vVEPA
                                 United States
                                 Environmental Protection
                                 Agency
                                 Industrial Environmental Research
                                 Laboratory
                                 Cincinnati OH 45268
                                 Research and Development
                                 EPA-600/S2-81-043  Apr 1981
Project  Summary
                                 Removal  of  Phenolic
                                 Compounds  From  Wood
                                 Preserving  Wastewaters

                                 Bruce K. Wallin, Arthur J. Condren, and Roy L. Walden
                                  Laboratory and pilot-scale studies
                                were undertaken to  develop
                                economically  feasible technologies
                                for the treatment of wastewaters from
                                wood preserving operations. Of prime
                                concern was the  removal  of phenol
                                and  its chlorinated  derivatives,  in
                                particular, pentachlorophenol.
                                Screening analysis of the wastewater
                                indicated that pentachlorophenol was
                                the only chlorinated derivative con-
                                sistently present in concentrations of
                                approximately 100 mg/l.
                                  Treatment  technologies  investi-
                                gated for  the treatment  of these
                                wastewaters included:

                                 1.  adsorption;
                                 2.  biological oxidation;
                                 3.  chemical oxidation;
                                 4.  coagulation;
                                 5.  extraction; and
                                 6.  pH adjustment.

                                  Each  of  the above, alone or  in
                                combination, was capable of yielding
                                a measurable reduction in the concen-
                                tration of  total phenols and penta-
                                chlorophenol in the untreated waste-
                                water.
                                  Two technologies  yielded consis-
                                tently high levels of treatment:
                                    pH  adjustment of the  waste-
                                    water, followed by adsorption
                                    with bentonite clay and final
                                    polishing  by  the  polymeric
                                    adsorbant, XAD-4; and
                                  2.  pH adjustment  of the waste-
                                     water,  followed by extraction
                                     with a mixture of #2 fuel oil and a
                                     co-solvent such as still bottoms
                                     from amyl alcohol production.

                                  Total annual operating costs for
                                 systems treating a typical 10,000 gpd
                                 of wastewater were calculated to be
                                 $40,000 and $23,600, respectively,
                                 for the two aforementioned technol-
                                 ogies.
                                  This report was submitted in fulfill-
                                 ment of Contract No. 68-03-2605,
                                 Work Directive No. 2, Parts 1 and 5,
                                 by the  Edward C. Jordan Co., Inc.,
                                 under the sponsorship  of the U.S.
                                 Environmental Protection  Agency.
                                 This  report covers the period Novem-
                                 ber 20, 1978 to May 20, 1980, and
                                 work was completed as of  May 20,
                                 1980.
                                  This Project Summary was develop-
                                 ed by EPA's Industrial Environmental
                                 Research Laboratory. Cincinnati, OH.
                                 to announce key findings  of the
                                 research report  that is fully docu-
                                 mented in a separate report of the
                                 same title (see Project Report ordering
                                 at back).

                                 Introduction
                                  The U.S. Environmental Protection
                                 Agency has been involved in extensive
                                 investigations of toxic compounds being
                                 discharged from  industrial facilities.
                                 Primary emphasis has  been on the 65
                                 "priority" pollutants, which are  con-
                                 tained in the Settlement Agreement of

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1976 and in the Clean Water K
1977 (PL 95-217). Phenolics and U,
chlorinated derivatives are a part of thiL
group and are commonly found in  the
wood products industry's wastewater
streams.
  The initial objective of this study was
to evaluate  the treatability of 2,4,6-
trichlorophenol, parachlorometacresol,
2-chlorophenol,    2,4-dichlorophenol,
and  pentachlorophenol in the wood
products industry's wastewater  The
wood preserving industry was selected
for this program  because wastewater
from  wood  preserving  facilities  is
usually low in volume but high in con-
centrations of chlorinated phenolics. A
chemical screening of the wastewater
revealed that it had a high organic con-
tent, but more significantly, it contained
pentachlorophenol  in  concentrations
exceeding 100 mg/l.  The program's
focus then shifted primarily to penta-
chlorophenol to the virtual exclusion of
all else, since only trace levels  of other
chlorinated phenolics were found.
  In  conjunction  with  the  treatability
aspect, the program was intended also
to  explore  atypical  pretreatment
schemes that would reduce chlorinated
phenolics, namely pentachlorophenol,
in typical wood preserving wastewater
to levels at which the wastewater could
be  discharged to  a   POTW  without
causing an upset  Owing to constraints
imposed by time and financial resources,
it was not the objective of this program
to investigate all aspects of each treat-
ment scheme (e g.,  residual  catalyst
after  PCP  removal,  toxicity  of   the
removal concentration, adsorptive
capacity of the regenerated resin). The
objective here was also not to improve
the  phenol-contaminated  wastewater
to drinking  water quality,  nor was it
within the bounds of the study to make
any conclusions concerning the toxicity
of the residual pentachlorophenol con-
centration in the wastewater that would
be discharged to the POTW.
  The physical/chemical properties of
pentachlorophenol,  as distinguished
from those of phenol, were important in
considering  the pretreatment systems
which would  be  capable of reducing
concentrations to an acceptable level.
Pentachlorophenol consists of a ben-
zene  ring (CeH6) with  all  six hydrogen
sites substituted by one hydroxyl group
(OH) and five chlorine atoms (CU). The
resulting compounds, CeCUOH,  is mildly
acidic, boils  at 309°C, and is soluble in
50°C water  at 30 mg/l Oils or emul-
                                c
                                .o

                                •8
                                .0
                                CU
                                (J
to
ID
Oc
t3
tb
i/i
<0
5)
b
                      ol
          2,4-Dichlorophenol
     a    2,4,6-Trichlorophenol
     0    Pentachlorophenol

 Figure 1.     Phenolic resistance to
              biodegradation (2).

sions  in wastewater can provide a
"carrier" effect, allowing pentachloro-
phenol to far exceed its normal solubility
in  water.  Table  1  summarizes  the
physical properties of several phenolic
compounds. Figure 1 presents phenolic
structures for  several compounds.
  A  review  of  available  literature
assisted the investigators in identifying
treatment techniques foi investigation.
Investigations  were  divided into two
phases, preliminary bench-scale treat-
ability studies and  an  evaluation  of
batch treatment techniques.
  Unlike  phenol,   which  is  quite
unstable  and  easily  oxidized  either
chemically or biologically, pentachloro-
phenol is stable and resistant to oxida-
tion  In  some instances, though, when
wastewater  containing  pentachloro-
phenol  in  concentrations  which  a
biomass can tolerate is run through a
biological treatment system, pentachlo-
rophenol is adsorped onto the biofloc.
Disposal of the sludge, now laden with
pentachlorophenol,  then  presents  a
hazardous  waste  problem. Alkyliniza-
tion of the  sludge, a relatively common
practice, would more than likely release
the pentachlorophenol intotheenviron-
ment If the sludge were incinerated,
2,3,7,8-tetrachlorodibenzo-p-dioxm,  a
thermal degradation product of penta-
chlorophenol, could be released into the
atmosphere.
  These  rather   ominous  prospects
make such treatment techniques as
solvent  extraction and batch polymeric
resin adsorption,  two schemes investi-
gated during this study, more appealing
from  the   standpoint of  avoiding the
creation of a hazardous waste problem
while improving water quality
  In   the   preliminary bench-scale
studies  the investigators  traveled to a
wood preserving  facility  on the  west
coast to evaluate treatment technol-
ogies,   described  m  the  literature,
designed to  lower pentachlorophenol
concentrations   Treatment  schemes
tested  included  pH  reduction,  acid
cracking, chemical coagulation, chemi-
cal   oxidation,   ultrafiltration,  resin
adsorption, and solvent extraction
  After  conducting  the  preliminary
bench-scale studies, the investigators
reported to representatives of the EPA.
Table 1.     Physical Properties of Several Phenolic Compounds
Compound
Phenol
o-Chlorophenol
m-Chlorophenol
p-Chlorophenol
2,4-Dichlorophenol
2,4,6-Trichlorophenol
Pentachlorophenol
o-Cresol
m-Cresol
p-Cresol
p-Chloro-m-Cresol
2. 4, 6- Trichloro-m-Cresol
Boiling Point
°C
182
173
214
220
210
246
309
191
201
202
196
265
Solubility in H2O
mg/l @ 25° C
93,000
28.000
26.000
27,000
4,500
900
30(50°C)
25.000
26,000
23,000
insol.
si. sol.
Ka x 10'°
1.1
77.0
16.0
6.3
Large
Very Large
Very Large
0.63
0.98
0.67
Unknown
Unknown
Ka = thermodynamic acid dissociation constant

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At  this time,  mid-course corrections
were suggested  It was suggested that
the  program emphasis  be shifted to
focus  on  only  those   pretreatment
systems that would both lower pervta-
chlorophenol concentrations to levels
acceptable for discharge to a POTW and
be economically feasible for wood pre-
servers
  To meet the revised criteria, pretreat-
ment schemes had to be both efficient
and  economically  feasible,   which
essentially eliminated from considera-
tion  the  more  elaborate  treatment
technologies (e.g., reductive degrada-
tion,  electrochemical  oxidation,  ion
exchange, rotary vacuum filtration with
activated carbon) The effectiveness of
these cannot be denied,  but the cost of
installing and operating any one of them
makes it economically impractical for
wood preservers.
  Batch treatment  systems were set up
at the southern facility to provide some
indication of which methods were cost
effective.  Technologies  tested  at the
southern facility included batch biolog-
ical treatment, chemical and polymeric
coagulation,  resin  adsorption,  acid
cracking, bentonite clay, solvent extrac-
tion, and filtration.  As at the west coast
facility, a  combination of these were
tested The size of  the batch treatment
reactors ranged from  several litersto 50
gallons, depending on the pretreatment
system being tested.
Summary and Conclusions
  Processes for the treatment of waste-
waters  from  two  wood  preserving
facilities  were  investigated at  the
laboratory and pilot scale  levels  In-
cluded were various chemical, physical,
and   biological  operations  selected
specifically for the removal of phenol
and its chlorinated derivatives. Of the
treatment technologies  investigated,
two systems  consistently lowered the
concentrations of pentachlorophenol in
the wastewater from 100 mg/l to less
than 1 mg/l.
  In the  first system, the wastewater
was first acidified to a pH of 4.0 ± 0.1,
then  bentonite  clay  was  added. A
polymeric adsorbant, amberlite XAD-4
was used in the final polishing process.
In the second system a mixture of No. 2
fuel oil and a cosolvent (amyl alcohol
still bottoms) was used to extract penta-
chlorophenol from the waste stream.
Reductions were consistently in excess
of 99 percent. Since No. 2 fuel oil is used
often in  the preserving  process, as it
was at this facility, it is conceivable that
a facility could operate this extraction
process  without  incurring  any
additional chemical  expense,  except
possibly for  the cosolvent. Trials with
No. 2 fuel oil alone yielded removal ef-
ficiencies in the vicinity of 97 percent,
which may be high enough to allow the
wastewater  to  be discharged  to  a
POTW. For  both systems to function
consistently, the wastewater first had to
be subjected to free oil separation and
flow  equalization.The following
summarizes the findings of other inves-
tigations,  based on reductions in total
phenol and/or pentachlorophenol con-
centrations.
pH Adjustment
  Lowering the pH of the wastewater
with sulfuric acid was found to induce
the formation of colloidal material. Sub-
sequent removal of this colloidal mate-
rial resulted in slight reductions in total
phenol concentrations as measured by
the modified lowry procedure described
in the  Project  Report.  Pentachloro-
phenol concentrations, however, were
consistently reduced  from  approxi-
mately 100 mg/l to less than 20 mg/l.


Biological Oxidation
  Biological oxidation was not found to
be an effective treatment technique be-
cause  bioadsorption  rather  than  bio-
transformation  was  found to be the
primary removal mechanism. Removal
rates  continued  to  diminish  as  the
adsorptive capacity of the biomass was
approached


Chemical Oxidation
  At high doses, chlorine  yielded  sub-
stantial reductions in the compounds of
concern. Hydrogen peroxide,  on the
other hand, had little effect. The  high
chemical demand observed  precludes
the use of chemical oxidation as a viable
treatment alternative


Coagulation
  Coagulation  with   alum, ferric
chloride,  and/or polymers resulted in
modest pollutant  reductions.  These
reductions were not deemed sufficient
to justify coagulation  as a sole treat-
ment technology.
Applicability of Technologies
  In turning now to the applicability of
the programs' findings to the wood pre-
serving industry as a whole, it should be
understood that the utility of any single
pretreatment option is contingent upon
both the volume and chemical make-up
of the waste  stream. Because wood
preserving  processes are so variant,
each facility must be evaluated in terms
of its  preserving process,  its  waste
stream,  and the  capital  available  for
investing in a pretreatment system The
systems devised for wood preservers in
connection with this study would prob-
ably not be transferable to the leather
tanning industry or to the paper indus-
try, not because a No. 2 fuel oil - cosol-
vent mixture would  not remove penta-
chlorophenol from leather tanning or
paper  industry   effluent  just  as
effectively as it would from wood pre-
serving   wastewater,  but   because
neither of these industries uses No. 2
fuel oil in its production  process (non-
combustion) as do some members of the
wood  preserving   industry  The
advantage  of  the fuel  oil  extraction
process is that the pentachlorophenol
can be removed from the wastewater
without creating  an additional  waste
and without bringing large capital and
operating expense to bear on the wood
preserver.
Recommendations
  If  results  obtained  during  these
investigations  are to  be verified,  a
continuously flowing pilot-scale system
must be established. Because this study
was  done on  a  quick response basis
with  limited  financial  resources,
researchers  could not investigate all
aspects of each  pretreatment scheme
(e.g., residual catalyst after pentachlo-
rophenol removal, toxicity of removal
concentrations, utility or necessity of
catalysts other than  amyl alcohol still
bottoms). Instead, the project provided
an overview of the many economically
achievable  approaches   to  removing
pentachlorophenol from  wastewater
and identified  two systems especially
successful  in  lowering  pentachloro-
phenol  concentrations in wood  pre-
servers'  wastewater to  levels  that
would allow it to be  discharged to the
POTW without causing an upset.
            : US GOVERNMENT PRINTING OFFICE 1981 757-012/7060

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       Bruce K Walhn, Arthur J Condren, and Roy L Wa/den are w/th the Edward C
         Jordan Co , Inc , Portland, ME 0417 2
       Donald L.  Wilson and Brian West fall are the EPA Project Officers (see below)
       The complete report, entitled "Removal of Phenolic Compounds from Wood
         Preserving Wastewaters, "(Order No  PB81 -172637, Cost $12 50,subjectto
         change) will be available only from
               National Technical Information Service
               5285 Port Royal Road
               Springfield, VA 22161
               Telephone  703-487-4650
       The EPA Project Officers can be contacted at
               Industrial Environmental Research Laboratory
               U S Environmental Protect/on Agency
               Cincinnati,  OH 45268
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
Postage and
Fees Paid
Environmental
Protection
Agency
EPA 335
Official Business
Penalty for Private Use $300

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