
<0.20
0.33
0.13
0.27
0.32
0
2.3
3.5
6.0
6.8
74.0
10.0
l.Z
1.1
L
7.0
140
0
15.5
18.5
L
Activated
A1um1na(l).
9.8
8.7
1790
4150
<0.10
<0.10
913
<0.01
<0.01
1.1
1.1
L
0.04
0.21
0.70
<0.05
<0.05
0.06
0.23
11.9

-------
                                                        TABLE 3 :  STATIC STUDY RESULTS OF CALCIUM FLUORIDE  SLUDGE LEACHATE «3
ro
Measured
Parameters
pH
Conductivity
C« (ng/1)
Cd (mg/1)
Cr (mg/1)
Cu (rog/1)
Fe (mg/1)
Hg (mg/1)
N1 (mg/1)
Pb (mg/1)
In (mg/1)
F- (mg/1)
CT (mg/1)
C)T (mg/1)
COD (mg/1)
TOC (mg/1)
Initial
Condition
of Bottom
Leachate Description* Ash
7.2
1680
318
<0.01
<0.20
0.10
<0.05
21.3
i
1
1
3
*
J
1.2
6.9
2780
4160
20.0
275
108
<0.01
<0.01
-
<0.20
<0.20
-
1) 0.25
2} 0.10
3) L
2
3
2
3
0.15 (2
(3
<0.20 (2
• (3
0.18
6.7
6S.O
0.05
44.0
16.0
r— fsj ro
I
I
i
2
3
<0.05
<0.05
93.2
90.0
L
<0.05
0.15
0
<0.20
<0.20
<0.01
0.14
0.10
0.31
3.0
9.3
500
550
0
0.07
0.06
L
40.0
80.0
0
U 0
2) 16.0
3) 0
Fly
Ash
(Acidic)
5.1
5.4
3150
3800
357
344
L
<0.01
<0.01
0.50
<0.20
0.29
0.34
L
<0.05
<0.05
64.4
98.0
0
1.40
1.55
0
0.30
0.30
0
1.6
1.8
0
1.7
7.5
L
10.0
70.0
0
0.04
0.04
0.03
<2.0
<2.0
105
0.50
0.70
38.3
* (1) Background of Sorbent Material (mg/1)
(2) Effluent Level After Treatment (mg/1)
(3) Sorbent Capacity ug Removed per g of Sorbent Used
** L Represents no Sorbent Capacity and a Reduction In
Fly
Ash
(Basic) VermlculHe
10.1
9.8
2030
2430
300
337
L
<0.01
<0.01
0.50
<0.20
<0.06
0.06
0.10
<0.05
<0.05
3.2
4.0
43.3
<0.05
<0.05
0.25
0.28
<0.20
<0.01
0.28
0
1.7
1.5
13.0
9.5
45.5
48.8
<0.03
<0.03
0.05
4.8
14.8
73.0
4.1
8.0
20.0
leaching
9.3
8.2
115
1120
1.5
266
65.0
<0.01
<0.01
<0.20
<0.20
<0.03
0.09
0
<0.05
<0.05
4.7
69.0
0
<0.05
0.50
0
<0.20
<0.20
<0.01
<0.01
2.1
1.2
7.2
L
2.9
60.0
5.0
<0.03
<0.03
0.02
13.0
39.9
4.1
Z.7
20.5
0
nine
3.0
3.2
4460
2360
2.5
325
0
<0.06
<0.01
0.70
<0.20
3.6
0.10
L
2.20
0.60
L
70.0
34.0
L
0.65
0.49
L
0.33
<0.20
1.5
0.74
L
0.33
0.31
79.9
2.7
40.0
313
<0.03
<0.03
0.25
15.8
22.9
264
0
10.3
71.3
of Contaminant When
Kaolin) te
5.1
4.5
295
1600
42.0
250
85.0
<0.01
<0.01
0.30
<0.20
0.16
0.27
0
<0.05
<0.05
4.9
23.5
0
<0.05
0.13
0.25
<0.20
<0.20
0.27
0.28
L
2.3
0.32
79.9
6.8
50.0
188
1.Z
1.2
0
7.0
40.5
43.8
15.5
21.3
L
Sorbent 1s
Activated
Alumina (I)
9.8
9.8
2790
3490
<0.10
<0.10
795
<0.01
<0.01
>o!so
0.04
0.04
0.15
<0.05
<0.05
0.06
0.10
53.0
<0.05
<0.05
0.25
<0.20
<0.20
<0.01
<0.01
0.43
Z.3
1.2
13.8
46.0
89.0
L
0.22
0.25
0
24.0
49.5
L
37.6
20.0
L
Mixed with
Activated
Carbon
9.4
8.7
575
1000
0.50
208
275
<0.01
<0.01
<0.20
<0.20
<0.03
0.09
0.25
<0.05
<0.05
0.10
12.8
21.3
<0.05
<0.05
0.25
<0.20
<0.20
<0.01
<0.01
0.43
0.04
5.2
3.8
5.0
75.0
0
<0.03
<0.03
0.05
<2.0
2.5
104
5.1
1.3
36.8
Leachate
Minimum
Detectable
Value
-
-
0.10
0.01
0.20
0.03
0.05
0.05
0.05
0.20
0.01
0.02
2.0
0.03
2.0
-


-------
                                                        TABLE 4 : COMPARISONS OF SORBENT CAPACITIES   IN  STATIC AND LYSIMETER TESTS

                                                                             (CALCIUM FLUORIDE SLUDGE LEACHATE)
ro
in
Measured
Parameters Description*
Ca
Cd
Cu
Kg
HI
f
cr
CN"
coo
TOC
Static Test fl
Static Test 12
Static Test 13
Lysimeter Test
Static Test 11
Static Test 12
Static Test 13
lysimeter Test
Static Test 11
Static Test 12
Static Test 13
Lysimeter Test
Static Test 11
Static Test 12
Static Test 13
Lysimeter Tost
Static Test i\
Static Test 12
Static Test »3
Lysimeter Test
Static Test 11
Static Test 12
Static Test 13
Lysimeter Test
Static Test 11
Static Test 12
Static Test *3
Lysimeter Test
Static Test 11
Static Test 12
Static Test 13
Lysimeter Test
Static Test 11
Static Test 12
Static Test 13
Lysimeter Test
Static Test #1
Static Test 12
Static Test 13
Lysimeter Test
Bottom
Ash
37.5
260
108
0.18
0.30
0.73
L
L
L
L
0
0.18
0.13
0
9.0
8.5
9.3
34.4
L
L
0
0.30
0
L
~L
L
0
100
MOOO
b
Fly
Ash
(Acidic)
L
350
-
L
2.2
0
250
0
L
109
0
0.03
105
704
38.3
156
Fly
Ash
(Basic)
L"
L
L
0
0.18
0.48
0.83
0.10
0.49
25.0
4.3
43.3
172
0.30
0.13
0.25
9.8
9.0
13.0
57.0
L
0
48. 8
0.10
0
0.05
93.5"
91.0
73.0
232
41.3
21.3
20.0
62.4
Zeolite
663
693
0.13
0.43
0.73
L
0
0.18
0.13
11.0
9.5
0
0
0.1S
0
L "
L
0
0
Vermicullte 11 lite
0
47.0
65.0
84.8
0.70
0.15
0.20
0
0
L
0
0
0
0.09
0.05
0
0.2
0.5
L
2.4
2.5
0
5.0
o.lo-
0
0.02
22.8
21.5
4.1
0
5.6
0.50
0
0
163
163
0
630
0.05
0
0
L
L
L
0
L
L
L
0
L
L
L
13.7
12.5
79.9
205
46.3
20.0
313
1.1
0.65
0.25
70.0
121
264
250
41.3
21.3
71.3
88.0
Kaolinlte
113
335
85.0
1190
0.18
L
0
0
8.9
L
0
0
0
0
0.13
0.25
7.5
6.0
79.8
183
21.3
10.0
188
L
L
0
268
0
0
44.0
102
0
L
L
Activated
Alumina
(I)
99S
913
795
6300
0.18
0.48
0.70
0.15
2.9
26.0
11.9
53.0
534
0.43
0.13
0.25
11.3
11.5
13.8
348
L
L
L
0.30
0
0
L
L
L
0
L
L
L
0
Activated
Alumina
(II) Culllte
1000
913
0.18
0.48
0.70
24.8
12.4
0.35
0.13
10.5
10.8
L
L
0.15
L
0
0
0
0
1000
912
0.15
L
0.18
20.0
11.5
0.03
0.13
10.3
10.0
0
0
0
0
L
L
L
L
Activated
Carbon
275
547
-
0.25
2.0
21.3
19.0
0.25
3.8
0.60
0
0.05
104
956
36.8
325
                         •  Sorbent Capacities are expressed In »g  of Ion  removal  per g of sorbent used.

                         -  Indicates data not obtained for specific sorbent.

                         **L  Represents no sorbent capacity and a  reduction 1n leaching of contaminant when sorbent is mixed with leachate.

-------
      In  Table 4  a  comparison  of  the magnitude of the micrograms of consti-
 tuents removed per gram  of  sorbent used between the various sorbents indicates
 which sorbents are the most effective  for removing a specific constituent.
 Chromium,  iron,  lead, and zinc are omitted from this table because their con-
 centrations  in the leachate are  not significantly greater than the minimum
 detectable value.   There is no single  sorbent material which is effective in
 removing all  measured parameters.  However, either a combination of the
 natural  sorbents basic fly  ash,  kaolinite, vermiculite, and illite or the re-
 fined sorbents,  activated alumina and  activated carbon, can be used to treat
 all  the  measurable ions  found in the calcium fluoride sludges provided that
 leaching of  ions from the sorbents does not exceed the sorbent's capacity for
 removing these ions.  The natural sorbents, basic fly ash and illite, exhibit
 leaching of  specific ions in  the presence of water which may reduce the effec-
 tiveness of  these  sorbents  for treating the calcium fluoride sludge leachate.
 The  basic  fly ash  leaches significant  amounts of calcium whereas the illite
 leaches  significant amounts of copper  and magnesium ions (see Tables 1, 2, and
 3).   However,  this  leaching is reduced when these sorbents are placed in con-
 tact with  the slightly alkaline  leachate.  This is indicated by the effluent
 concentration of the above  ions  being  significantly less than the concentra-
 tion level that is defined  by the mathematic sum of the concentration of the
 ion  in the leachate and  the background of sorbent material.  These were ob-
 tained with  leachates that  contained magnesium ion concentrations of 5.0 mg/1,
 11.0 mg/1  and 21.3 mg/1.

      The above reason however doesn't  explain the results where significant
 sorbent  capacities are obtained  for the removal of a specific ion in one or
 two  leachates  but  not in the  third leachate.  The calcium ion concentration in
 all  three  fluoride leachates  is above  300 ppm (see Tables 1, 2, and 3).
 Yet,  the illite exhibits significant sorbent capacities for calcium in lea-
 chate #1 and  leachate #2 but  no sorbent capacity for calcium in leachate #3.
 The  reason for these results  is  not clear at  the present time.  However,  re-
 moval capacities may be  highly pH dependent,  and a slight difference in the
 leachate pH  will give different  results.  That  is, the pH of leachates #1 and
 #2 was 7.5,  and  that of  #3  was 7.2.

      Of  the natural sorbents, illite was found to be the most effective for
 fluoride,  chloride, cyanide, and organic removal.   Among the refined sorbents.
 activated  alumina was best able to reduce fluoride levels.   Calcium and copper
 removal was best accomplished with activated alumina.   Regarding the natural
 sorbents,  kaolinite could be used for calcium and basic fly ash for copper
 removal.    Basic fly ash and activated alumina were the most effective for mag-
 nesium and nickel removal.   Vermiculite was  the most effective for removing
 cadmium.

     Marked variations  in the sorbent capacity for the removal  from the three
 leachates of specific contaminants can be observed in  Table 4.   One of the
 possible  reasons  is that the sorbent capacity was  determined using a constant
 ratio of leachate to sorbent.   The concentration of some of the contaminants
 in the leachate using this  ratio  may not have been sufficient to saturate the
 sorbent.   As a result,  the  magnitude of these capacities  could increase with
 the concentration of the contaminant in the  leachate  being  examined.   For
example,  the sorbent capacities  exhibited by the basic fly  ash for the  magne-


                                     26

-------
slum ion in the three leachates are 25.0, 4.3,  and 43.3.

Metal Finishing Sludge Leachate

     Analysis of the leachate prepared from the three metal  finishing  sludges
collected over a period of a year showed much greater variations  in  particular
contaminant concentrations than those encountered with the calcium fluoride
sludge leachate.  Here, the concentration in some cases varied by at least a
factor of six when a specific constituent within the three leachates was  com-
pared.  For example, the calcium concentration  ranged from 6.5 mg/1  to 38 mg/1
(see Tables 5 to 7).

     The analysis of the metal  finishing sludge leachates indicated  the pre-
sence of significant concentrations of calcium, copper, magnesium, nickel,
fluoride, chloride, as well as  organics (see Tables 5 to 7).   The concentra-
tions of chromium, cadmium, iron, lead, cyanide, and zinc did not differ  sig-
nificantly from the minimum measurable levels that can be determined using the
atomic absorption spectrometer  and specific ion probes.

     The sorbent capacity of the eleven natural and refined sorbents,  with
respect to each of the measurable constituents  in the leachate, is represented
in Tables 5 to 7.  The sorbent  capacities for the natural zeolites,  the syn-
thetic activated alumina II and cullite were again evaluated using only the
metal finishing sludge leachate #1 and leachate #2.  The sorbent capacities
for acidic fly ash and activated carbon were determined using leachate #3.
The sorbent capacities were obtained according to the calculations described
earlier.

     A comparison of the sorbent capacities (see Table 8) indicates  the most
effective sorbent material for removing specific constituents. Cadmium,
chromium, iron, lead, and zinc  were omitted from this table because  their con-
centrations in the leachate were at levels that could not be measured.  The
natural sorbent, illite, was found to exhibit the largest sorbent capacity for
the oraanics and fluoride ion.   Kaolinite exhibited the largest caoacity for
calcium; vermiculite for magnesium, nickel and  copper.  Vermiculite  and illite
exhibited a capacity for chloride removal.

     As in the case of the calcium fluoride sludge leachates, there  is no
single sorbent material which is effective in removing all ions from the lea-
chates examined.  However, a combination of vermiculite, illite and  kaolinite
shows promise for treating the metal finishing sludge leachate provided that
the leaching of ions from one of the sorbents does not exceed the other sor-
bent 's capacity for removing these ions.  The vermiculite exhibits the best
capacity for magnesium, copper, and nickel; kaolinite for calcium; illite and
vermiculite for the organics and chloride; and illite for fluoride.

     A significant reduction in the copper leaching from illite, as  was the
case for the fluoride sludge leachate, was only observed for leachate  #3 (see
Table 7).  The lack of this reduction in copper when the illite was  mixed
with leachate #1 and leachate #2 is not understood at the present time.
                                     27

-------
                                                         TABLE 5 : STATIC STUDY RESULTS OF METAL FINISHING SLUDGE  LEACHATE II
ro
oo
Initial
Condition
Measured of Bottom
Parameters Leachate Description* Ash
pH 8.9
Conductivity 1200
•
Ca (mg/1) 6.5
Cd (mg/1) <0.01
Cr (mg/1) <0.20
2
{
1
2
3
t
2
3
i
Cu (mg/1) O.K J2
Fe (mg/1) <0.05
Mg (ng/1) 18.0
N< (mg/1) 0.15
Pb (mg/1) <0.20
Zn (mg/1) <0.01
F" (mg/1) 1.2
Cl" (mg/1) 125
CN" (mg/1) <0.03
COD (mg/1) 97.0
TOC (ng/1) 39.9
1
2
3
1
2
3
(1
2
3
1
2
3
1
2
3
2
3
2
3
1
3
2^
1
I
7.2
8.7
2780
3750
20.0
22.0
L**
<0.01
0.02
0

-------
                                                          TABLE 6 : STATIC STUDY RESULTS OF METAL FINISHING SLUDGE LEACHATE  12
ro
Measured
Parameters
PH
Initial
Condition
of Bottom
Leachate Description* Ash
8.8
Conductivity 1670
Ca (fig/1)
Cd (mg/1)
Cr (ng/1)
Cu (rng/1}
Fe (mg/1)
Hg (mg/D
Hi (ng/1)
Pb (ng/1)
Zn (mg/1)
r ("9/1 )
Cr (mg/l)
Of (rag/1)
COD (mg/1)
TOC (mg/1)
13.5
<0.01
0.25
(
0.05 (.
<0.05 (<
20.0 i
0.12 2
C
1
<0.20 i
C
(i
 0.28
i) 0
<0.05
! <0.05
i
93. Z
' 46.0
! L
<0.05
• 0.15
1 0
) 0.13
0.07
0.07
0
<0.05
<0.05
169
54.0
L
<0.05
0.16
0
O.ZS
0.28
0
0.03
0.03
0
0.51
1.9
0
126
425
L
0.04
<0.03
26. ft
127
688
0
53.2
260
Vernlcullte
8.1
8.6
182
1360
1.5
8.0
55.0
<0.01
<0.01
<0.20
<0.20
0.50
<0.03
<0.03
0.20
<0.05
<0.05
4.7
15.0
50.0
<0.05
0.08
0.40

-------
                                                         TABLE 7  : STATIC STUDY RESULTS OF METAL FINISHING SLUDGE LEACHATE 13
OJ
o
Measured
Parameters
pH
Conductivity
Ca (mg/1)
Cd (rcg/1)
Cr (mg/1)
Cu (mg/1)
Fe (mg/1)
Mg (mg/1)
Ni (mg/1)
Pb (mg/1)
Zn (mg/1)
r (mg/1)
el' (mg/1)
CN' (mg/1)
COD (mg/1)
TOC (mg/1)
Initial**
Condition
of Bottom
Leachate Description* Ash
8.2
1140
38.1
<0.01
<0.20
0.53
<0.05

{
2
•1

7.2
7.5
2780
3800
20.0
30.5
19.0
<0.01
<0.01
<0.20
<0.20
T} 0.25
2) 0.39
3) 0.35
U> INJ — «
(1
25.5 (?
(3
0.19 (2
b
<0.05
<0.05
93.2
95.8
L
0.20
0.25
L
(1) <0.20
<0.20 (Z) <0.20
(3)
(1) <0.01
0.06 (2) 0.10
(3) L
1.5
95.0
2
3
<0.03 (2
(3
49.8
0.31
0.90
1.4
500
575
0
0.07
0.05
0
1) 40.3
2) 70.9
3) 0
(1) 0
19.7 (2) 19.5
(3) 0
Fly
Ash
(Acidic)
5.1
6.6
3150
4580
357
446
0 •
<0.01
<0.01
0.50
<0.20
0.29
0.13
1.0
<0.05
<0.05
64.4
15.3
25.5
1.4
1.4
0
0.30
0.30
0
1.6
1.4
L
1.7
1.6
L
' 10.0
75.0
50.0
' 0.04
0.04
0
<2.0
19.8
75.0
0.50
6.6
32.8
Fly
Ash
(Basic)
10.1
8.9
2090
2600
300 "
472
0
<0.01
<0.01
0.50
<0.20
0.06
0.16
0.93
<0.05
<0.05
3.2
2.2
58.3
<0.05
0.10
0.23
0.28
<0.20
<0.01
<0.01
0.13
1.1
1.1
0.88
9.5
57.5
93.8
<0.03
<0.03
4.8
26.4
58.5
4.1
12.0
19.3
Vermtcullte
9.3
8.4
115
1075
1.5
16.3
273
<0.0l
<0.01
0.13
2.1
1.0
1.2
4G.O
79.9
37.8
0.22
0.30
0
24.0
63.2
L
37.6
39.3
0
Activated
Carbon
9.4
9.0
575
1125
o;so
6.5
79.0
<0.01
<0.01
<0.20
<0.20
<0.03
<0.03
1.3
<0.05
<0.05
0.10
2.1
58.5
<0.05
0.10
0.23
<0.20
<0.20
<0.01
<0.01
0.13
' 0.04
1.6
0
5.0
75.9
47.8
<0.03
<0.03
<2.0
3.9
115.0
5.1
4.4
38.3
Minimum
Detectable
Value
-
-
0.10
0.01
0.20
0.03
0.05
0.05
0.05
0.20
0.01
0.02
2.0
0.03
2.0
-
                              1)  Background of Sorbtnt Material  (mg/1)
                              2)  Effluent Level  After Treatment  (mg/1)
                              3)  Sorbent Capacity ug Removed per g of
                             L    Represents no Sorbent Capacity  and  a
Sorbent used.
Reduction In Leaching of Contaminant when
Sorbent 1s mixed with Leachate.

-------
                             TABLE 8 :  COMPARISONS OF SORBENT CAPACITIES  IN STATIC AND LYSINETER TESTS

                                                 (HETAL FINISHING SLUDGE  LEACHATE)
Measured
Parameters Destriotion*
Ca
Cu
Hg
HI
F'
cr
coo
TOC
Static Test *1
Static Test 12
Static Test 13
Lysi meter Test
Static Test 11
Static Test «
Static Test »3
Lysineter Test
Static Test 
-------
Petroleum Sludge Leachate

     Analyses of the leachates prepared from the tank bottom sludge and the
A.P.I, gravity separator sludge indicated significant concentrations of cal-
cium, copper, iron, magnesium, nickel, zinc, fluoride, chloride, cyanide,  and
organics (see Tables 9 and 10).  However, marked differences in the concentra-
tions of constituents in each leachate were observed.  The leachate prepared
from the tank bottom sludge contained a greater number of constituents of
higher concentration levels than those present in the A.P.I, separator sludge
leachate.  For example, the organics in the tank bottom sludge leachate are
some four times higher than found in the separator sludge leachate.  The cya-
nide concentration in the bottom sludge leachate is 40 times higher than in
the separator sludge leachate.  Also, the tank bottom sludge leachate contain-
ed significant levels of iron and nickel whereas the levels of these metals in
the separator sludge leachate were not significantly higher than the minimum
detectable values observed using the atomic absorption spectrometer and the
specific ion probes.

     The sorbent capacities exhibited by eleven sorbents for the removal of
constituents in the leachate is represented in Tables 9 and 10.  The sorbent
capacities of the zeolite, cullite, and activated alumina II were determined
with the tank bottom sludge leachate.  The acidic fly ash capacity was only
determined with the A.P.I, sludge leachate because we depleted our supply of
the tank bottom sludge leachate.

     The sorbent capacities are listed in Table 11.  Here, a comparison of the
sorbent capacities indicates the most effective sorbent for removing a speci-
fic constituent.  Cadmium and chromium were omitted because their concentra-
tion levels in the leachate were not significantly different from the minimum
measurable concentrations.

     In the natural sorbent category, illite appears to be effective for re-
moving magnesium and fluoride.   Illite and vermiculite are effective for
chloride and the organics.  Vermiculite is more effective than illite for re-
moving the cyanide ion in the tank bottom leachate but the reverse is true for
the A.P.I,  sludge leachate where the cyanide ion concentration is lower.  Il-
lite exhibits a greater sorbent capacity than the kaolinite for the calcium in
the tank bottom sludge leachate where high leachate concentrations of calcium
are encountered (see Table 9).  On the other hand, kaolinite exhibits a grea-
ter sorbent capacity for the calcium in the A.P.I, sludge leachate where the
calcium leachate concentration is significantly lower.  Activated carbon is
the best sorbent in the refined category for the removal of the chloride,  cya-
nide, fluoride, and organics.  Vermiculite exhibits the best sorbent capaci-
ties for copper in the A.P.I, sludge leachate, iron in the tank bottom sludge
leachate, and zinc in both leachates.  Basic fly ash exhibits a capacity for
nickel  for  both leachates.  Thus, combination of basic fly ash, kaolinite,
vermiculite, and illite shows promise for treating the constituents present in
both petroleum sludge leachates provided that the leaching of ions from one
sorbent does not exceed the other sorbent's capacity for removing these ions.
For the case of the refined sorbents, activated alumina and activated carbon
show promise for treating both leachates.
                                     32

-------
                                                        TABLE 9 : STATIC STUDY RESULTS OF TANK BOTTOM PETROLEUM SLUDGE LEACHATE
co
CO
Measured
Parameters
pH
Initial
Condition Fly
of Bottom Ash
Leachate Description* Ash (Basic) Zeolite
7.4
Conductivity 15000
Ca (mg/1)
Cd (mg/1)
Cr (mg/1)
Cu (aig/l)
Fe (mg/1)
Hg (mg/1)
N1 (mg/1)
Pb (mg/1)
Zn (mg/1)
327
0.05
0.22
0.09
0.20
400
0.23
0.48
0.06
F" (mg/1) 1.5
CT (ng/1)
Of (mg/1)
COO
TOC
10990
7.9
1299
(
448
1
2
[
1
3
1
2
3
I
1
2
3
1
I
2
3
1
*
i
2
3
i
2
i
2
3
1
1
2
3
t— 
-------
                            TABLE 10 :  STATIC  STUDY  RESULTS FOR API SEPARATOR PETROLEUM SLUDGE LEACHATE
Measured
Parameters
P«
Conductivity
Ca (pig/1)
Cd (rag/1)
Cr (mg/1)
Cu (mg/1)
Fe (mg/1)
Kg (mg/1)
N1 (mg/1)
Pb (mg/1)
Z.i (mg/1)
F" (rag/1)
Cl* (mg/1)
CN" (mg/1)
COD (ng/1)
TOO («ig/l)
Initial
Condition
of Bottom
Leachate Description* Ash
ii J3
|i
(I
50.0 (2
(3
27SO
230
20.0
102
) 0
	 ' — hr • *0.35
<0.05
<0.05
93.2'
71.4
L
...... .. fl_M
0.20
L
(i) 
-------
CO
en
                                                           TABLE 11 : COMPARISONS OF SORBENT CAPACITIES III STATIC AND LYSIMETER TESTS


                                                                                  (PETROLEUM SLUDGE LEACHATE)
Measured
Parameters
Ca
Cu
Fe
«g
Ni
Zn
f
cr
or
COO
TCC
Description*
Static Test *1
Static Test 12
Lyslmeter Test
Static Test 11
Static Test i2
Lysimater Test
Static Test 11
Static Test #2
Lysimeter Test
Static Test tl
Static Test *2
Lyslmeter Test
Static Test #1
Static Test 12
Lyslireter Test
Static Test *1
Static Test 12
Lyslmeter Test
Statfc Test #1
Slatic Test *2
Lysimeter Test
Static Test fl
Static Test *2
Lysimeter Test
Statvc Test *1
Static Test 12
Lysimeter Test
Static Test i\
Static Test *2
Lysimeter Test
Static Test #1
Static Test 12
Lysimeter Test
Bottom
Ash
0
0
157
L
0.35
0.04
0.15
L
L
0
0
L
0.08
0.30
0.23
1.3
0.90
0
1C630
L
12.5
0.33
0
"628
588
495
208
224
219
Fly
Ash
(Acidic)
0
0
L
2.7
-
L
0
0
L
2.0
L
9.9
40.0
0.43
3.3
825
4545
318
1813
Fly
Ash
(Basic)
L
L
0
0
0.28
2.5
0.38
7.5
58.8
140
0.10
0.13
0.08
0.30
2.0
0.50
0.25
7.2
11980
75.0
7.5
0.35
3.3
1 628
712
5125
225 '
273
983
Zeolite
0
0
0
110
0
0.05
1.3
10630
12.3
703
175
Vermiculite
0
0
1010
0
1.8
1.6
1.0
100
0
90.0
0.20
0
0.30
1.5
6.4
1.0
L
0
49600
313
45.0
1.8
13.0
2850
2900
12555
810
1124
4995
Illite
415
0
1110
0.15
0.
0
0
0
70.0
25.6
180
0
L
0
L
0
3.Z
10.1
12.1
19780
1750
16.3
2.1
15.5
"1628
3526
5525
618
1325
2620
Kaollnite
300
100
14.0
0.15
L
0
0
37.5
18.8
753
0
0.25
L
1.5
o •
3.3
L
4.3
17280
350
6.5
0
4.2
465
3200
795
213
1240
273
Activated
Alumina
(I)
812
125
200
0.15
0.28
0.39
0.38
995
68.0
107
0.25
0.13
0.10
0.30-
0.43
2.7
L
3.4
11530
15.0
6.5
0
0
575
308
556
253
125
248
Activated
Alumina
(ID
811
0.15
0.38
995
0.23
0.05
1.9
11630
4.8
448
189
Cull He
765
L
0
903
0.03
0.05
1.6
13730
1.8
420
108
Activated
Carbon
723
92.8
160
0.08
0.23
0
0.38
468
43.8
10.0
0.15
0.13
0.10
0.30
1.3
3.3
0.50
1.3
20490
288
19.0
0.43
2.9
2985
753
300J
1055
289
1270
                           *   Sorbsnt Capacities are expressed In  g of Ion  removal  per g of sorbent used.

                               Indicates data not obtained for specific sorbent.

                           **L  Represents no sorbent capacity and a reduction 1n leaching of contaminant when sorbent  Is nixed with Leachate.

-------
 DISCUSSION OF STATIC RESULTS

      The  results of the static tests on the three types of leachates (i.e.,
 calcium fluoride, metal finishing, and petroleum) indicate that constituents
 present in these leachates in some cases can be removed by the same sorbent,
 and  in other cases, different sorbents must be used to remove the same consti-
 tuent in  the leachate.  The fluoride, chloride, cyanide, and organics in all
 three types of leachate can be treated with illite.  Vermiculite exhibits re-
 moval capacities for the copper in the metal finishing sludge leachate and
 petroleum sludge leachate whereas basic fly ash exhibits the highest capacity
 for  copper ion in the fluoride sludge leachate.  Magnesium  in the calcium
 fluoride  sludge leachate can be best treated with basic fly ash.  In the
 petroleum sludge leachate, illite is the most effective for magnesium whereas
 vermiculite is most effective in treating the magnesium in two of the three
 metal finishing sludge leachates.  Calcium in the fluoride and metal finishing
 sludge leachates can be treated with kaolinite.  On the other hand, the illite
 is more effective than the kaolinite in removing the calcium ion in the tank
 bottom sludge leachate.  Nickel, in the fluoride sludge leachate and petroleum
 sludge leachate, may be treated with basic fly ash and in the metal finishing
 sludge leachate, with vermiculite.

      The  reason for the above differences in behavior of the sorbents toward
 the  same  constituents in different leachates is not known at this time.  How-
 ever, it  is believed that the effectiveness of a specific sorbent for removal
 of a  contaminant may be influenced by the other contaminants present in the
 leachate  because of competition for available sorbent sites.  Thus, some of
 the  constituents may tend to bind more readily to the active sites on the sor-
 bents than others.

 RESULTS OF THE LYSIMETER STUDIES

     As a result of the static studies using the leachates prepared from the
 three industrial  sludges, the natural  sorbents (i.e., basic fly ash, vermicu-
 lite, illite, kaolinite) and the refined sorbents (i.e., activated alumina and
 activated carbon) showed the most promise for treating the constituents found
 in the three leachates.  Although  bottom ash and acidic fly ash were not as
 effective in the static studies, they are also included in the lysimeter stu-
 dies because preliminary examinations under flowing conditions indicate a
 greater removal  than under static conditions.

     The vermiculite, illite, and kaolinite used in these lysimeter studies
 consisted of a mixture of 20 percent sorbent and 80 percent inert Ottawa sand
 because the permeability exhibited by the "pure" sorbents was so low that
 virtually no flow was obtained.   The results of a series of permeability stu-
dies using different mixtures of sand and clay indicated that the above clay-
sand mixture would provide the minimum flow  of leachate through the solids
that could be measured within a reasonable time.

     In these lysimeter studies, only the leachates prepared from the calcium
fluoride sludge  #3,  metal  finishing sludge #3, and the petroleum sludge from
the gravity separatory were used.   There was not enough of the calcium fluo-
ride sludges #1  and  #2, metal  finishing sludges #1 and #2 and the petroleum

                                     36

-------
tank bottom sludge remaining after the  static  studies to permit the prepara-
tion of the 50 gallons of each leachate required  for the lysimeter studies.

     In view of the large number of measurements  required  for  the lysimeter
studies, the analyses for the constituents  in  the effluent from the lysimeter
were performed only on those constituents whose concentrations were signifi-
cantly higher than the minimum measurable concentration or exceeded the ac-
ceptable concentration for raw water standards (18).  The  analysis for the
calcium, copper, magnesium, fluoride, and organics were carried out with the
calcium fluoride sludge leachate.  Cadmium, chromium, iron, and lead were ex-
cluded because the concentrations in leachate  #3  were below the measurable
levels (see Table 3).  Both zinc and chloride  were not  determined because
their concentrations in the leachate were below  raw water  standards.

     The analysis for calcium, copper,  magnesium, nickel,  fluoride, and the
organics were performed on the metal finishing sludge leachate #3.  The cad-
mium, chromium, iron, lead, and cyanide were excluded because  their concentra-
tions were below measurable levels (see Table  7).  Both  zinc and chloride were
below raw water standards.

     The analysis for the calcium, copper,  magnesium,  zinc, fluoride,  cyanide,
and the organics were performed on the A.P.I,  separatory  sludge leachate.  The
cadmium, chromium, and iron were excluded because their concentrations were
below measurable levels (see Table 11).  Chloride was  excluded because its
concentration was below raw water standards.

Calcium Fluoride Sludge #3 Leachate

     The effectiveness of selected sorbents for removing calcium,  magnesium,
copper, fluoride, and the organics under flowing conditions was determined by
measuring the concentration of these constituents in the leachate before and
after it had been percolated through the sorbent.  The pH of the leachate
before and after it passed through the sorbent was also monitored.   The re-
sults are represented in Figures 3 through 9.  Here, the concentration of the
constituent remaining in a sample collected, after a known volume of leachate
was passed through the column, is plotted against this volume of leachate.
The background of the sorbents were  not evaluated using water under flowing
conditions because leaching from the sorbent was indicated when the effluent
concentration exceeded the influent  leachate concentration of a particular
contaminant.

     The pH of the specific leachate samples collected from the lysimeter
changed as leachate  is passed  through  the columns  (see Figure 3).   The pH
values of the effluent leachate  collected initially are defined by the pH of
the sorbent.  For example, the pH of the leachate sample collected initially
from the illite-sand mixture  is  3.   This sorbent, when mixed with water, ex-
hibits a background  pH of  3  (see Table 3).  However, after 4  liters of lea-
chate were passed through  the  sorbent, the pH of the effluent approached that
of the leachate.  This is  observed  for all the sorbents studied.

Calcium Removal--
     Kaolinite,  activated  alumina,  activated  carbon, illite,  vermiculite, and

                                       37

-------
       11
u>
00
     m
     -h
     -h
     (D
     3
     •o  7
                                 8
                                                          	 Leachate
                                                          O Activated Alumina
                                                              Activated Carbon
                                                           Q .Fly Ash (Acidic)
                                                           • *Fly Ash (Basic)
                                                           Q Illite
                                                           O Vermiculite
                                                          A Kaolinite
                                                                      JL
                           Q Bottom Ash
16
                                                Effluent Volume, liters
24
32
               Figure 3.  Lysimeter Studies of pH in Calcium Fluoride Sludge Leachate.

-------
acidic fly ash were examined in the lysimeter for their  ability  to  remove cal-
cium under dynamic conditions.   Leachate was  passed through  these columns un-
til the concentration of calcium in the sample effluent  leachate approached
that of the influent leachate or excessively  low permeability  was encountered.

     The results indicate that activated alumina is the  most effective  for
treating the calcium in the calcium fluoride  sludge #3 leachate  up  to the
addition of 29 liters of leachate (see Figure 4).  Beyond this point, the per-
meability of the activated alumina became excessively low (see Figure 10).
For the inexpensive sorbents, kaolinite-sand  mixture is  the  most effective
with break-through occurring after 10 liters  of leachate had been passed
through this sorbent.

     The sorbent capacities that are exhibited by each sorbent for  a specific
contaminant in the calcium fluoride sludge leachate #3 were  determined  from
the curves in Figure 4.  The area under each  lysimeter curve,  which also in-
cludes that portion where (in some cases) the concentration  of contaminant
exceeds that in the influent, was integrated  and multiplied  by the  total vol-
ume of effluent collected until break-through was achieved or  the permeability
exhibited by the sorbent  became  excessively  low.  (Break-through  is defined
as  the point where  the concentrations  of a specific contaminant in the  influent
and effluent leachates are comparable and there is no longer any significant
removal of a specific contaminant by the sorbent.)  This provides  the total
amount of contaminant added to the lysimeterj the result is  equal  to the total
amount of contaminant removed by the sorbent.  This latter value is determined
by multiplying the concentration of the contaminant in the influent leachate
by the volume of leachate used.  The sorbent capacity is determined by divi-
ding the total amount of contaminant removed by the amount of sorbent used in
the lysimeter.

     The sorbent capacities for activated alumina, activated carbon,
acidic fly ash, illite, vermiculite and kaolinite are presented in Table 4.
Here, it is shown that activated alumina exhibits the largest capacity  follow-
ed by kaolinite, illite, and then activated carbon.

     A comparison of the sorbent capacities exhibited by the acidic fly ash
and illite under static and dynamic condition reveals that calcium is only
removed from the leachate under flowing conditions.  These results are  proba-
bly due to the greater increase in pH  that occurs as the slightly alkaline
leachate flows through these sorbents  than is achieved under static conditions.
The initial fraction of leachate effluent collected shows that  calcium  is
being leached from  both sorbents  (see  Figure 4).  The pH of the acidic  fly ash
and illite effluents collected initially are 5  and 3.2 respectively (see
Figure 3) and are comparable or slightly more acidic than the pH of those
effluents collected  under static conditions  (see Table 3).  The analysis of
the next effluent fraction  collected from the acidic fly ash and illite lysi-
meters show removal  of the  calcium ion from both leachates.  The pH of  these
fractions are 6.0 and  3.8 respectively.

     There are significant  variations  in the concentration of calcium  ion in
the initial effluent fractions collected from the  lysimeters  containing the


                                      39

-------
n>
o
o
o
n>
01
o>
     300
     200
     100
O
A
9
o
o
A
Leachate
Activated Alumina
Activated Carbon
Fly Ash  (Acidic)
Illite
Vermiculite
Kaolin!te
                                                 12            16

                                           Effluent Volume,  liters
               20
         Figure 4.   Lysimeter Studies of Calcium Ion in Calcium Fluoride  Sludge Leachate.

-------
different sorbents.  This is presumably due to the different amounts of cal-
cium  leached from the various sorbents.

Copper Removal--
     The sorbents which  are  effective for removing copper,  based  on  the  static
results, from the calcium fluoride sludge #3 leachate are  basic fly  ash,  acti-
vated alumina,  and activated carbon.   Their removal  capacities were  0.10,
0.15, and 0.25  micrograms removed per gram of sorbent used, respectively (see
Table 4).  Thus, these sorbents  were examined for removal  of the  copper  under
flowing conditions.   The kaolinite, vermiculite,  and acidic fly ash  were also
examined.

     The effective sorbents  for the treatment of copper were found to be aci-
dic fly ash, activated alumina,  activated carbon, and kaolinite  (see Figure
5).  The vermiculite-sand mixture showed no removal  of copper under  flowing
conditions.   Acidic fly ash  and kaolinite-sand mixture were found to be  ef-
fective for copper treatment under flowing conditions even though their  static
tests showed no sorbent capacity for copper.  pH may be a factor, in both
cases.  As leachate is added to the acidic fly ash in the lysimeter, the pH  is
raised from 4 to slightly above 7 after 4 liters have passed through the col-
umn (see Figure 3).   When the effluent leachate becomes slightly  alkaline, the
copper is removed.  The concentration of copper in the effluent leachate now
falls below the dotted line  which represents the initial concentration of
copper in the untreated leachate.  For the case of the kaolinite  the pH  of the
initial kaolinite effluent collected is significantly more alkaline  than the
pH of the kaolinite effluent obtained under static conditions.   The  pH of this
effluent remains relatively constant at slightly greater than 6 and  becomes
neutral when break-through occurs (see Figure 5).

     Considerable variations of the copper ion concentration is observed in
the initial  fractions of effluent collected from the different lysimeters.
This is probably due to the different amounts of copper that are leached from
the various sorbents.  In fact, the concentration of copper in the first 0.09
liters of effluent collected from the acidic fly ash is 2.5 mg/1.  This  is far
in excess of the background concentration of 0.06 mg/1 obtained in the static
studies (see Table 3).

     These excessive concentrations, when'compared to the static data, occur
because the leachate to sorbent ratio for the initial effluent collected from
the lysimeters is equivalent to only 0.2 to 1, as opposed to the water to sor-
bent ratios of 2.5 to 1 used for the determination of background of sorbent
material in the static studies.

     These results indicate that the maximum amount of copper that can be lea-
ched from the acidic fly ash was not achieved (as defined by the conductance
measurements) using the water to sorbent ratio of 2.5 to 1 or that the lower
pH of 4.2 exhibited by this effluent fraction resulted in greater leaching of
the copper than had occurred in the static studies -where a pH of 5.4 was en-
countered.

     The sorbent capacities for the removal of copper by the acidic fly ash,  kao-
linite-sand mixture, activated alumina and activated carbon are 2.2, 8.9, 2.9,

                                      41

-------
-p.
ro
m
-h
-h

n>

rt-

o
o
3
O
            H-

            QJ
O
3

O
-h

O
£Z
u


ua
                0,10
                0.05
                               (2.5 mg/1, at 0.09 1)
                           (0.28 ng/1, at 0.08 1)
                                                                 Leachate
                                                                 Activated Alumina
                                                                 Activated Carbon
                                                                 Fly Ash (Acidic)
                                                                 Fly Ash (Basic)
                                                                 Vermlculite

                                                                 KaolJnlte
                                                             12            16

                                                     Effluent Volume, liters
                                                                             20
                  Figure 5.  Lysimeter Studies of Copper Ion  in Calcium  Fluoride Sludge Leachate.

-------
and 2.0 micrograms of copper removed per gram  of  sorbent used.  The sorbent
capacity for the kaolinite-sand mixture is  significantly greater than the
other sorbents, even though it is not apparent from  a  comparison of the curves
in Figure 5 because the amount of kaolinite used  in  the lysimeter is only 20
percent of the weight of the other sorbents used.

     The kaolinite-sand coefficient of permeability  shows  a  significant de-
crease with the addition of leachate to the lysimeter. However, this levels
off at the point of copper break-through (see  Figure 10).  This reduction in
coefficient of permeability for the kaolinite-sand mixture is  not as signifi-
cant a problem as would occur if the next best sorbent, activated alumina,
were used.  The coefficient of permeability for the  activated  alumina shows no
leveling off.  Thus, a point could be reached  where  the activated alumina
could form an impermeable barrier.

Magnesium Removal —
     Acidic and basic fly ash, activated alumina, and activated carbon were
examined for removing the magnesium from the leachate under  flowing conditions.
The results indicate that basic fly ash and activated alumina  are effective
sorbents for treating the magnesium in the leachate  (see  Figure 6).  Acidic
fly ash was found to be effective for removing the magnesium after the pH of
the leachate became alkaline.  This occurs after approximately 2  liters of
leachate has been passed through this sorbent.  Prior to  this, magnesium was
continuously leached from acidic fly ash.  Thus,  basic fly ash should be used
with the acidic fly ash in a layered system to remove the magnesium during
this initial leaching period.

     The activated alumina appears to exhibit the greatest capacity for remov-
al of magnesium ion and is capable of handling the largest volume of  leachate
(30 liters).  Beyond this, its permeability becomes  excessively  low.

     The sorbent capacities for acidic and basic fly ashes,  activated  alumina,
and activated carbon were determined to be 250, 172, 534, and  19  micrograms  of
magnesium removed per gram of sorbent used.  This order of effectiveness  for
removing the magnesium ion is also apparent from the lysimeter curves  (see
Figure 6) since all the lysimeters contain 100% of the sorbent.

Fluoride Removal~
     The effectiveness of acidic and basic fly ashes, bottom ash, illite,  ver-
miculite, kaolinite, activated alumina, and activated carbon were investigated
for the treatment of fluoride sludge #3 leachate.  The results show  that  the
refined sorbent, activated alumina, is the most effective for  removing  the
fluoride (see Figure 7) even after 26 liters of leachate was added to  the
lysimeter.  Acidic fly ash appears to be the most effective  natural  sorbent
for fluoride removal.  The illite-sand mixture and bottom ash  exhibit  similar
types of removal curves.  Both vermiculite and activated carbon  are  least
effective.

     The sorbent capacities for the bottom ash, acidic and basic  fly  ashes,
vermiculite-sand mixture, illite-sand mixture, kaolinite-sand  mixture,  acti-
vated alumina, and activated carbon are listed in Table 4.  Illite and acti-
vated alumina, which proved to be the most effective  in treating fluoride

                                      43

-------
   25
   20
-h
215
c
fD
3
ft-
O
O
O
n>
Ol
O
3
   10
to
(59
                 [—
            .5 mgjl,
              T
at 0.19  1)
                                                   —  Leachate
                                                   ^  Activated  Alumina
                                                   £  Activated  Carbon
                                                   Q  Fly Ash  (Acidic)
                                                    A   Fly Ash  (Basic)
                                                I
                                        12          16           20
                                          Effluent Volume,  liters
                                                                     24
                                                                    28
32
          Figure 6.  Lysimeter Studies of Magnesium Ion  in  Calcium  Fluoride Sludge Leachate.

-------
n>
O
O
o
o>
-x
Ol
     0
          	 Leachate
          O Activated Alumina
          A Activated Carbon
          O Bottom Ash
          ® Fly Ash (Acidic)
          •  Fly Ash (Basic)
              Illite
              Vermiculite
                                                      D
                                                      O
                                                      A
             Kaolinite
                                                                                                    -ft
     12             16
Effluent Volume, liters
                                                                              20
        Figure 7.   Lysimeter Studies  of Fluoride  Ion  in  Calcium Fluoride Sludge Leachate

-------
 under static  conditions, also appear to be most effective under flowing condi-
 tions.   However,  the basic fly ash and bottom ash, which appear to be more
 effective  than acidic  fly ash for fluoride treatment under static conditions,
 are  not  as effective under flowing conditions.

      The removal  of fluoride under flowing conditions appears to be favored by
 acidic conditions.  The acidic fly ash exhibits significantly better removal
 than  either the bottom ash or basic fly ash when acidic conditions are encoun-
 tered during  the  initial 4 liters of effluent collected.  As the effluent be-
 comes basic,  the  removal of fluoride by the acidic fly ash decreases (see
 Figure 7).  In the case of the illite-sand mixture and kaolinite-sand mixture,
 the  fluoride  is removed until their effluents become basic.  At this point, no
 removal  of the fluoride is observed for both sorbents.

      Considerable variation was observed in the amount of leachate influent
 passed through the sorbents before break-through occurred.  Activated alumina
 again appeared to be able to handle large volumes of leachate before fluoride
 break-through occurred (see Figure 7).   Fluoride break-through for the acidic
 fly  ash  did not occur  until approximately 12 liters of leachate had been
 passed through this sorbent.  The kaolinite exhibited fluoride break-through
 at 10 liters.  Fluoride break-through for the illite-sand mixture and bottom
 ash occurred  at slightly above 4 liters.

 Organic  Removal--
      Bottom ash, acidic and basic fly ashes, vermiculite-sand mixture, illite-
 sand  mixture, kaolinite-sand mixture, activated alumina, and activated carbon
 were  examined for their effectiveness in  removing the organics under flowing
 conditions.   The results indicate that acidic fly ash and activated carbon are
 the most effective sorbents for removing  the organics in the calcium fluoride
 sludge #3 leachate (see Figures 8 and 9).   The performance of the activated
 carbon was as expected since it is widely used for the removal of organics in
 waste streams.  The illite-sand mixture,  however, which appears to be the most
 effective under batch  conditions (see Table 4) is not as effective as acidic
 fly ash  under flowing  conditions even though account is taken of the fact that
 the illite lysimeter contains only 20 percent illite.  The removal capacity of
 acidic fly ash for both COD and TOC is 704 and 156  micrograms removed  per gram
 of acidic fly ash used, respectively, as  compared with the removal capacity of
 illite for both COD and TOC of 250 and 80 micrograms removed per gram of il-
 lite  used, respectively.

      Acidic conditions appear to be a factor in the removal of the organics
but the acidic fly ash is seen to be less  dependent than the illite.   Break-
through of organics for the illite is observed when its effluent becomes alka-
line  but the acidic fly ash continues to  remove the organics even though its
effluent is alkaline (see Figure 8).

     The treatment of appreciable volumes  of leachate before COD and TOC
break-through occurs can better be handled by the activated carbon than acidic
fly ash.   The COD and TOC break-through for acidic fly ash occurs after 9
liters of calcium fluoride sludge #3 leachate was passed through the sorbent
 (see  Figures 8 and 9).   For the case of the activated carbon sorbent, the flow
of leachate through this sorbent was stopped after 12 liters had been passed

                                      46

-------
m
-*>
o>
o
o
O
a>
O»
O
=3
O
O
  -  Lcachate
A   Activated Carbon
O   Bottom Ash
     Fly  Ash (Acidic)
     Fly  Ash (Basic)
     Illite
                                                       A   Kaolinite
                                             Effluent Volume, liters
         Figure 8.  Lysimeter Studies af COD in Calcium Fluoride Sludge Leachate

-------
00
          m
          -h
          o>
          o
          o
          o
          (D
          Ol
          rt-
          o
          -h
          O
          o
          (£>
Leachate
Activated Carbon
Bottom Ash
Fly Ash (Acidic)
Fly Ash (Basic)
Illite
                                                                     Kaolinite
                                                      6            8
                                                    Effluent Volume, liters
         10
12
14
                      Figure 9.   Lysimeter Studies of TOC in Calcium Fluoride Sludge Leachate

-------
through.  However, even at this point, effective removal  of the organics  con-
tinued to be observed.


Permeability Results--
     The use of refined and natural sorbents for the removal  of specific  con-
stituents in the leachate of industrial sludge depends on the removal  capaci-
ty of the sorbent for a constituent in the leachate.  The sorbent should  also
exhibit suitable permeabilities to handle hydraulic loadings  without ponding
occurring at the bed surface.  A series of constant head permeability tests
were performed on activated alumina, activated carbon, bottom ash, basic  fly
ash, the illite-sand mixture (20 percent illite 80 percent Ottawa sand),  and
vermiculite-sand mixture (20 percent vermiculite, 80 percent Ottawa sand)
using the calcium fluoride sludge #3 leachate in order to determine the per-
meability characteristics of these sorbents.  Here the coefficient of permea-
bility versus leachate volume was determined for each sorbent until break-
through of organics from the illite-sand mixture occurred at about 5 liters
(see Figures 8 and 9).

     The results indicate that the coefficient of permeability remains essen-
tially constant with effluent volume for the sorbents tested, with the excep-
tion of activated alumina and kaolinite (see Figure 10).   The coefficient of
permeability for the activated alumina is reduced from an initial value of
7.7 x 10'4 cm per sec. to 2.1 x 10-5 cm per sec. at the completion of the
test (see Table 12).  This amounts to approximately one-fortieth of its ini-
tial value  but then appears to level off after break-through of contaminants
has occurred.  Apparently, the removal of constituents from the leachate by
these sorbents results in a reduction in pore volume through which the leach-
ate flows.  This does not appear to be the case for the other sorbents where
the coefficient of permeability remains fairly constant as the constituents
are removed from the leachate.  Thus, although activated alumina is effective
in removing the cations from the calcium fluoride sludge #3 leachate under
flowing conditions (see Table 4), its presence in a bed for treatment of
leachate from calcium fluoride sludge over a period of time may lead to pond-
ing due to the marked reduction in its coefficient of permeability.

Summary of Results

     In general, a comparison of the results of the batch tests with those
obtained with the lysimeter using the same calcium fluoride sludge #3 lea-
chate indicates that significantly greater removal capacities for given con-
stituent are obtained under flowing conditions than under static conditions
(see Table 4).  For example, the fluoride sorbent capacity obtained for il-
lite under non-flowing conditions was 79.9 micrograms of fluoride removed per
gram of illite used as compared to 205 micrograms of fluoride removed under
flowing conditions.  Also, in some cases, where the static test results show-
ed no sorbent capacity the lysimeter tests showed significant removals.  The
sorbent capacity of acidic fly ash for magnesium under non-flowing conditions
was zero.  Under flowing conditions, 250 micrograms of magnesium was removed
per gram of acidic fly ash used (see Table 4).

     In some cases, the removal of calcium, copper, and magnesium by sorbents


                                     49

-------
 such  as  illite-sand mixtures and acidic fly ash appears favored by an increase
 in  pH to alkaline  conditions.  As the pH of their effluent is increased, the
 cations  that  are leached from these sorbents at lower pH are removed at the
 higher pH.   In other cases alkaline conditions do not appear to favor the re-
 moval  of copper and magnesium by the basic fly ash, or calcium by the vermicu-
 lite-sand mixture.  Greater removals are achieved by these sorbents under
 flowing  conditions, even though the effluent collected from the lysimeters and
 from  the static test are both alkaline.  The reasons for the latter observa-
 tions  are not known at this time.  However, it is presumed that the selecti-
 vity  of  specific sorbents for the removal of a constituent is influenced by
 other constituents in the leachate.  In the static tests, the more competitive
 constituents  could bind to the sorbent first and thus reduce the available
 binding  sites to the less competitive constituents.  However, under flowing
 conditions, the more competitive constituents may be primarily removed in the
 top of the column.  The less competitive ions may bind to the sorbents further
 down  the columns as a result of decrease in the concentration of the more com-
 petitive constituents in the top of the column.  The combined effects of pH,
 ion exchange  capacity and sorption capacity on the interaction between the
 contaminants  in the leachate and the sorbents are the areas that need further
 study.

 Metal  Finishing Sludge #3 Leachate

      The effectiveness of acidic and basic fly ashes, vermiculite, illite,
 kaolinite, activated alumina, and activated carbon for removing calcium,
 copper,  magnesium, nickel, fluoride, and organics in the metal finishing
 sludge #3 leachate, was examined under flowing conditions.  The above consti-
 tuents were selected because their concentrations in the leachate were at
 levels that could be measured using the atomic absorption spectrophotometer or
 specific ion  probes.  In addition, the pH, before and after the leachate
 passed through the sorbents, was monitored to determine if pH has an effect
 on the sorbent's ability to remove a specific constituent.

     The results of this study are shown in Figures 11  to 18.  The dotted
 lines  in each of these figures represent the concentration of the constituent
 present  in the metal finishing sludge #3 leachate prior to treatment with a
 sorbent.

     The pH of the effluent leachate samples collected from the lysimeter con-
 taining  the different sorbents again approaches (with the exception of activa-
 ted alumina and kaolinite) upon the addition of leachate, the pH of the in-
 fluent leachate (see Figure 11).  It is presumed that if additional volumes
 of leachate were added to the activated alumina and kaolinite, the pH of their
 effluents would also approach that of the leachate.  The collection of lea-
 chate from the activated alumina was stopped after 10 liters because its per-
meability became excessively low (see Figure 20).   The kaolinite was not taken
 beyond 10 liters because break-through of calcium occurred at this point
 (see Figure 12).   After 4 liters of leachate was added  to the sorbents,
the pH of the effluent metal  finishing sludge leachate  approached that of
the influent.   Sixteen liters  of leachate was required  to reach this point
for the  fluoride sludge leachate,  however.   The stronger alkalinity of the
metal  finishing sludge #3 leachate (pH = 8.2) may be the reason for this


                                     50

-------
             10
   u
   OJ
   CO
   •o
   c
                      O  Activated Alumina
                      O  Bottom Ash
                       O  Fly Ash  (Basic)
                       D  Illite
                       O  Vermiculite
                      ^  KaoTinite

                      fc  Fly Ash  (Acidic)
                                       l
                              10              20
                                 Effluent Volume,  liters
                                                   30
Figure 10.  Permeability Studies of Sorbent Materials with Calcium Fluoride
            Sludge Leachate
                                     51

-------
   10
-h
-b
CD
3
rt-

T3
—  Leachate
O  Activated Alumina
A  Activated Carbon
O  Fly Ash (Acidic)
C  Fly Ash (Basic)
D  Ulite
O  Vertniculite
A  Kaolinite
                                                            J_
                                         12           16          20
                                          Effluent Volume, liters
                           24
28
32
                 Figure 11.  Lysimeter Studies of pH in Metal Finishing Sludge Leachate

-------
behavior.  As a result, the pH of the effluent  in  all  cases becomes alkaline
after a little less than 2 liters has passed through the sorbents.

Calcium Removal-
     The removal of calcium from the metal finishing sludge #3 leachate by the
sorbents,  under flowing conditions, is represented in Figure 12.   Here, the
illite-sand mixture, vermiculite-sand mixture,  kaolinite-sand  mixture,  and
activated alumina were shown to be effective sorbents  for  the  removal of cal-
cium.  The sorbent capacity exhibited by  each of these sorbents is 1828, 1280,
930, and 737 micrograms of calcium removed per  gram of sorbent used,  respective-
ly (see Table 8).   The sorbent capacity obtained for the activated alumina  is
lower than the clay-sand mixtures even though it appears more  effective (see
Figure 12).  Calculation of this sorbent  capacity  is based on  only 10 liters
of leachate being passed through this sorbent,  as  compared with 22 liters  and
14 liters of leachate passed through the  illite and vermiculite,  respectively.
The flow of leachate through the activated alumina essentially stopped  after
10 liters had been passed through this sorbent.

     It should be noted that both acidic  and basic fly ashes exhibit  leaching
at leachate volumes below 2 liters (see Figure  12). After this,  the  calcium
is removed.  The concentration of calcium in initial effluent  fractions col-
lected from the fly ash lysimeters is greater than that obtained  when the
acidic and basic fly ashes were mixed with water under static  conditions  (see
Table 7).  The volumes of effluent collected from  the  acidic and  basic  fly
ash lysimeters is equivalent to leachate  to sorbent ratios of  1.2 to  1  and 0.6
to 1, respectively.  This is significantly lower than  the  water to sorbent
ratio of 2.5 to 1  used in the static studies to achieve maximum leachate con-
centrations as indicated by conductance measurements.   Apparently, the  larger
ratio did not provide a saturated concentration of Teachable calcium  since the
concentrations of calcium in the initial  effluent  fraction collected  from the
lysimeters is greater than that obtained  in the background of  sorbent mater-
ials determinations under static conditions.

     Considerable variations are observed in the concentrations of calcium
present in the initial fractions of effluent collected from the lysimeters
(see Figure 12).  This is presumed to be  due to the different  amounts of cal-
cium that may be leached from the sorbents as is apparent  from the data for
background of sorbent materials obtained  under  static  conditions  (see Table
' / •

     Greater sorbent capacities were obtained under flowing conditions  than
under static conditions (see Table 8).  In fact, no sorbent capacities  were
obtained for the acidic and basic fly ashes and illite under static conditions,
but significant removals were obtained under flowing  conditions.

     The reason for this  is not clear at this time.  The pH does  not  appear to
be a factor, as was indicated earlier for the calcium fluoride sludge leachate
lysimeter  results, since  the initial fractions  of effluent collected  from the
acidic and basic fly ash lysimeters exhibit alkaline pH.

     The illite-sand mixture appears capable of handling the greatest volume
of leachate before break-through of calcium occurs (see Figure 12).   Activated

                                     53

-------
                                                             TABLE 12 :  PERMEABILITY CHARACTERISTICS OF  SORBENT MATERIALS
                                 SORBENT MATERIAL
cn
1.   Illlte (20X) mixed with Ottawa Sand (SOX)
2.   Vermlcullte (20X) nixed with
3.   Fly Ash (Acidic)
4.   Fly Ash (Basic)
5.   Bottom Ash
6.   Kaollnlte (20X) mixed with Ottawa Sand (80X)
7.   Activated Alumina
8.   Activated Carbon

1.   Illlte (20!) mixed with Ottawa Sand (80X)
2.  Vennicullte (20X) mixed with (
3.  Fly Ash (Acidic)
4.  Fly Ash (Basic)
5.  Kaollnlte (20X) mixed with OH
6.  Activated Alumina
7.  Activated Carbon
                       1.  Illlte (201) mixed with Ottawa Sand (BOX)
                       2.  Vermlcullte (20X) mixed with (
                       3.  Fly Ash (Addle)
                       4.  Fly Ash (Basic)
                       5.  Bottom Ash
                       6.  Kaollnlte (20X) mixed with Ottawa Sand (SOX)
                       7.  Activated Alumina
                       8.  Activated Carbon
A.
fid (SOX)
rf» Sand (SOX)



Sand (80X)


B.
id (80X)
» Sand (80X)


Sand (80X)


C.
id (BOX)
(a Sand (BOX)



Sand (SOX)


e K} (Cm/sec)
Calcium Fluoride Sludqe Leachate
0.52
1.83
1.41
1.38
0.69
0.79
2.07
1.66
Metal Finishing
0.49
1.81
1.50
0.84
0.53
2.29
1.45
Petroleum Sludge
0.44
2.01
1.50
1.01
0.64
0.40
2.20
1.50
2.2
5.8
1.5
1.1
3.3
7.1
7.7
5.2
x
x
X
X
X
X
X
X
IO-5
io-5
io-4
ID'4
ID'4
ID'5
io-4
io-2
K^Cm/sec) K^l^ d10(«n.)
3.7 x
6.4 x
1.3x
9.9 x
3.8 x
2.1 x
2.1 x
6.4 X
ic-5
io-5
io-5
ID'5
io-5
ID'5
io-s
io-2
0.6
0.9
1.2
1.1
8.7
3.4
36.7
0.8
0
0
0
0
0
0
0
1
.016
.20
.0041
.010
.028
.028
.075
.1
Cu
37.5
3.0
2.0
1.4
6.4
21.4
1.3
1.8
Specific
Gravl ty,Gs
2.68
2.52
2.13
2.25
2.69
2.67
3.24
1.26
Sludge Leachate
9.2
1.4
2.1
9.4
2.5
1.4
7.2
X
X
X
x
x
X
X
ID'4
io-4
io-4
10'5
10"5
io-3
io-2
2.7 x
1.1 x
4.7 x
1.3x
1.2 x
4.5 x
8.6 x
io-4
ID'5
io-5
io-5
ID'5
ID'6
io-2
3.4
12.7
4.5
7.2
2.1
311.
0.84
0
0
0
0
0
0
1
.016
.20
.0041
.010
.028
.075
.1
37.5
3.0
2.0
1.4
21.4
1.3
1.8
2.68
2.52
2.13
2.25
2.67
3.24
1.26
Leachate
1.2
8.5
2.7
1.3
4.4
1.4
1.2
6.7
X
X
x
X
x
x
X
X
io-4
ID'5
10'4
ID'4
10
10
ID'3
ID'2
7.5 x
6.3 x
3.1 x
1.8 x
1.5 x
3.0 x
1.7 x
6.7 x
ID'5
io-5
io-4
ID'4
10'6
io-6
ID'6
ID"2
1.6
1.4
0.9
0.7
293.
4.7
706.
1.0
0
0
0
.016
.20
.0041
0.010
0.028
0.028
0.075
1.1
37.5
3.0
2.0
1.4
6.4
21.4
1.3
1.8
2.68
2.52
2.13
2.25
2.69
2.67
3.24
1.26
                                            REMARKS:    e    "Void Ratio
                                                        K,   -  Initial Coefficient of Permeability
                                                        Kg   •  Terminal Coefficient of Permeability
                              d10(mm) •
                                 Cu   «
                                                                Grain Size Diameter at 10X finer
                                                                Coefficient of Uniformity

-------
 m
 -t>
 -h

 c
 n>

 F+

 o
 o
 =3
 O
 n>
 3
o
-h

O
(Q
    40
    35
30
    25
    20
    15
    10
           —i—i—i—\—r—

           (535 mg/1, at 0.6 1)

           (344 mg/1, at 0.30 1)
       -J
                                                 Leachate

                                             O  Activated Alumina

                                             A  Activated Carbon

                                             O  Fly Ash  (Acidic)

                                                 Fly Ash  (Basic)

                                                 Illite

                                                 Vermiculite
 9
 a
 o

A
                                                     Kaolinite
       OOKM—
-------
 alumina would  probably  handle  the  greatest volume of leachate prior to break-
 through if the samples  of  effluent leachate could be collected beyond the 10
 liters  of leachate  that were passed  through the activated alumina.  This could
 not be  shown because  the flow  through this sorbent virtually stopped after 10
 liters  had been passed  through the sorbent.

 Copper  Removal--
      The removal  of copper from the  metal finishing sludge #3 leachate can be
 achieved by the acidic  fly ash,  the  illite-sand mixture, the vermiculite-sand
 mixture, and activated  carbon  (see Figure 13).  Although acidic fly ash ap-
 pears to be more effective for removing the copper than the illite and vermi-
 culite-sand mixtures, it must  be remembered that the amount of vermiculite and
 illite  used in these  tests is  only 20 percent by weight of the acidic fly ash
 used.   If this is taken into account, the illite and vermiculite are then
 found to exhibit sorbent capacities  of 57.5 and 20.5 micrograms of copper re-
 moved per gram of sorbent  used,  as compared with 16.5 micrograms of copper re-
 moved per gram of the acidic fly ash (see Table 8).

      No leaching of copper from the  acidic fly ash is observed.  The fact that
 the pH  of the  effluent  leachate  from this sorbent is never acidic may be the
 reason,   when  the effluent leachate  is acidic, as was encountered with the
 illite  at volumes below 1  liter, copper is leached out of illite (see Figure
 13).

      An analysis of the sorbent capacity exhibited by the illite for copper
 shows a significant removal capacity for copper under flowing conditions
 but none under static conditions (see Table 8).  Apparently, the fact that
 the pH  of the  illite  effluent  was  significantly acidic in the static studies
 resulted in leaching  rather than removal of the copper.


      Activated  carbon appears  to be able to treat copper in the largest volume
 of  metal  finishing  sludge  #3 leachate (see Figure 13).   Acidic fly ash and the
 illite-sand mixture appear to  be next for treating large volumes of this lea-
 chate.

 Magnesium  Removal--
      The activated  alumina, acidic fly ash, and illite-sand mixture appear
 to  be the  most  effective sorbents  for the removal  of magnesium and for hand-
 ling  the  largest volumes of the metal finishing sludge #3 leachate before
 break-through occurs (see  Figure 14).  The sorbent capacities for each of
 these sorbents were 495, 488,  and  1840 micrograms  of magnesium removed per
 gram of  sorbent  used, respectively (see Table 8).

     No  Teachable magnesium was observed with the  acidic fly ash, as was en-
countered with fluoride leachate.  This may be due to the fact that the pH of
acidic fly ash, even in the initial effluent fractions  collected, remains
above 7.

Nickel Removal--
     Activated carbon, acidic  fly ash and activated alumina appear to be the
most effective in removing the nickel in the metal  finishing sludge #3 lea-


                                     56

-------
tn
                                                                 	  Leachate
                                                                 O  Activated Alumina
                                                                 A  Activated Carbon
                                                                      Fly  Ash (Acidic)
                                                                      Fly  Ash (Basic)
                                                                      Illite
        Vermiculite
                                        8             12             16

                                              Effluent Volume,  liters
20
24
           Figure 13.  Lysimeter Studies of Copper Ion in Metal  Finishing  Sludge Leachate.

-------
tn
CO
Leachate
Activated Alumina
Activated Carbon
Fly Ash (Acidic)
Fly Ash (Basic)
Illite
Vermiculite
                                                       12            16

                                                  Effluent Volume, liters
            Figure 14.  Lysimeter Studies of Magnesium Ion in Metal  Finishing Sludge Leachate

-------
chate (see Figure 15).   However,  if account is  taken  of the  fact  that the
illite-sand mixture contains only 20 percent by weight of the activated carbon
and acidic fly ash used, then illite is the most effective.  The  sorbent capa-
cities for illite, activated carbon, acidic fly ash and activated alumina are
7.3, 7.2, 4.9, and 2.5  micrograms of nickel removed per gram of sorbent used
(see Table 8).  These sorbents are also capable of handling  the largest volume
of leachate before break-through  of the nickel  occurs.  Break-through for the
illite-sand mixture occurs at 24  liters whereas, with acidic fly  ash or activa-
ted carbon, break-through of the  nickel did not occur even after  24 liters of
metal finishing leachate had passed through these sorbents (see Figure 15).

Fluoride Removal —
     Significant removal of fluoride in the metal finishing  sludge  #3 leachate
appears to be difficult.  Neither the illite-sand mixture, kaolinite-sand mix-
ture nor activated alumina (which were effective for  removing  fluoride from
the calcium fluoride leachate) seems suitable for treating the  fluoride  in
this leachate (see Figure 16).  The removal capacities for the  illite and
activated alumina are only 2.7, 3.6, and 11.4 micrograms of fluoride  removed
per gram of sorbent used, respectively (see Table 8)  as compared  to 205, 183,
and 348 micrograms of fluoride removed per gram of sorbent used for the  fluo-
ride sludge leachate (see Table 4).

     Apparently, the basic conditions encountered in  the effluents  from  the
lysimeters due to the addition of the alkaline metal  finishing sludge leachate
minimizes the removal of the fluoride.  In the illite lysimeter,  fluoride  is
removed where acidic conditions were encountered.  Above 1 liter, where  alka-
line pH was measured, break-through of the fluoride from the illite lysimeter
is observed (see Figure 16).

Organic Removal —
     The activated carbon, acidic fly ash, and the illite-sand mixture  appear-
ed to be the most effective sorbents for the removal  of organics  (see Figures
17 and 18).

     The COD sorbent capacity exhibited by these sorbents are  1476, 1228,  and
3060 micrograms of COD removed per gram of sorbent used, respectively (see
Table 8).  The TOC removal capacities are approximately one-third of  that  ob-
tained with the COD measurements.  A comparison of the sorbent capacities  for
the illite-sand mixture and activated carbon reveal that the clay-sand  mixture
is more effective than the activated carbon in removing the organics  from this
leachate.  These results are significant because an inexpensive sorbent  has
been identified for treating the organics in the metal finishing sludge  lea-
chate that shows  as much promise as the activated carbon.  The activated  car-
bon is generally recognized as being an excellent sorbent for  the removal  of
organics in waste streams.

     The sorbent capacity exhibited by these sorbents for the  organics  in  the
metal finishing sludge #3 leachate is much higher than that obtained  in  the
removal of organics from the fluoride sludge leachate.  Apparently, the acidic
conditions which favored the removal of organics from the calcium fluoride
sludge leachate are not required for the removal of organics from the metal
finishing sludge leachate.  In all cases, with the exception of  the initial


                                      59

-------
0.20
     D-n-a   CHD/-D—n
                                                        Leachate
                                                        Activated Alumina
                                                        Activated Carbon
                                                        Fly Ash  (Acidic)
                                                        Fly Ash  (Basic)
                                                        Illite
                                                      O Vermiculite
                                                12             16
                                             Effluent Volume, liters
       Figure 15.   Lysimeter Studies of Nickel Ion in Metal  Finishing  Sludge  Leachate.

-------
CTl
         n>
         o
         o
         n
         OJ
             1.5
             0.5
—  Leachate
O  Activated Alumina
 D  Illite
     Kaolinite
                                                    6            8

                                                Effluent Volume, liters
                10
12
         Figure 16.   Lysimeter Studies  of Fluoride  Ion  in Metal Finishing Sludge Leachate.

-------
01
I\3
    Leachate
    Activated Carbon
        Ash  (Acidic)
        Ash  (Basic)
D   Illite
                                                       12            16

                                                Effluent Volume, liters
             Figure 17.  Lysimeter Studies of COD in Metal Finishing Sludge Leachate.

-------
en
CO
Leachate
Activated Carbon
Fly Ash (Acidic)
Fly Ash (Basic)
Illite
Vermiculite
                                                        12              16

                                                    Effluent Volume, liters
                      Figure  18.   Lysimeter Studies of TOC in Metal Finishing Sludge Leachate.

-------
 o
 O)
 o
(O
0)
CL
O)
•r-
U
     „
0)    O
O    --1

°    X
                           -—-A	A-	A	A
            A-"
               X
                            	A	
            	A-	A
Calcium Fluoride  Sludge  Leachate
Metal Finishing Sludge Leachate
Petroleum Sludge  Leachate
                       10
       20
30
   Figure 19.   Permeability  Studies  of Activated  Carbon.
                               64

-------
fraction collected from the illite lysimeters,  the  pH  of the effluent from the
lysimeters is basic (see Figure 11).   In fact,  the  break-through of organics
did not occur for the illite when its effluent  became  basic as occurred with
illite in the removal of organics from the calcium  fluoride sludge leachate.

Permeability Results--
     In addition to the sorbent capacities exhibited by  activated alumina,
activated carbon, acidic and basic fly ashes,  illite-sand  mixture, and vermi-
culite-sand mixture, for the various  constituents in the metal finishing
sludge #3 leachate, variations in the permeability  exhibited by these sorbents
as the leachate passes through were also examined.   All  the sorbents examined,
with the exception of activated carbon (see Figure  19) exhibited a decrease  in
the coefficient of permeability.  The results  again show - as was the case
with the calcium fluoride sludge #3 leachate -  that the  activated alumina ex-
hibits the greatest reduction in the coefficient of permeability upon the
addition of influent (see Figure 20).  This decrease was approximately a hun-
dred times greater than the decrease encountered with  the  fluoride leachate
(see Table 12).  In addition, the coefficient of permeability for the basic
fly ash and the vermiculite-sand mixture showed significant  decreases.  This
decrease was approximately an order of magnitude greater than that observed
with the fluoride leachate.

Summary of Results

     In view of the above results, the effective treatment of calcium,  copper,
magnesium, nickel, and the organics can be best handled by the  use  of the
illite-sand mixture, vermiculite-sand mixture, and kaolinite-sand mixture  in a
layered system.  The vermiculite-sand mixture, although not so  effective  as
the illite, could be used to remove the calcium because the lysimeter results
for the illite suggest the possibility of leaching of calcium from this sor-
bent during the period when the effluent from the illite is acidic (see Figure
12).  Kaolinite is effective for the fluoride removal.  However,  the reduction
in the permeability of vermiculite and permeability of kaolinite must be con-
sidered in the design of a bed to minimize the possibility of ponding at the
surface.

     Activated alumina, which is effective for removing the majority of the
constituents in the metal finishing leachate, does not appear suitable for the
treatment of this leachate.  The marked decrease in the coefficient of permea-
bility exhibited by this sorbent could result in the  formation of an imperme-
able barrier.

Petroleum Sludge Leachate from  an A.P.I. Gravity Separator

     The effectiveness of activated alumina, activated carbon,  bottom ash,
acidic and basic fly ashes,  illite and vermiculite for the removal  of calcium,
copper, magnesium,  zinc, fluoride, cyanide, and  tbe organics was investigated
under flowing  conditions.  These constituents were selected because they were
at concentration levels  in the  leachate that could be readily measured with
the atomic absorption  spectrometer and  specific  ion probes.  In addition, the
pH of the leachate,  before and  after  it was treated with  the sorbents, was  also
monitored to study  the effect  that pH may  have on  the removal of the various


                                      65

-------
   o
   
   (O
   0)
   O)
   a.
   o

   •M
   c
   OJ
   •r~*
   O
   O)
   O
   o
          o
          rH

          X
           O
           1-1

           X
          vO

           O
           X!
                               10               20

                                Effluent Volume,  liters
30
Figure 20.  Permeability Studies of Sorbent Materials with Metal  Finishing
            Sludge  Leachate.
                                     66

-------
constituents by these sorbents.   The results  of  these studies are shown in
Figures 21  to 29.

     The monitoring of pH in the effluent  leachate  collected from the lysi-
meter containing the different sorbents  again showed that  the pH of the ini-
tial effluent samples was similar to that  exhibited by each sorbent, but soon
approached that of the leachate (see Figure 21).   In fact, the pH of each  of
the sorbents became acidic after 6 liters  of  leachate was  passed through.

     An examination of the changes in pH of the  ill He and acidic fly ash,
which both exhibit acidic conditions initially,  revealed different behavior.
The effluent from the illite  remained acidic, as would be expected since the
leachate added to it is acidic, but the  acidic fly  ash became alkaline and
then acidic again (see Figure 21).  The  reason for  this latter observation  is
not understood at this time.

     Lysimeter effluent samples of activated  alumina and bottom ash were not
collected and analyzed beyond a volume of  2 liters  because of the marked re-
duction in permeability exhibited by both  of  these  sorbents  (see Figure 28).

Calcium Removal--
     The removal of calcium in the petroleum  sludge leachate by activated
alumina, activated carbon, illite-sand mixture,  kaolinite-sand mixture, vermi-
culite-sand mixture, and bottom ash is shown  in  Figure  22.  Here it may be
seen that both the illite-sand mixture and vermiculite-sand  mixture are most
effective for removing calcium, followed by activated carbon and kaolinite-
sand mixture.  Their sorbent capacities  are  1110,  1010,  160  and  74 micrograms
of calcium removed per gram of sorbent used,  respectively  (see Table  11).   The
initial effluent fraction collected from the  illite lysimeter  indicates  that
calcium is being leached from this sorbent.   However, as  leachate  is  contin-
ually added to this lysimeter, the calcium begins  to be removed.

     The reason for the calcium being leached initially and  then removed  upon
further addition of leachate is not clear at  this  time.   The alkaline  condi-
tions which favored the removal of calcium in the  calcium fluoride  sludge
leachate and metal finishing sludge leachate  by  the illite do  not  appear  es-
sential for the removal of calcium in the petroleum sludge leachate  by the
illite.  Acidic conditions were encountered in the effluent  from the  illite
until break-through of the calcium occurred at 9 liters (see Figure  22).

     The activated alumina would probably exhibit  a greater sorbent  capacity
for calcium than the illite-sand mixture as seen from the lysimeter  result
(see Figure 22) if additional effluent could be collected from this  lysimeter.
However, such low flows were encountered through this sorbent after  2  liters
of leachate passed through, that the time required for  collection  of signifi-
cant volumes of effluent could not be justified within  the scope of this  in-
vestigation.

     The vermiculite-sand mixture, although not as effective as  the illite-
sand mixture in removing the calcium, should be used in combination with the
illite-sand mixture in a layered system.  The illite exhibits leaching of
calcium in the initial fractions of effluent collected from the lysimeter.

                                      67

-------
                    11
                                                                             T
                                 T
CO
                 m
                 -h
                 -tl
                 CD
                 3
                 c-f

                 TJ
                                                    o
                                                    A
                                                    O
                                                    ®
                                                    o
                                                    D
Leachate
Activated Alumina
Activated Carbon
Bottom Ash
Fly Ash  (Acidic)
Fly Ash  (Basic)
Illite

  A
A Kaolinite
O Vermiculite
                                               A           6            8

                                                Effluent Volume, liters
                           10
                         Figure 21.  Lysimeter Studies of pH in Petroleum Sludge Leachate.

-------
          80
          60
vo
     m
     -b
     o
     3
     O
     ft)
2
     o
     o
     Q>
     to
     •^  20
         40
                        (158 mg/1,  at 0.30 1)
                                     I
                                                   —  Leachate

                                                   O  Activated Alumina

                                                   A  Activated Carbon

                                                   D  Ulite

                                                   O  Vermiculite

                                                   A  Kaolinite
                                                               I
I
                                                                         I
             o
                                                                      8
      10
  246

                    Effluent Volume,  liters


Figure 22.  Lysimeter Studies of Calcium Ion in Petroleum Sludge  Leachate.
12

-------
 Thus, the vermiculite-sand mixture could  remove  this  initial  Teachable calcium
 and reduce its concentration  in  the effluent.

 Copper Removal--
      Activated alumina,  activated carbon,  bottom ash, acidic  and basic fly
 ashes, illite and vermiculite were investigated  for removal of the copper in
 the petroleum sludge leachate.   The most  effective sorbents under flowing con-
 ditions were observed to be acidic and  basic  fly ashes followed by vermicu-
 lite-sand mixture, activated  alumina, and  bottom ash.  The sorbent capacities
 were 2.7, 2.5, 1.6, 0.39 and  0.04 micrograms  of  copper used per gram of sor-
 bent used, respectively  (see  Table 11).   Break-through of copper for the aci-
 dic and basic fly ashes  is not apparent even  after these sorbents were treated
 with 9 liters of leachate (see Figure 23).  The  acidic fly ash again appeared
 to leach copper until  the effluent leachate became alkaline.  The copper be-
 gan to be removed by this sorbent when  slightly  less than 2 liters of leachate
 had been passed through  this  sorbent.

      No removal  of copper is  observed with the illite.  In fact, copper is
 leached from this sorbent until  10 liters  of  effluent have been collected.
 Alkaline conditions were not  encountered  in the  effluent.  The effluent re-
 mained acidic for all  the fractions  collected (see Figure 21).  Significant
 variations are observed  in the copper concentrations present  in the initial
 fractions of effluent  collected  from the  lysimeters.  These variations are
 presumed to be the result of  the  different amounts of copper  that are leached
 from the sorbent into  the effluent.  Illite exhibited the greatest amount of
 copper leaching  in the static  studies (see Table 10).  In the lysimeter stu-
 dies,  it also exhibited  the greatest amount of leaching.  The initial 0.6
 liters of illite effluent collected  contains  1.4 mg/1 of copper.

      The basic fly ash,  although  not as effective as the acidic fly ash in
 the removal  of copper, should  be  used in combination in a layered system with
 acidic fly ash to  remove  the  Teachable  copper from the acidic fly ash.  The
 copper is  leached  from the acidic  fly ash until   its effluent becomes alkaline.

 Magnesium Removal--
     The basic fly ash and the kaolinite-sand mixture appear to be the most
 effective,  followed  by illite-sand mixture, activated alumina, and vermicu-
 lite-sand  mixture  for removing the magnesium ion according to the lysimeter
 results  (see  Figure  24).   Break-through of the magnesium occurs after 4 liters
 of  leachate  is added to the basic fly ash and after 5 liters of leachate have
 been added  to  the  kaolinite.  However, the kaolinite-sand mixture exhibited a
 significantly  greater sorbent capacity than the basic fly ash.  There were
 753 and  140 micrograms of magnesium  removed per gram of sorbent used, respec-
 tively.  The larger sorbent capacity for the kaolinite resulted from the fact
 that the amount of kaolinite used in the lysimeter was only 20 percent of
 that used for  the basic fly ash.   The sorbent capacities for the illite-sand
mixture, activated alumina, and vermiculite-sand mixture were 180,  107,  and
 90 micrograms of magnesium removed per gram of sorbent used, respectively.

     The acidic fly ash was observed to exhibit significant leaching of mag-
nesium in the  initial  4  liters of effluent collected  from the lysimeter.
The maximum concentration of magnesium that was  encountered was 49.5 mg/1  in

                                     70

-------
        mg/
-------
 the column effluent collected at 1.9 liters (see Figure 24).   Changes in pH of
 the effluent to more alkaline conditions do not appear to inhibit this leach-
 ing.  This leaching appeared in the effluents that exhibited  acidic pH and
 those that exhibited alkaline pH.   The reason for this is not clear at this
 time.  The effect of changes in pH on specific ion exchange and adsorption
 interactions between the contaminants in the leachate and these sorbents is an
 area of study that may provide the answer to above results.

 Zinc Removal--
      The removal  of zinc from the  petroleum sludge leachate under flowing con-
 ditions can be achieved with the use of acidic and basic fly  ashes,  followed
 by the vermiculite-sand mixture, activated carbon, activated  alumina and bot-
 tom ash (see Figure 25).  However,  if account is taken that the vermiculite
 used is only 20 percent of the fly  ash used, then vermiculite appears to be
 the most effective sorbent for zinc removal  based upon the  sorbent capacities.
 The sorbent capacities exhibited by vermiculite, acidic and basic fly ashes,
 and activated carbon,  activated alumina and bottom ash are  6.4, 2.0,  2.0,  1.3,
 0.43, and 0.23 micrograms of zinc  removed per gram of sorbent used,  respective-
 ly (see Table 11).

      The acidic fly ash exhibited  leaching of the zinc when its lysimeter ef-
 fluent is acidic   but  began to remove the zinc once this  effluent became alka-
 line.   The alkaline condition  occurred after slightly greater than 1  liter of
 leachate has  been  added to  this  sorbent (see Figure 21).

      Both the illite-sand mixture and kaolinite-sand mixture  exhibited  leach-
 ing of the zinc until  9 and 6  liters  of leachate were added to  the 1111te  and
 kaolinite lysimeters,  respectively.   After the addition of  these  volumes,  the
 concentration of zinc  in the effluents  coincided with the concentration  of
 zinc  in  the influent and no removal of  zinc  was  observed  (see Figure  25).

      The effluent from illite  column  exhibited only acidic  conditions.   The
 lack  of  pH change in the lysimeter  effluent  may  be  responsible.   Where  there
 was a  pH change from acidic  to basic  effluent, such  as for  the  acidic fly  ash,
 leaching of zinc from  the acidic fly  ash was inhibited.

 Fluoride Removal--
     The activated alumina,  activated carbon,  acidic  and basic  fly ashes,  il-
 lite,  kaolinite, and vermiculite were examined for  their effectiveness in  re-
 moving fluoride from the  petroleum sludge  leachate.   The results  indicated
 that the  illite-sand mixture, acidic and basic fly ashes are the most effec-
 tive sorbents studied,  followed by kaolinite-sand mixture, activated alumina,
 and activated carbon, for removing fluoride.   No removal of the fluoride by
 the vermiculite-sand mixture was observed.  The  concentrations of fluoride in
 the lysimeter effluent were the same as in the influent (see Figure 26).

     The sorbent capacities exhibited by the illite-sand mixture, acidic fly
ash, basic fly ash, kaolinite-sand mixture, activated alumina  and activated
carbon for fluoride removal are 12.1, 9.9, 7.2, 4.3, 3.4 and 1.3 micrograms of
fluoride removed per gram of sorbent used , respectively (see  Table 11)
                                      72

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CO
                                           (49.5 mg/1, at 1.9 1)
                                       A
                                — Leachate
                                O Activated Alumina
                                   Fly Ash (Acidic)
                                   Fly Ash (Basic)
                                   Illite
                                   Vermiculite
                                                               Kaolinite
                 Figure 24.
                      Effluent Volume,  liters

Lysimeter Studies of Magnesium Ion  in Petroleum Sludge Leachate.

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   0.14
   0.12
2  0.10
CD
t~>
o
o
3
rfr
-S
c-l-
«j.
O
O
-h
               'I        ''                ''        I
             Q(0.54  mg/1, at 0.6 1)   '                '                '                '
                    (0 (0.24 mg/1, at 1.5 1)
        10.40  rag/1,   A           D(0.22  mg/1,  at 3.5 1)
          at  0.25 1)   *™?l SS(r    A          D (0.20 mg/1, at 5.5  1)
                                        (0.24 mg/l,              0(0.16 mg/1,  at  7.3 1)
                                         3 L 1 * _L •*- /
                                                             ._A	D	
   0.08
    0.06
    0.04
    0.02
                                             O
    Leachate
<^>  Activated Alumina
A  Activated Carbon
    Bottom Ash
    Fly Ash  (Acidic)
    Fly Ash  (Basic)
    Illite
    Kaolinite
    Vermiculite
                                        4                6
                                        Effluent Volume, liters
                                                                                       10
       Figure 25.  Lysimeter Studies of Zinc Ion in Petroleum Sludge Leachate.

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                    1.6
en
                G
                ID
               o
               o
               o
               n>
o
o
Leachate
Activated Alumina
Activated Carbon
Fly Ash (Acidic)
Fly Ash (Basic)
Illlte
Kaolinite
Vermiculite
                   0.4
                                                Effluent Volume,  liters
                  Figure 26.  Lysimeter Studies of Fluoride Ion in Petroleum Sludge Leachate.

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 Cyanide  Removal--
      The activated alumina, activated carbon, acidic and basic fly ashes, bot-
 tom  ash, illite-sand mixture, kaolinite-sand mixture, and vermiculite-sand
 mixture  were  investigated to determine their effectiveness in removing cyanide
 from petroleum  sludge leachate.  The results indicated that all the sorbents,
 with the exception of activated alumina and bottom ash, exhibited removals of
 the  cyanide (see Figure 27).  Their sorbent capacities were 2.9, 3.3, 3.3,
 15.5, 4.2, and  13.3 micrograms of cyanide removed per gram of sorbent used,
 respectively  (see Table 11).  The illite-sand mixture followed by the vermi-
 culite-sand mixture appeared to be the most effective based upon a comparison
 of the sorbent  capacities.  No removal of cyanide was obtained using either
 bottom ash or activated alumina.

 Organic  Removal--
     The activated alumina, activated carbon, bottom ash, basic and acidic
 fly  ashes, illite-sand mixture, kaolinite-sand mixture, and vermiculite-sand
 mixture  were examined to determine their effectiveness in removing organics
 from the petroleum sludge leachate, under flowing conditions.   The results
 indicate that all these sorbents exhibit some removal of the organics (see
 Figures  28 and  29).  A comparison of the sorbent capacities indicate that the
 vermiculite-sand mixture is the most effective in removal of COD and TOC,
 followed by the illite-sand mixture, basic and acidic fly ashes, activated
 carbon,  activated alumina, and bottom ash in decreasing order (see Table 11).

     It  should  be noted from the sorbent capacities that the vermiculite-sand
 mixture  is significantly more effective than the activated carbon in removing
 the  organics from this leachate for the 10 liters of leachate added to these
 lysimeters.  This finding is significant in that activated carbon is consider-
 ed to be an effective sorbent for the removal of organics from waste streams.

 Permeability Results—
     The type of leachate being treated by a sorbent has a significant effect
 on the permeability of the sorbent, with the exception-of activated carbon.
 The  initial magnitude of the coefficient of permeability exhibited by the
 activated carbon was not influenced by the leachate (see Figure 19).  Also,
 it did not change significantly upon the addition of leachate.  On the other
 hand, the activated alumina decreased markedly upon the addition of the lea-
 chate (see Figure 30).  The coefficient of permeability for bottom ash also
 exhibited a parallel behavior.

     The coefficient of permeability for acidic and basic fly ashes, illite-
 sand mixture and vermiculite-sand mixture in general exhibited far less var-
 iation upon the addition of the petroleum sludge leachate than either the
 activated alumina or bottom ash.   The coefficient of permeability for the
 kaolinite initially was much lower than the above sorbents.   However, it ex-
 hibited  less of a decrease upon the addition of leachate than  either the bot-
 tom ash or activated alumina.

Summary of Results

     The basic fly ash, the vermiculite-sand mixture and the kaolinite-sand
mixture appear to be the most effective sorbent combination for treating the

                                     76

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    0.25
-t>
-Jj
to
o
o
o
n>
-s
Q>
O

O
-h
o
    0.20
0.15
0.10
    0.05
O
A
O
®
9
D
O
Leachate
Activated Alumina
Activated Carbon
Bottom Ash
Fly Ash  (Acidic)
Fly Ash  (Basic)
Illite
Vermiculite

Kaolinite
        0            2            4            6           8           10

                                    Effluent Volume, liters

Figure 27.  Lysimeter Studies of Cyanide Ion in Petroleum Sludge Leachate.
                                                                            12

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                300
            o
            ft)
            01
            O
            -h
            O
            O
200
00
                100
                                       	 Leachate
                                       O  Activated Alumina
                                           Activated Carbon
                                           Bottom Ash
                                           Fly Ash (Acidic)
                                           Fly Ash (Basic)
                                           Illite
                                           Vermiculite
                                                       A
                                                       O
                                                        D
                                                        O
                                                                         t
                                                  468
                                                      Effluent  Volume, liters
                                                                               10
12
                                    Figure 28.  Lysimeter Studies of COD  in  Petroleum  Sludge Leachate.

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               160
               120
          o
          o
vo
                                                                      	 Leachate
                                                                          Activated Alumina
    Activated Carbon
O  Bottom Ash
41  Fly Ash (Acidic)
•  Fly Ash (Basic)
G  Illite
o  Vermiculite
                                                               6              8
                                                      Effluent Volume, liters
                         Figure 29.  Lysimeter Studies  of TOC in  Petroleum Sludge Leachate.
                                                                                                            12

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             10
     u
     OJ
     to
     o
     •p
     
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petroleum sludge leachate.   The basic fly ash would be used  for  removing  the
copper and fluoride, the vermiculite-sand mixture for the  calcium,  zinc,  cya-
nide and the organics and the kaolinite-sand mixture for removing the magnesium
ion.

     The kaolinite-sand mixture is significantly more effective  than the  other
sorbents for removing the magnesium ion based upon a comparison  of  the  sorbent
capacities.  Hence, it is included in the above combination  even though it
exhibited leaching of zinc ion.  The presence of a significant amount of  ver-
miculite-sand mixture in a layered system could minimize this  problem.

     Although illite was found to be the most effective for  the  removal of
calcium, fluoride and cyanide based upon a comparison of the sorbent capaci-
ties, the illite does not show promise because it exhibited  leaching of copper
and zinc in over half of the effluent fractions collected  from the  lysimeter.
Similarily, the acidic fly ash was found to be the most effective for the re-
moval of the copper and the next most effective for fluoride,  but it was  not
selected because in over two-thirds of the effluent fractions  that  were analy-
zed for magnesium, the acidic fly ash showed leaching of this  ion.
                                      81

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                                   REFERENCES


 1.  Deb, P.K., A.J. Rubin, A.W. Launder, and K.H. Mancy, (1966), "Removal of
     C.O.D. from Wastewater by Fly Ash" Engineering Bull., Purdue University,
     No. 121.

 2.  Nelson, M.D. and Carmen F. Fuarino, (Nov. 1969), "The Use of Fly Ash in
     Municipal Waste Treatment," Journal WPCF, Vol. 41, No.  11, pt. 1, pgs.
     1905-1911.

 3.  Ballance, R.C., J.P. Capp and J.C. Burchinal, (1966), "Fly Ash as a
     Coagulant Aid in Water Treatment" U.S. Dept. Interim, Bureau of Mines,
     Report of Investigations - 6869.

 4.  Grim, Ralph E., (1967), Clay Mineralogy (2nd Ed.), McGraw Hill Book Co.,
     Inc., New York.

 5.  Brown, G. (ed.), (1961), The X-Ray Identification and Crystal Structures
     of Clay Minerals, Jarrold and Sons, Ltd., Norwich.

 6.  Fried, M. and R.E. Shapiro, (1956), "Phosphate Supply Pattern of Various
     Soils," Soil Sci. Soc. Am. Proc., Vol. 20, p. 471-475.

 7.  Olson, Sterling R. and Frank S. Watanable, (1957), "A Method to Determine
     a Phosphorous Absorption Maximum of Soils as a Measure  by the Langmuir
     Isotherm," Soil Sci. Soc.  Am. Proc., Vol. 21, p. 144-149.

 8.  Ellis, B.G.  and A.E. Erickson, (1969), "Movement and Transformation of
     Various Phosphorous Compounds in Soils," Report to Michigan Water Resources
     Commission.

 9.  Tiller, K.G., (1967), "Silicic Acid and the Reactions of Zinc with Clays,"
     Nature, Vol. 214, p. 852.

10.  Sharpless, R.G., E.F. Wallihan, and E.F. Peterson, (1969), "Retention of
     Zinc by Some Arid Zone Soil Materials Treated with Zinc Sulfate," Soil Sci.
     Soc. Am.  Proc., Vol. 33, p. 901-904.

11.  Bittel, J.E. and Raymond J. Miller (1974), "Lead, Cadmium, and Calcium
     Selectivity, Coefficients  on a Montrnorillonite.  Illite, and Kaolinite,"
     J. Environ.  Quality, Vol.  3, No. 3, p. 250-253.

12.  Fuller, Wallace H., Collen McCarthy, B.A. Alesii, and Elvia Niebla,"
     (1976), "Liners for Disposal Sites to Retard Migration  of Pollutants,"
     Residual  Management by Land Disposal, Proc.  Hazardous Waste Research

                                       82

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     Symposium, U.S.E.P.A.,  p.  112-126.

13.   Griffin, R.A., R.R.  Frost  and N.F.  Shimp,  (1976)," Effect of pH on  Removal
     of Heavy Metals from Leachates by Clay Minerals," Residence Management by
     Land Disposal, Proc.  Hazardous Waste Research Symposium, U.S.E.P.A.,
     p. 259-268.

14.   McHenry, J.R., D.W.  Rhodes and P.P. Rowe,  (Dec.-1955),  "Chemical  and
     Physical Reactions of Radioactive Liquid Wastes  with Soils," in Sanitary
     Engineering Aspects  of the Atomic Energy Industry, A.E.G. Publication No.
     TID-7517, Cincinnati, Ohio.

15.   Likens, Gene E., (Nov.  22, 1976), "Acid Precipitation", Chemical  and
     Engineering News, pp. 29-44.

16.   E.P.A.  (1974), Methods of Chemical  Analysis of Water and Waste,"  U.S.E.P.-
     A. Tech. Transfer, Cincinnati, Ohio.

17.   Scott,  R., (1963), Principles of Soil Mechanics. Addison-Wesley Publish-
     ing Co., Waltham, Mass.

18.   U.S. Public Health Service, 1962 Public Health Service Drinking Water
     Standards PHS Pub. No.  956, Washington, D.C.
                                      83

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing)
 1. REPORT NO.
   EPA-600/2-78-024
                                                          3. RECIPIENT'S ACCESSION'NO.
 4. TITLE ANDSUBTITLE
   SORBENTS FOR FLUORIDE, METAL FINISHING,  AND PETROLEUM
   SLUDGE LEACHATE CONTAMINANT CONTROL
              5. REPORT DATE

              March 1978 (Issuing
              6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
   Paul  C.  Chan, Robert Dresnack, John  W.  Liskowitz
   Angelo Perna, Richard Trattner
                                                          8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS

   New Jersey Institute of Technology
   Newark, New Jersey  07102
                                                           10. PROGRAM ELEMENT NO.
                  1BB610
              11. CONTRACT/GRANT NO.
                                                              B803717
 12. SPONSORING AGENCY NAME AND ADDRESS
   Municipal  Environmental Research Laboratory—Gin.,OH
   Office of  Research and Development
   U.S.  Environmental Protection Agency
   Cincinnati, Ohio  45268
              13. TYPE OF REPORT AND PERIOD COVERED
                Final  report 6/75 to 5/77
              14. SPONSORING AGENCY CODE
                  EPA/600/14
15. SUPPLEMENTARY NOTES
   Project Officer:  Fred Ellerbusch
   Contact:  Robert E. Landreth  (513)  684-7871
16. ABSTRACT
     This  report  covers the initial laboratory studies  carried out to identify the most
Dromising  sorbents  that may be used to significantly  reduce the concentration of meas-
urable contaminant  in  calcium fluoride sludge leachate,  metal  finishing sludge leachate
and petroleum  sludge leachate.  Laboratory evaluations were made of bottom ash, acidic
and basic  fly  ashes, vermiculite, illite, activated carbon, kaolinite, natural zeolite,
activated  alumina,  and cullite for the removal of contaminants in the leachate and
liquid portion of these three industrial sludges.

     Batch and lysimeter studies were carried out to  evaluate  the static and dynamic
 orbent capacity  for the constituents present in the  leachate.   Permeability exhibited
by these sorbents when contacted with an industrial sludge  leachate was also studied.
 he pH, conductivity,  chemical oxygen demand (COD), total organic carbon (TOC), cationii
and anionic species  in the leachate before and after  contact with the sorbent materials
and the coefficient  of permeability were determined.

     Considerable variations in composition and concentration  of leachate constituents
vere shown.  Batch and lysimeter studies revealed that no single sorbent could be used
to reduce the  concentration of the constituents found in the leachate of a specific
 ludge; rather, combinations of two or more sorbents  could  be  used.
 7.
                               KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
 b.IDENTIFIERS/OPEN ENDED TERMS C.  COS AT I Field/Group
           Leaching
           Pollution
           Waste treatment
           Linings
           Sorbents
   Solid  waste management
   Industrial  sludaes
13B
 3. DISTRIBUTION STATEMEN1
   RELEASE TO PUBLIC
 19. SECURITY CLASS (ThisReport)
   UNCLASSIFIED
                                                                        21. NO. OF PAGES
94
                                             20. SECURITY CLASS (Thispage)
                                                UNCLASSIFIED
                                                                        22. PRICE
EPA Form 2220-1 (9-73)
84

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