D A u-s- Environmental Protection Agency Industrial Environmental Research      EPA
-• •» Office of Research and Development Laboratory                _  ..
                     Research Triangle Park, North Carolina 27711 April
                              EPA-600/7-77-034
METHOD FOR ANALYZING
EMISSIONS FROM ATMOSPHERIC
FLUIDIZED-BED COMBUSTOR
Interagency
Energy-Environment
Research and Development
Program Report

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                       RESEARCH  REPORTING  SERIES
Research reports of the Office of  Research and Development, U.S.
Environmental Protection Agency, have  been grouped into seven series.
These seven broad categories were  established to facilitate further
development and application of environmental technology.  Elimination
of traditional grouping was consciously  planned to foster technology
transfer and a maximum interface in  related fields.  The seven series
are:

     1.  Environmental Health Effects  Research
     2.  Environmental Protection  Technology
     3.  Ecological Research
     4.  Environmental Monitoring
     5.  Socioeconomic Environmental Studies
     6.  Scientific and Technical  Assessment Reports (STAR)
     7.  Interagency Energy-Environment  Research and Development

This report has been assigned to the INTERAGENCY ENERGY-ENVIRONMENT
RESEARCH AND DEVELOPMENT series.   Reports in this series result from
the effort funded under the 17-agency  Federal Energy/Environment
Research and Development Program.  These studies relate to EPA's
mission to protect the public health and welfare from adverse effects
of pollutants associated with energy systems.  The goal of the Program
is to assure the rapid development of  domestic energy supplies in an
environmentally—compatible manner by  providing the necessary
environmental data and control technology.  Investigations include
analyses of the transport of energy-related pollutants and their health
and ecological effects; assessments  of,  and development of, control
technologies for energy systems; and integrated assessments of a wide
range of energy-related environmental  issues.

                            REVIEW NOTICE

This report has been reviewed by the  participating Federal
Agencies, and approved for publication. Approval does riot
signify that the contents necessarily reflect the views and
policies of the Government, nor does  mention of trade names
or commercial products constitute endorsement or recommen-
dation for use.
This document is available to the public through the  National  Technical
Information Service, Springfield, Virginia  22161.

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                                 ABSTRACT

     A methodology for comprehensive sampling and analysis of emissions
from an atmospheric fluidized-bed combustor has been developed and tested
experimentally.  The methodology tested is a first attempt to develop an
approach to the Level 1 methodology as defined by TRW and is aimed at
providing a cost and information effective environmental assessment of
fluidized-bed combustion (FBC) units.  Included in the report is a general
discussion of the pertinent areas likely to be encountered in sampling
and analyzing specimens from FBC units, as for example, the streams
encountered in FBC units, the selection of streams, procedures for sampling
the gaseous, solid, and liquid streams, and the multi-level analysis
approach to characterization of emissions from combustion units as
defined by EPA.
     The adopted experimental methodology was put into practice, using
Battelle's 6-inch atmospheric FBC unit.  The details involved in sampling
and analyzing the samples from the 6-inch FBC unit are discussed in relation
to (1) the preparatory work, i.e., background information, site survey,
development of a sampling and analysis plan, installation of equipment,
and shake down runs, (2) sampling procedures involved with the FBC unit,
and (3) analyzing the samples taken from the FBC unit.  The analytical
data obtained from two runs made with the unit are presented and
discussed, mainly in terms of the trace element data obtained.  These
data and other pertinent gaseous and particulate data are compared to
data obtained from other FBC and/or conventional fired units.  The
report concludes with the presentation of a generalized sampling and
analysis plan to be used as a guide in characterizing the emissions
from FBC units.
                                    iii

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                                  CONTENTS
Abstract	
Figures   	     v
Tables  	     v

     1.  Introduction and Objectives  	     1
     2.  Preliminary Plan Development 	     2
            Technical Background - Review of Sampling Analysis
              Procedures and Concepts 	     2
                 Selection of Influent and Effluent Streams ....     2
                 Sampling Procedures for Solid, Liquid, and
                   Gaseous Streams  	     5
                 Sampling and Analysis Strategy 	     8
                 Sample Preservation and Handling 	    10
                 Quality Control in the Sampling Program  	    12

     3.  Methodology Development  	    14
            Development of a Comprehensive Sampling and Analysis
              Plan	    14
                 Background Information 	    14
                 Sampling and Analysis Plan	    18
                 Site Survey	    18
                 Installation and Operation of Equipment  	    22
                 Shake Down Runs	    25
            Collection and Preparation of Samples for Analysis  .  .    25
                 Sampling 	 .....    27
                 Sampling Problems  	    32
                 Labeling	    32
                 Analyses of Samples	    32
                 Additional Considerations in the Analyses of
                   Samples	    32
                 Analyses Problems  	    35

     4.  Evaluation of Emission Data	    36
                 General	    38
                 Trace Elements	    38

     5.  Recommended Sampling and Analysis Plan	    45
            Areas Needing Further Study and/or Consideration  ...    47

References	    49
Appendix	    50
                                    iv

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                                  FIGURES

                                                                      Page

1.  Generalized Fluidized Bed Combustion System 	     4

2.  Scale Drawing of 6-In. Fluidized Bed Combustor  	    16

3.  6-In. Fluidized Bed Combustor 	    17

4.  Flue Gas Analyzer Flow Schematic	    23

5.  Typical Gas Absorption Train  	    26

6.  Schematic Outline of Fluidized Bed Combustor and Sampling
    Locations	28
                                  TABLES

1.  Stream Identification for Generalized FBC System  	     3

2.  General Characteristics of Phased Level 1-Level 2 Strategy  .  .    11

3.  FBC Sampling — Analysis Plan	    19

4.  Sample Identification and Analyses  	    33

5.  Changes Made Between Run Nos. 1 and 2	    37

6.  Comparison of Data from Fluidized Bed and Pulverized Coal
    Combustion	    39

7.  Comparison of Trace Element Data from Coal and Ash of Illinois
    No. 6 Coal	    40

8.  Comparison of Trace Elements in Coals and Coal Products ....    41

9.  Sampling and Analysis Matrix for Comprehensive Analysis of
    FBC Streams	    46

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                                SECTION 1
                        INTRODUCTION AND OBJECTIVES

     Fluidized-bed combustion (FBC) offers specific advantages over other
coal-fired combustion processes in that it provides high thermal efficiency
and capability for in-situ antipollution control.  Total environmental
assessments of FBC processes are only now being initiated, thus compre-
hensive procedures for collecting and analyzing FBC emission products as
well as reactant products are needed.  The objective of this program was
to develop and test primarily a Level 1 methodology* for comprehensive
analysis of emissions from an atmospheric FBC unit and to consider the
application to pressurized fluidized-bed combustors as well as to other
coal-burning processes.
     This report summarizes a program carried out under Task 33, EPA
Contract No. 68-02-1409.  The emphasis in this program was mainly on
establishing a general methodology for comprehensive sampling-analysis
from FBC units and not to define the precision and/or accuracy of the
techniques employed.  To achieve the overall objective of the program,
four distinct phases were considered.  These were:
     A.  Developing a preliminary approach for comprehensive analysis
     B.  Designing and conducting a test program
     C.  Evaluating the emission data
     D.  Refining the preliminary comprehensive analysis approach.
     Along with developing the general methodology, the development was
tested using Battelle's 6-inch fluidized-bed combustor.
*  Level I methodology similar to that defined by TRW  (1); all references
   are on page 49.

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                                 SECTION  2
                       PRELIMINARY  PLAN DEVELOPMENT

     At the time this  program was undertaken two  pertinent^ activities were
in progress.   MITRE Corporation (2) was completing a state-of-the-art
survey of fluidized-bed sampling and analysis procedures  and was developing
guidelines for carrying out these procedures, and IERL/RTP (3)  was in
process of formalizing the Level 1-2-3 sampling-analysis  concepts.  Both
of these programs impacted on this  program  and provided useful  background
information.   Pertinent information in these program is reviewed here.
TECHNICAL BACKGROUND - REVIEW OF SAMPLING
ANALYSIS PROCEDURES AND CONCEPTS
     The MITRE report* is pertinent to this sampling program in that it
presents a detailed up-to-date study of the tentative procedures for
environmental assessment of fluidized-bed units.   The primary objective
of the work covered in the MITRE report was to develop sampling and
analysis procedures for use by source contractors in support of the environ-
mental assessment of fluidized-bed  combustion technology.  The review
presented here covers  briefly the areas of  interest  to this program, i.e.,
sampling and analyses  procedures and concepts, and constituents likely
to be encountered in fluidized-bed  sampling.  Pertinent information from
a Battelle planning study report (4) is included in  the review.
Selection of Influent  and Effluent  Streams
     In order to characterize the emissions from combustion processes, it
is important  to consider all possible streams in the combustion system
which may lead to pollutant formation.   In  the case  of the FBC units, a
total of 30 different  streams have  been  recognized as possible sources of
pollutants.  The 30 streams are shown in  Table 1.  The relationship of
the various streams to a generalized FBC  system is shown in Figure 1.
*  The review  covered  in  this  report is  from the First Draft of the MITRE
   report.  A  Second Draft  of  the  report has been completed  and some changes
   are likely  to have  been made.

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       TABLE 1.  STREAM IDENTIFICATION FOR GENERALIZED FBC SYSTEM
Stream No.                             Stream Identification
   1        Stack Gas from FBC
   2        Particulate Removal Discard from FBC
   3        Bed Solids Discard from FBC
   4        Particulate Removal Discard—Regeneration Operations
   5        Other Effluents from Regeneration and Sulfur Recovery Operations
   8        Product from Sulfur Recovery (Sulfur or Sulfuric Acid)
   9        Fugitives from Fuel Preparation
  10        Fugitives from Sorbent/Additive Preparation
  11        Raw Fuel to Preparation
  12        Raw Sorbent/Additive to Preparation
  14        Air to Combustor
  15        Air/Steam to Regenerator
  16        Fuel Feed to FBC
  17        Fuel Feed to Regenerator
  18        Start-Up Fuel Feed to FBC
  19        Prepared Sorbent/Additive Feed to FBC
  20        Bed Solids to Regenerator
  21        Flue Gas from FBC to Particulate Removal
  23        Recycle of Particulates from Particulate Removal to FBC
  24        Recycle of sorbent from Regeneration
  31        Fugitive or secondary Emission from Fuel Storage Facility
  32        Fugitive or Secondary Emission from FBC Discard Bed Material
  33        Fugitive or Secondary Emission from FBC Particulate Disposal
  34        Effluent Gas from Secondary Stack Gas Cleaning Device (Similar to
              Streams 25 & 26 in MITRE Study)
  35        Discard from FBC Secondary Stack Gas Cleaning Device
  36        Flue Gas from Regenerator to Particulate Removal
  37        Fugitive or Secondary emission from Regeneration Bed Discard
  38        Stack Gas from Regenerator to Sulfur Recovery Operations
  39        Fugitive or Secondary Emissions from Regenerator Particulate Disposal
  40        Fugitive or Secondary Emissions from Sorbent Storage Facility

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  SORBENT/
  ADDITIVE
PREPARATION
 OPERATIONS
AND STORAGE
                                                                                              SECONDARY
                                                                                              STACK GAS
                                                                                              CLEANING
                                                                                              DEVICE
                                           FUELS
                                         PREPARATION
                                           OPERATIONS
                                         AND STORAGE
                                                                                              SULFUR
                                                                                              RECOVERY
                                                                                              OPERATIONS
PARTICIPATE
  REMOVAL
 OPERATIONS
 (CYCLONES)
                                                                                          DISPOSAL
                                                                                          OPERATIONS
                       FIGURE 1.  GENERALIZED FLUIDIZED BED COMBUSTION SYSTEM

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The numbering system has been adopted from MITRE.  '
    Many  of  the  streams  listed  in  the table  are  encountered  in  combustion
processes other  than  FBC units  and would  be  considered  there as appropriate.
On  the  other hand,  some  streams encountered  in some  FBC units have been  in-
tentionally  omitted from Table  1 on  the basis of their  low priority, or  be-
cause they apply to units  which were judged  inappropriate for inclusion  in
this study program, e.g.,  the CAFB units.
    For each FBC unit sampled,  certain criteria  should  be considered before
selecting or rejecting a sample stream.   Overall,  stream characterization
should  be made when:
     •  A direct emission  stream is  representative of a FBC process
        release  to  the environment
     •  A feed or supply stream will significantly affect direct
        emissions
     •  A within-process stream might significantly affect an emission
        stream or the performance  of an emission control device
     •  A fugitive  emission is  identified, or suspected, which might
        be characteristic  of a  reduced-to-practice FBC unit
     •  A secondary emission is simulated in a supplementary test
        involving a supply or effluent stream.

Sampling  Procedures for  Solid,  Liquid, and Gaseous Streams
     Many of the  selected  streams  will require special  sampling techniques.
The following discussion is a synopsis of the recommended techniques to be
used in sampling  solid,  liquid, and  gaseous  streams, as well as suggestions
for sampling fugitive  emissions.   These are  presently the tentative recommend-
ed procedures.
Solid Streams—
    Recommended  techniques for  sampling solid streams include:
    •   Grab-full stream  cut
    •   ASTM  pulverized coal samples
    •   Automatic-full stream cut-Vezin type  samples
    •   Stopped belt sampling method.

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  In using  these  techniques, one should also take into consideration,
       1.   Heterogeneous nature of the material and degree of
           stratification  likely to be encountered
       2.   Tendency of different size fractions to concentrate
           certain materials in sample, e.g., some trace elements
           may  tend to concentrate in the smaller size fractions.
  With  the  above  two points in mind, it would appear that the full stream cut
  or the stopped  belt methods would provide the best representative samples
  from  solids.
       The  following considerations should also be observed in sampling solid
  streams to minimize contamination of the sample.
       1.   Sampling equipment surfaces in contact with sample
           should be made of stainless steel to minimize erosion
           effects.
       2.   Sample container material should have weak erosive
           potential and be acid resistant and free of toxological
           contaminant.  Kapton is generally acceptable.
      3.  Air-tight stainless steel containers should be used for
          high temperature samples.
 Liquid Streams—
      The recommended  procedures  for sampling liquid streams include:
      •  Grab-full stream cut
      •  Tap
      •  Automatic  high volume samples
      •  Carbon absorber concentration  techniques.
 Sampling  liquid  streams is  relatively  straightforward if there are no sus-
 pended particles or non-miscible  liquids in the stream.   Since this is not
 generally  the  case, representative  sampling of liquids  becomes more difficult.
 Point  sampling and high non-isokinetic  flow rate sampling are the prevalent
 methods in water sampling.  These techniques can be considered accurate for
 most needs but may not  suffice for  trace sampling.   Further work is needed to
 verify the sampling techniques in this  area.
     In sampling liquids  for  trace metals,  the liquid is  filtered on  site and
 the filtrate stabilized with  nitric  acid.   For trace  organics, no filtering is
 involved;  the sample is preserved by refrigeration  at 4° C.  In sampling
 liquid systems,  Teflon, stainless steel  and glass are the only materials
usually used.

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Suspended Particulate—
     The Source Assessment  Sampling  System  (SASS) train is the recommended
technique (5) for suspended particulate sampling of fluidized-bed units.  This
unit and the Method 5 train fulfill  the following criteria necessary for
efficient particulate sampling:
     1.  Provide sufficient quantity of sample for analyses
         at each particle-size fraction desired.
     2.  Minimize number of sampling trains and avoid excessive
         personnel interference.
     3.  Meet precision and accuracy goals defined for each
         sampling level (Level 1 and Level 2 discussed later).
     The SASS train meets all the above criteria for Level 1 particulate samp-
ling and criteria 1 and 2 for Level  2 sampling.  The Method 5 rig with an
impactor and a high volume cyclone train meets criteria 3 for Level 2 partic-
ulate sampling, and in some cases may meet criteria 1.
     The following considerations are important in particulate sampling for
minimizing contamination of either the trace organic, trace inorganic measure-
ments, or bioassay procedures.
     •  Stainless steel 316 should be maintained as the principal
        material of construction with Viton-A used as gasket  materials.
     •  Filters should be high-purity quartz material and should  be
        routinely analyzed to insure low inorganic concentration.
     •  Trains must be packed and unpacked in a clean room environment
        to minimize contamination.
Gases—
     The recommended techniques for  sampling of gaseous components include:
     •  EPA Methods 3 through 7 (6), and 10 (7)
     •  ASTM methods
     •  Absorbing solution methods
     •  Condensation methods and others.
All of the chosen techniques have had proven field experience,  except for the
porous polymer adsorber technique for nonvolatile hydrocarbons.   Options to
some of the selected methods are available and are presented  in the Mitre
report.
     Other considerations in sampling gases are
     1.  Organic grab samples taken  in glass bombs should
         not be left in sunlight and should be analyzed as
         soon as possible.
                                      7

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      2.  Precautions must be taken to  insure no  stratification
         of  sample  occurs.
      3.  Materials  of  construction must be inert towards
         the sample material.
 Fugitive Emissions—
      Fugitive emission measurements are made on  the basis of  a  background
 versus  operating  plant method.  Background ambient air quality  measurements
 are documented prior to  the plant's construction or during a  plant  shutdown
 for those  plants  already constructed.  In the latter case, the  aggregated
 storage piles would have to be  covered during the background  measurements.
 The background measurements are compared to measurements made during  plant
 operation  and fugitive emission levels determined from the two  measured  levels.
 A meteorologist should determine the duration of background and operation
 fugitive testing.
 Sampling and Analysis  Strategy
      A  multilevel approach is used in  sampling and analyzing  samples  from the
 various selected  streams of a combustion process.  The levels are referred to
 as Level 1,  2,  and  3.  Each of  the levels is defined below, as  taken  verbatim
 from reference (3).  A more detailed report covering Level 1  sampling and
 analyses has been issued recently by EPA (5) .  Level 2 procedures are currently
 being worked out.   Level 3 will require further considerations.
 Level 1 Sampling—
      'Level 1 sampling  stresses  the concept of completeness by presuming  that
 all streams  leaving the  process will be sampled unless empirical data equiva-
 lent  to Level  1 outputs  already exist.  Further, Level 1 sampling is  not  pre-
 dicated on a priori judgements as to the composition of streams.  The
 techniques prescribed presume that whatever prior knowledge is  available  is at
 best  incomplete.  Predictive and extrapolation techniques employed during
 environmental assessments serve as a check on the empirical data and  not  as a
 replacement  for it.
     Level 1 sampling programs are therefore envisioned to permit detection of
 the presence of all  substances in the stream.  They do not necessarily produce
 information as to specific  substances or their chemical form.   For example, if
sulfur-containing gases are in the gas stream, Level 1 sampling will  trap and
retain the  sulfur.   However,  it is not designed to preserve the sulfur com-
                                      8

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pounds as H2S, S02, COS, C^H^S,  (CI^^S, etc.  (In many cases a reasonably
specific compound Identification may result at Level 1, but conceptually it is
not necessary in judging the success of Level 1.)
     Level 1 sampling programs are designed to make maximum use of existing
samples and stream access sites.  While some care must be exercised to ensure
that the samples are not biased, the commonly applied concepts of multiple-
point, isokinetic or flow proportional sampling are not rigidly adhered to.
Normally, a single sample of each stream should be collected under average
process operating conditions, or alternatively, under each condition of in-
terest.  These samples should be time-integrated over one or more process
cycles.  When a series of discrete samples results, they are combined to pro-
duce a single "average" for analysis.
Level 2 Sampling—
     Level 2 sampling programs are directed towards a more detailed charac-
terization of stream composition.  They are not as "complete" as Level 1 in
that resources are expended to improve information on streams of a critical
nature.  Additional sampling of  other streams may be deferred because Level 1
information has indicated a potentially less-significant level of environ-
mental impact.  Level 2 sampling is optimized for specific compounds or classes
of compounds contained in the streams sampled.  It also provides a more
quantitative description of the  concentrations and mass flow rates of the
various substances in the stream.
     Level 2 sampling is considerably more refined than Level 1, since it is
being conducted on streams that have already been identified as having poten-
tially adverse environmental effects.  In some instances, Level 2 will use
the same sampling techniques and equipment as Level 1.  The primary difference
will be a more rigorous attention to selection and preparation of sampling
sites and adherence to procedures for acquiring a representative sample.
Level 2 sampling should also provide for replication of samples in order to
further improve on accuracy and representativeness.
     In many cases, Level 2 sampling will utilize modifications of Level 1
techniques and/or the application of entirely new methods.  Such cases result
from the necessity to identify more definitively the materials which produce
the adverse environmental problems.  For example, if Level 1 has indicated a

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high concentration of sulfur-containing species, Level 2 sampling must be
specifically designed to provide isolation of the materials into appropriate
forms for subsequent analysis.
Level 3 Sampling—
     At Level 3, emphasis is placed on the variability of stream composition
with time and process or control system parameters to define accurately the
range of values to be expected.  An effective Level 3 sampling program is de-
signed to monitor a limited number of selected compounds or compound classes.
     Level 3 sampling is designed to provide information over a long period
of  time.  To be cost effective, such programs must be tailored to the specific
requirements of each stream being monitored.  Based on the information
developed at Level 2, specialized sampling procedures can be designed to track
key "indicator" materials at  frequent intervals.  Level 3 should also incor-
porate continuous monitors if at all possible.
      During  Level  3  programs,  it is anticipated  that more complete  Level  2
 type sampling  will be conducted at predetermined  intervals to check the  limited
 Level 3  information.  Further, recommended  procedures for compliance testing
 should  be introduced  into the program at  a  time  appropriate to  the  status of
 process  or control technology development."
      Table 2 characterizes the Level 1-Level  2  strategy for combustion samp-
 ling.  Although the  extent of the Level 2 and Level 3 sampling will depend  on
 results  from Level 1 and Level 2 sampling,  respectively, it is  likely that
 hybrids  of these levels will  be used in most  combustion sampling programs.  As
                                                                      i
 seen later in  this report the present sampling  program used a combined Level 1-
 Level  2  approach.  The extent to which this occurs depends largely  on the in-
 formation desired and the relative cost incurred  in obtaining the extra  data.
 Sample Preservation and Handling*
     Avoidance  of contamination and degradation of samples is of prime  impor-
tance in the comprehensive analysis of FBC  units.  Contamination considera-
tions extend from the preparative and packing stages,  through the various
collection procedures, and to the analysis  of the collected samples.
 *  Discussion  taken  from  reference  4,  page 33.
                                      10

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     TABLE  2.    GENERAL  CHARACTERISTICS  OF  PHASED LEVEL  1-LEVEL  2 STRATEGY  (2)
              Issue
                                                      Level  1
                                                                                                Level 2
GENERAL

  •  Goal



  •  Process operating conditions
  •  Streams considered

  •  Pollutant classes/species
     addressed
Detection of potential pollutants and
planning basis for Level 2

Steady-state representative condition
All system Influents and effluents
All pollutant claaaes
Accurate measurement of specific
pollutants and determination of
mass emission rates
Steady-state representative condition
Selected system Influents and.effluents
Selected class/species
SAMPLING CHARACTERISTICS

  •  Representative of sample


  •  Sampling technique
  •  Sampling location
  •  Replications
  •  Sample quantity
Sufficient for detection of all
potential pollutants

Particulates: initially isokinetlc,
single point
Gases: single point grab unless stra-
tification exists (then full traverse)
Solids and liquids: partial stream cut

Level 2 sampling locations (aa incor-
porated into generic plant design) used
for Level 1 sampling where practical
Particulates: cross-section point of
average velocity
Gases: same location as for partlcu-
lates
Solids and liquids: most convenient
location consistent with obtaining
partial stream cut

Particulates: 3 minimum; composite
two samples and analyze
Gases, solids, liquids: none
Gases and particulates: dictated by
analytical method employed
Solids and liquids: per ASTM method
Consistent with Level 2 goals

Particulates: isoklnetic,  full  traverse
Gages: single point unless stratifica-
tion exists (then full traverse);
combination of integrated  grab,  vet
Federal Register methods,  and
continuous on-line samplers
Solids and liquids: full stream  cut
(minimum requirement)

Recommend Level 2 sampling capability
be incorporated in generic plant
design
Farticulates: full traverse of cross-
section; distances from disturbances
sufficient to minimize Irregular flow
patterns
Gases: same location as for particu-
lates
Solids and liquids: most convenient
location consistent with obtaining
full stream cut

Particulates: 3 minimum; separate
analysis for each sampling
Gases: complies with Federal Register
specs; statistically designed to
relate manual with continuous on-line
Gases and particulates: dictated by
analytical method employed
Solids and liquids: per ASTM method
and Federal Register specs
ANALYTICAL CHARACTERISTICS

  •  Sensitivity

  •  Accuracy

  •  Replication

  •  Specificity



  •  Gas analysis

  •  Elemental analysis

  •  Anlon analysis

  •  Organic solids and liquids
Highest sensitivity (consistent with
Level 1 resources)

Order of magnitude
None planned

Broad classes of organlcs
Some species (inorganic and organic)

Gas chromatography; absorption tubes

Spark source mass spectrometry

Not performed

Extraction, separation into functional
classes
Analysis by fourler transform infra-red
spectroscopy
Sensitivity requirements  dictated
by Level 1 output

High accuracy
Statistically designed

Individual species corresponding
to class/species Identified  at
Level 1
Primary reliance on GC (or best
method for Individual  species

Atomic absorption spectroscopy  (or
best method for individual species)

Method dependent on individual  species

Extraction, separation by high
resolution
Liquid chromatography
Analysis by GC mass spectroscopy, IR,
NMR (or best method for individual
species)
BIOASSAY CHARACTERISTICS

  •  Analyses performed
Cytotoxicity, mutagenlclty
Cytotoxicity, mutagenlclty,  carcino-
genlcity
                                                          11

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Containers used for packaging reagents for field use and storage of samples
should be dedicated to this purpose and scrupulously cleaned before put in
storage for subsequent use.
     The collection and packaging of samples to be used for carcinogenicity
and mutagenicity should be handled in such a way as to minimize the amount of
degradation brought about by air, temperature, and light.  Ideally, the
collected samples should be placed in brown bottles, purged with nitrogen or
argon, sealed, and frozen in dry ice.  Brown bottles are often difficult to
obtain and cylinders of inert gas are frequently not available for field use.
When these adverse conditions prevail, the sample collection protocol would
be altered to use clear wide mouth jars or bottles.  Immediately following
the collection of the sample, the container is sealed with tape around the
lip of the lid and wrapped in aluminum foil.  Once sealed, the containers
should be carefully packed in dry ice of sufficient quantity to ensure arrival
of the frozen samples at their destination.  Refrigeration at temperatures
near freezing or below is the best preservation technique available, but is
not applicable to all types of samples.  Samples in water solutions cannot
be frozen in glass bottles due to possible breakage.  At best, preservation
techniques can only retard the chemical and biological changes that inevi-
tably continue after the sample is removed from the parent source.  Contami-
nation and degradation of samples can best be avoided by analyzing the
samples as soon as possible after collection.
Quality Control in the Sampling Program*
     Quality control must be supplied in the sampling program to assure that
representative samples are obtained from the various process streams and
that the sample integrity is not compromised prior to delivery to the ana-
lytical laboratory.  Obtaining representative samples requires that appro-
priate sampling locations and sampling technique be selected.  These factors
will be especially critical when sampling the stack and flue gas streams for
particulates.  Maintenance and calibration of equipment is also essential to
collection of representative samples.  Calibration of flow meters and tempera-
ture measuring devices should be performed before each field trip.  Pitot
*  Discussion taken from reference A, page 35.

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tubes should be calibrated and leak tests made on the sampling trains on a
regular basis.  Checks should be performed in the field to verify the equip-
ment is still within calibration.  Spares should be available to replace
defective equipment.
     Maintaining sample integrity demands that careful consideration be given
to materials used in the sampling systems or equipment.  Materials should be
chosen to minimize the introduction of contaminants.  Sample recovery from
particulate sampling trains must be performed in an area and using equipment
and techniques which will not contaminate the samples.  All samples must be
stored in containers which are leak-tight and which do not introduce contami-
nation.  Certain samples (for organic analyses and bioassays) must be pro-
tected from light and temperature extremes to maintain the integrity.
     Continuous gas monitoring instrumentation presents special calibration
requirements.  During a field program, these instruments should be calibrated
before and after each test using standard gas mixtures.  Periodic analyses
should be performed to verify the concentrations of these calibration (span)
gases stated by the gas suppliers.
                                     13

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                                   SECTION 3
                            METHODOLOGY DEVELOPMENT

      In consideration of the preceding discussions,  the methodology develop-
 ment in the present program was  based  around  sampling  and  analysis experi-
 ments with Battalia's 6-in.  fluidized-bed unit.   The Battelle unit provided
 a means for evaluating the generality  of  proposed procedures  in the laboratory.
 DEVELOPMENT OF A COMPREHENSIVE SAMPLING AND ANALYSIS PLAN
      A considerable amount of planning and preparation was required prior to
 carrying out the sampling and analysis plan for  the  6-inch FBC unit.   The
 preliminaries include,  appropriate  background  information  on  the unit, develop-
 ment of a sampling  and  analysis  plan for  the unit, site survey and planning,
 installing and  operating equipment, and shake  down runs.
 Background Information
      Prior to the actual sampling of a FBC unit,  it  is essential that  the
 appropriate personnel become  throughly familiar with the design and general
 operation  of the unit.   Pertinent areas of interest  include but are not
 limited  to
      •   Process description
      •   Process schematic flow sheets
      •   Plant layout
      •   Equipment specification
      •  Plant personnel data
      •  General range of firing conditions capable with  the FBC
     •  Results of any previous emission  testing.
     Background information relating to the design and general operating  fea-
tures of the Battelle unit is discussed below.
                                     14

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Battelle 6-in. FBC—
     The 6-in. FBC facility at Battelle can be fired in different velocity
modes with solid fuels at rates up to 50 Ib/hr.  Preheaters enable the
incoming gases to be heated to nearly 1000 F, as desired, prior to
combustion.  Fluidized-bed operating temperatures from 1400 to 1800 F
are established through control of the fuel feed-rate and preheat
temperatures.
     Figure  2 shows a scaled drawing of the 6-in. FBC unit used in this
program.  Figure 3 is a photograph of the unit.  For this work, it was
desirable to  fire the combustor in a low velocity mode typical of that
used in conventional FBC units.  High sulfur Illinois Number 6 coal was
used for the  fuel and grove limestone served as the bed material.   These
are fed to the combustion chamber on a small conveyer belt.  Cyclones are
used in the  flue gas and sampling streams to fractionate particle sizes.
Normally, two cyclones are present in the flue gas stream from the FBC
unit, but for this sampling program, only one cyclone was used in this
stack gas region.  This cyclone (No. 1) removes all particulates above
about 27 microns.  A second smaller cyclone was installed in the Method
5 rigs to remove particulates between about 27 and 2.3 microns in the
sampled gas.  This is discussed later.
     Sampling ports are available at several different points in the
combustor.   These are indicated in Figure 2 by the capital letters A, B,
C, D, and E.  The legend in the figure describes the general type
sampling taking place at each port.  An overflow tube (T) inside the
bed reaction  chamber maintains the height of the bed at 4-ft and allows
continuous removal of the bed materials during a run.  The overflow
tube acts essentially as a sampling port within the fluidized-bed region.
     The flue gas, after passing the final sampling Port C, is directed
into a water scrubber where the gases are further cleaned before exiting
to the atmosphere.  Solid material (sludge collected in the scrubber)
is removed from the scrubber by filtering.
     The above background information provided a basis for choosing
sampling locations, proper sampling conditions, and selection of appropri-
ate sampling streams with subsequent development of a sampling and analysis
plan.
                                    15

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                58-
                    LEGEND
             Continuous Monitoring
             Sorption Monitoring
             Particulate Monitoring
             Gas  (NO ) Monitoring
                   X
                                                             --T/Z.
                                                             ~-Tio
FIGURE 2.  SCALE DRAWING OF 6-IN. FLUIDIZED-BED COMBUSTOR
                           16

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FIGURE 3.  6-IN. FLUIDIZED-BED COMBUSTOR
                       17

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Sampling and Analysis Plan
     The initial efforts in this program were directed to the development of
a comprehensive sampling and analysis (S&A) plan applicable to fluidized-bed
combustors and other coal burning units.  The plan was developed around the
design and operating features of the Battelle FBC unit.  Since the Battelle
unit is essentially a bench scale FBC model, many of the streams shown in
Table 1 were not applicable to this unit.  Notably absent from the Battelle
unit were those streams relating to regenerative processes and fugitive emis-
sions.  Other streams were omitted on the basis of low priority.  The streams
chosen for sampling in this program were:
     •  Stack gas
     •  Particulate removal discard
     •  Bed solids discard
     •  Prepared fuel feed to combustor
     •  Prepared sorbent feed to combustor
     •  Scrubber discard.
     The S&A plan derived from the Battelle unit was refined and later final-
ized into the form shown in Table 3.   The tabulation shows the streams sampled,
the constituents measured in the streams, the analysis methods used, and the
procedure used to obtain the sample.   This plan was later generalized to in-
clude all streams likely to be encountered in FBC S&A programs.  The general-
ized plan is given in the final sections of this report (Table 9).
Site Survey
     A site survey is conducted prior to carrying out the S&A plan developed
for the FBC unit.   A site survey is an important part of the sampling program
in that it provides proper coordination of the plant's physical layout with
the test plan strategy.   The more important points considered at the site
survey inspection for this program were:
     a.   Are the sampling sites accessible and is there proper space
         allocation and  supports (tables, platforms, etc.) for all
         the equipment and supplies?
     b.   Are there  a sufficient number of sampling ports and do
         the sampling sites  meet all  the criteria for representative
         sampling?
     c.   Do  the  sampling  sites  have access to utility outlets of the
        number  and  type  required by  the sampling equipment?

                                     18

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                                             TABLE 3.   FBC  SAMPLING —  ANALYSIS PLAN

                                         Level  1 — Scanning for  Classes  of Compounds
                                          Train and/or Sampling Method
                                                                                       Analysis Method
                                                                                                                                   1976
                                                                                                                                 Eat. Cost
COAL

  Pollutant

  Proximate/Ultimate

    Moisture
    Ash
    Volatile matter
    Fixed carbon (by difference)
    C, H, N, S,  0 (by difference)

  Sulfur - Total

    Pyritic
    Organic
    S0,=
                                                                                                                                 (525)
                                      Obtain three or four grab  samples,
                                      -100 grams each, at intervals during
                                      run and combine for representative
                                      bulk sample
                                                                                  ASTM D291
                                                                                  ASTM D2492-68
  Trace metal
  Na, Ca
  Particle size
  Heating value

LIMESTONE

  Particle size
  Ca, Mg, CO',  NO',  N0~

  Trace metals

OVERFLOW BED MATERIAL

  Particle size
  (Chemical identification)
  Trace metals
  SO", SO",  S=
              NO",  NO,
  Organic classes
ASH
  -325 mesh material from overflow
    bed material (weigh)
  Trace metals
SO',  SO",  S-
                NO-,
                                        Obtain three or four  grab samples,
                                        -100 grams each,  at intervals during
                                        run and combine for representative
                                        bulk sample
                                        Collect all of overflow material;
                                        sieve for -325 mesh material; weigh
                                        -325 mesh sample and  use for ash
  Organic classes
                                                                                    SSMS
                                                                                    AA
                                                                                    Sieve
                                                                                    Calorimeter/ASTM D2015-66
                                                                                  Sieve
                                                                                  AA - Spectrophotometric, phenol desulfonic
                                                                                      acid
                                                                                  SSMS
Sieve

SSMS
Wet chemical methods

Extraction/liquid  chromatography/IR
Sieve

SSMS
Wet chemical methods

Extraction/liquid  chromatography/IR
                                                                                                                                   (345)
                                                                                                                                   (780)
                                                                                                                                 (780)

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                                                  Train and/or Sampling Method
                                                                                         Analysis Method
                                                                                                                                            1976
                                                                                                                                          Est. Cost
t-o
O
       SLUDGE
         C, H, N, S, 0
         so'
         so'3

         Trace metals
         Organic classes

       FLUE GAS STREAM

         1.  Participate >27 v
             a. Trace metals
                1) 60 (approx)
             b. Minor elements (cations)
                1) Fe,  Al, SI, K
     c.  Anlons
        1)  Chloride, fluoride
        2)  CO-
        3)  NO",  NO-

        4)  SO',  SO'

     d.  Organics
        1-8)  Organic classes
        9)  POM
        10) Organic-reduced sulfur
            compounds (8 classes
            combined)
     e.  C,  H, N, S, 0
     f.  Size analysis
 2.  Partlculate (<27 u, >2.3 y)
     a.  Trace metals
     b.  Minor elements (cations)
     c.  Anions
     d.  Organics
     e.  C,  H, N, S, 0
     f.  Size analysis
2a.  Partlculate <2.3 u
     a.  (Same analyses as under
         Section 2)
                                                                                                                                             (790)
                                        1 gallon sample from scrubber at  end
                                        of run; sample filtered and dried for
                                        4 hrs at -160 F, remaining solid  used
                                        for sludge sample;  solution stored in
                                        capped bottle
                                        Cyclone No.  1 emptied two or three
                                        times during run and at end of run;
                                        sample combined and stored in dark;
                                        ahort-term exposure for high-level
                                        material; long-term exposure for low-
                                        level materials
                                                Two M-5 trains, Isokinetlc sampling,
                                                approximately 2 hrs; sample taken
                                                from cyclones in M-5 rigs and stored
                                                in dark
                                                Sample from filters in M-5 rigs, or
                                                cascade impactor; sample stored in
                                                dark
Barium perchlorate tltratlon
H.O./Barium perchlorate titratlon

SSMS
Extraction/liquid chromatography/IR
SSMS

SSMS
SSMS
AA

Spectrophotometric, phenol disulfonic acid

Barium perchlorate titratlon (H_02 with SO


Extraction/liquid chromatogtaphy/IR
Fluorescence - fraction No. 2 above
GC/FPD
 Sieve

 (As described  in No.  1  above)
                                                                                                                                   (1160+)
                                                                                                                                            (11604-)
 (As  described in  No.  1  above)
(1160+)
                                                                 TABLE 3.    (Continued)

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                                           Train and/or Sampling Method
                                                  Analysis Method
                                                                                                                                      1976
                                                                                                                                    Est. Cost
  3.   Gases
      a. Acid gases*
         1) C02
         2) S02
         3) NO - NO,
         4) SO     ^
      b. Inorganic*
         1) CO
         2) 02
      c. Organic
         1) Total gaseous hydrocarbon
         2) Organic classes:
            alkanes, alkylbenzenes,
            POM, thiophenes, carba-
            zoles and esters,
            aldehydes, PCB, ketonea,
            and alcohols
         3) Organics - reduced sulfur
            (8 classes combined)
      d. Hg, Cd, As, Pb, Se
      e. HC1, HF, HCN, NH *
                                                                                             (755)
Continuous
Continuous
Continuous
Continuous
Continuous

Continuous or bag
Sample stored in dark
Bag or Tenax

10% KMnO, or K.Cr.Oy acid solutions;
use HO. prior to solutions to remove
SO ; solutions stored in dark
Gas absorption train (Figure 5 in
text); 0.01 N, NaOH used to collect
HC1 and HF, 5% KOH solution for HCN
and IN H,SO, to collect NH
NDIR
NDIR
NDIR - Chemiluminescence
Goks«Syr-Ross

NDIR
EC - Polarograph

FID
Tenax extraction/liquid chromatography/IR
CG/FPD

AA
Ion chromatograph (HC1, HF) and specific
ion electrode (HCN, NH,)
*  Level 2 scanning for specific compounds.

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     d.  Do  the  sites meet critical OSHA requirements?
     e.  What arrangements must be made for  transporting  equipment
         from the  ground  to the sampling site?
     f.  Does the  plant have adequate laboratory  space  available;
         if  not, can the  cleanup van be parked  in close proximity
         to  the  sampling  area?
     g.  Does the  plant have personnel available  to assist  in the
         acquisition of solid and liquid samples?
     h.  What is the plants normal operating schedule and down-time
         of  equipment?
     i.  What type and condition is the on-line measurement
         ins trumentation?
     j.  Are support services available to the  field team such
         as  storeroom, welders, glass blowers,  etc.?
 Occasions  may arise where other points may need consideration but  these major
 areas  should suffice for  most FBC sampling programs.
 Installation and Operation of Equipment
     A wide  variety of instruments and sampling units are required in sampling
 a FBC  or other type combustion unit.  Gas, liquid, and  solid  samples  are
 generally  involved.  Some instrumentation is likely to  be available and in
 operation  at the plant site.  If so, consideration should be  made  as  to their
 suitability  for  use in the comprehensive analysis program.
 Continuous Gas Monitoring—
     Continuous  gas monitoring instruments were available and in operation  at
 the  Battelle FBC unit and were used in this program for measuring  CO,  C02,
 S02> NOX,  02 and total hydrocarbons from the combustor.   The  instruments used
 for  measuring each  gas are given in the S&A plan  shown  in Table 3.  Figure  4
 is a schematic of the gas analysis system.  The sample  tubing to these in-
 struments  was made  of stainless steel and/or Teflon and of  proper  diameter
 to allow sufficient gas flow to the instruments.  Stainless steel  tubing was
 installed  at all sampling ports in preference to  Teflon because of the some-
 what high  temperature for Teflon.
     Calibration procedures were worked up for each instrument prior  to the
 sampling runs.   Flow rates to the instruments for either  sample gases  or
 span gases  were  adjusted  to the needs of the instrument as  specified  by the
manufacturer.  Stainless  steel bellows pumps were used  to provide  sample gases
                                      22

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N>
OJ

Particulant

Water traps trap _ 	 ; 	 n





««^i



N2 — 
CO — $>
span





Icebath pirex wool f "\
^ I
vJ^ ATH

s
S.S. Bellows
pump

\ \
T • Y
V
V^vr
•••tr

H
=
IL
'

1



f Water, trap
dry icebath
5 1 1 jj- |
6b nn Y °

N2-<2>- N2-^~
Co2——
span span
L J-, -« 	 -Sllicn gel
=^ ^i coiuim
O O
T ¥ Y
• i 1
S02 Anal. NO Anal. 02 Anal. 13
t t 1
                                                                                                                          flow nctcrs
                                               FIGURE 4.  FLUE GAS ANALYZER FLOW SCHEMATIC

-------
to the instruments.  Room temperature fluctuations were not a problem in our
sampling, but temperature conditions must be considered if cold weather or
wide fluctuations in temperatures are involved.  Traps were used  to  remove
particulates and moisture from the sample gas prior to entering the  instru-
ments.  Pyrex wool served as a filter to remove the particulates  and a wet-
or dry-ice bath was used to effectively reduce the moisture content  of the
sample gas stream to an acceptable level for operating the instruments.   (A
word of caution here.  While the removal of particulate and water vapor from
the sample line is imperative to proper operation of most of the  instruments,
the total effect of the removal processes on the sampled constituents mainly,
N02 and SC>2, is questionable.  As noted later, more consideration should be
given to the effects of the removal processes.)
Method  5 Sampler for Particulate and POM Samples—
     Method 5 samplers, were installed to obtain particulate samples in this
program.  Modifications were made to the Method 5 sampler as follows,  (1)  in-
stallation of a small glass cyclone inside the heated chamber prior  to the
filter  to further fractionate the particulates, and (2) installation of  a
tenax column downstream of the filter outside the heated chamber  to  collect
POM samples.
      A "Y" probe was constructed so that two Method 5 rigs could be used  to
sample particulates simultaneously from a single sampling point within the
flue gas stream.  Sample ports were installed so that samples could  be taken
at about midstream of the duct at least 10 tube diameters downstream from any
elbows.  Gas velocities were measured during the shake down run for  isokinetic
sampling.  Operation of the Method 5 rig was in accordance with the  Federal
Register procedures (6), except no traverse of the duct was made.
Bubbler Samples—
     In addition to the continuous monitors and the Method 5 rigs, sorption
trains were constructed and used in this program for collecting acidic (HC1,
HF, and HCN)  and basic  (NH3>  gaseous components present within the gas stream.
Although not  specifically required in a Level 1 analysis scheme, these sorp-
tion trains were installed to collect and analyze each of the gases  for  a  more
complete characterization of  the emissions from the FBC unit.   An oxidizing
solution was  also  installed to collect certain trace metals that may be

                                      24

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present in vapor form in the stream.  The metals of interest were Pb, Hg, Se,
Te, Be, As, and Cd.  Figure 5 shows a single typical absorption train used in
the program.
     Although SO-j can also be collected in solutions such as alcohol-water
mixtures, it was decided that the Gtfksoyr-Ross method would be the better one
to use for 803 since much of the alcohol-water solution would evaporate over
a two-hour period.  Therefore, the Goksoyr-Ross apparatus was installed in
place of a sorption train to collect 803.  The manifold and sample line to
the Goksoyr-Ross unit beyond the manifold were heated with heating tape, to
prevent H2SC>4 condensation.  It is important that these areas be heated to at
least 325 F to avoid loss of 803 (as H2S04).
Shake Down Runs
     Unless the FBC unit has been run previously at the desired operating con-
ditions, it is generally worthwhile to make at least one preliminary or shake
down run prior to the actual sampling runs.  In so doing, the technicians
operating the fluidized-bed unit are able to check their calculated values
for producing the desired bed temperature and gas flow rates, SC>2 levels, ex-
cess air, etc., and make appropriate adjustments where needed prior to the
actual sampling run.
     Shake down runs were made prior to the sample Runs 1 and 2 in this pro-
gram.  Fluidized-bed operation was checked out and proper adjustments made.
The technicians taking the samples were then able to make preliminary checks
on the sampling conditions of the unit under the desired operating conditions.
Appropriate temperatures of the various sampling ports were checked and gas
velocities measured, where necessary, to allow for isokinetic sampling during
the actual sampling runs.  Instruments were checked out for proper operation
and checks were made for leaks in the sampling units.  At the completion of
each shake down run, the FBC unit was prepared for the sampling run which
followed the next day.
COLLECTION AND PREPARATION OF SAMPLES FOR ANALYSIS
     Details of the procedures involved in obtaining, handling, and preparing
samples for analysis from our fluidized-bed combustor are discussed in refer-
ence to the sampling and analysis plan shown in Table 3.  This plan was
closely followed in each of the sampling runs made.

                                      25

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SAMPLING
ZONE
PROBE





V
.







['//////7//J
V/M///A

HEATED
GLASS
FIBi.R
FILTER





....

















^

»





r""

HEATED
MANIFOLD


*












1
1
I
^

•
.Fir .








1
1
1
. i
\ / EMPTY SILICA
• 1MPINGERS rr, , rr,
V*LZ L> L* lj LZ Iw
TO VENT  —*-
i-QJ:
                                              PUMP
                          DRY
                          GAS
                         METER

                FIGURE 5.   TYPICAL GAS ABSORPTION TRAIN
                                                               X
                                                            CHECK
                                                            VALVE
                                26

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Sampling
     Samples were taken from the various selected streams after stabilizing
the FBC unit at the desired firing conditions.  Sampling was started after
the SC>2 level in the gas stream was reduced to the desired level, approxi-
mately 700 ppm, via reaction with the limestone.  Six major streams were
sampled as indicated earlier.  The sampled streams are discussed in the order
given in Table 3.  Figure 6 is a schematic outline of the sampling locations
in the FBC unit.  Each sample stream discussed below is numbered in accordance
with the numbered locations in Figure 6.
(l)-Coal Feed Stream—
     Three or four grab samples of coal, about 100 grams each, were taken at
about equal time intervals over the 2-hour sampling period.  The crushed coal
was fed to the FBC unit on a small conveyor belt.  Since the unit burned only
about 15 Ib/hr or less of coal, the coal stream to the unit was small and
cross-section samples of the stream were used as representative of the coal
mass.  In larger units where much more coal is used, the procedure for col-
lecting a representative coal sample is more involved.  The proper procedures
have been noted in an earlier section of this report.
     The 3 or 4 grab samples of coal were combined, as the run progressed, in
a single plastic container and, at the end of the run, the total sample was
sealed in the plastic container and stored.
(2)-Limestone Feed Stream—
     The limestone was also fed to the FBC unit on a small conveyor belt and
samples of limestone were taken in the same manner as for coal.  The total
sample was sealed in a plastic container and stored.  As with the coal, the
large combustors would require more detailed sampling procedures.
(3)-Overflow Bed Material—
     This material consisted mostly of limestone and was continuously sampled
through the overflow pipe in the reactor bed during the entire 2-hour sampling
period.  A representative sample was taken from the overflow container at the
end of the run.  This was done by scooping samples from various part of the
mass bed material and combining them in a plastic container.  The container
was sealed and stored in the dark.  (All samples to be analyzed for POM and
other organics were stored in the dark to minimize decomposition.)
                                      27

-------
           Cyclone
            #1
   n
  Bed  /
     •—s
     3
       z_
Air
          Particulate

           >2?K.  (
  Coal



Limestone ©
      Ash
                                       Flue Gas Analyzer
                                      n - 1 — i - 1 - 1     i
                                      CO  C02   02  S02   NOX  THC
                                              Gas Absortion
                                                 Trains    I
                                           rtffi"
                                   Scrubber
                                              Sludge
                                                      xTenax Plug
                                                       (Pom, He)
Mod. Method 5 Trains
    I     I  |
    Particulate
                                     Particulate
                                              I
           FIGURE 6.  SCHEMATIC OUTLINE OF FLUTDI7.ED-BED COMBUSTOR

                    AND  SAl-IPLTNG LOCATIONS
                                    28

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(4)-Ash—
     The ash sample referred to here was taken from the overflow bed material.
It is the small -325 mesh particles remaining in the overflow bed material at
the completion of the run.  All of the overflow bed material was sieved at the
end of the run into several size fractions.  The smallest fraction (-325 mesh)
was used as a representative ash sample from the bed material.  Generally less
than 0.1 percent of the total overflow bed material remained in this smallest
fraction.  However, sufficient sample was obtained in most runs for the proper
analysis.  The ash sample was sealed in a plastic container and stored in the
dark.
(5)-Sludge—
     The sludge sample is the solid material caught in the water scrubber
attached to the end of the flue gas stack.  In obtaining a sludge sample, the
water used for scrubbing the flue gas was continuously removed from the
scrubber barrel and passed into a large centrifuge.  The centrifuge was lined
with a fine filter which retained the solid material while passing the liquid.
The centrifuge was run during the entire sampling period.  Several liquid
filtrate samples  (about 1 gallon each) were taken from the centrifuge drain
at recorded time interval during the run and stored in large plastic bottles.
The solid material remaining on the filter was removed by scraping; the solid
sample was dried and sealed in a plastic container and stored with the other
samples in the dark.
(6) through  (9)-Flue Gas Stream—
     A large number of samples was taken from the flue gas stream.  Samples
were obtained from the in-stream cyclone and from two Method 5 rigs, several
sorption trains and a number of continuous monitors.  Particulate and gaseous
samples were involved.  Sampling procedures are described below.
(6), (7), and (S)-Particulate—Particulate samples were obtained from two
sources (1) the solid material removed by the cyclone in the flue gas stream,
and (2) from samples taken by the Method 5 rigs.  The cyclone and Method 5 rigs
provided three size fractions of particles.  These were (approximately as cal-
culated from cyclone dimensions),
     1.  Particles greater than 27 y diameter
                                      29

-------
     2.  Particles less than 27 y greater than 2.3 y diameter
     3.  Particles less than 2.3 y diameter  (0.1 y limit).
The larger cyclone, which was a part of the  flue gas stream, removed  the
larger particles  (>27 y ).  A smaller cyclone installed  in  each Method  5 rig
'removed the intermediate size particles (<27 y , >2.3 y). The  filter  in the
Method 5 rig removed the remaining particles down to about  0.1 y.
     Samples from the larger in-line cyclone (>27 y) were withdrawn from a
particulate collection chamber at the bottom of the cyclone at the  end  of the
2-hour run.  The  samples were sealed in a plastic bottle and stored in  the
dark.
     Particulate  samples <27 y, >2.3 y were  obtained from the  cyclone in the
Method 5 rig under the following conditions.
     1.  Method 5 (isokinetic) sampling procedure was used.
     2.  Sample was collected at midstream of 4-in. diameter
         stainless steel duct at a position  about 1-ft from
         end of duct  (sample point C in Figure 2).
     3.  Heated stainless steel tubing, 1/2-in. I.D. was used
         to withdraw sample from stream into Method 5 rig at
         the rate of about 0.75 cfm (using appropriate size
         nozzle to obtained desired isokinetic flow rate).
     4.  Particulate samples were collected  for period of 2
         hours.
     5.  Samples  were taken from cyclone in  Method 5 rigs
         after run was completed.
     6.  Samples  were stored in sealed glass containers  in  a
         dessicator (in the dark and under N£ gas if stored
         for several days).  Particulate samples were combined
         for analysis if more than one sample taken during  run.
A problem was encountered in the separation  of particle  sizes.  The designated
fractions were not always obtained from the Method 5 rig samples since  the
smaller cyclone tended to clog rendering the separation meaningless.  In those
instances,  the filter and cyclone samples from the Method 5 rig were  combined
to form a less than 27 y fraction.  Particulates were also  washed from  the
sample probe with  acetone followed by wash with methylene chloride.   These
samples were dried and added to the <27 y catch.  Filter samples in the Method
5 rig were removed when filter loading became sufficiently  high.  The filter
and loading were weighed and placed in a glass container, sealed and  dessi-
cated.   The samples were removed from the filter prior to analysis  by flexing

                                      30

-------
the filter material; this released most of the caked-on sample.  The filters
were reweighed and particulate sample weight determined.  All particulate
samples were stored in  glass containers, and placed in dessicators in the
dark.
(9)-Impinger Samples—These  samples were obtained  by  sorption of a particular
constituent in a  solution which  efficiently trapped the desired material.  For
each sorption train, two solutions were used in  series to insure more complete
removal of the desired  constituent.  The second  solution collected only  a
small fraction of the total  sample  (<10 percent).  The impingers were immersed
in wet ice for better sorption of samples.  Each unit (sorption train) was op-
erated independent of each other.  Flow rates and  total gas sampled were re-
corded in each sorption unit.  Pumps were downstream  of the bubblers and all
gases were dried  with drierite prior to entering the  pumps.  Sampling rates
were about 0.2 cfm; the sampling period was usually 2 hours.  Approximately
10 to 20 cubic feet of  gas passed through each bubbler.
      At  the  end  of a 2-hr  sampling  period,  the  solutions were removed from
 each impinger and placed  in a separate glass  bottle.   Volumes were measured
 and  samples  were stored in a cabinet  at  room temperature until  ready for dis-
 tribution and analysis.
      The G8ksoyr-Ross  unit was washed  with  distilled  water  then 3 percent
 peroxide solution and acetone to remove  the SO-  (as H-SO,).  The volume
 of solution was  recorded and the sample  stored with  the  above impinger samples.

 (9a)-POM—POM samples were collected  on a tenax column attached to  the  samp-
 ling line of the Method 5 rig downstream of the filter.   The tenax  column was
 covered at all times to keep out light.   At the end  of the run,  the column
 was removed and filled with nitrogen,  sealed and stored in a refrigerator
 (kept in the dark at all times).
 (lO)-Gases—
      The remaining samples from the flue gas stream involved essentially the
 gaseous  species  in the stream.  The acid gases  C02,  S02,  and N0-N02 and  the
 inorganic gases  CO and 02  were monitored continuously as described  earlier.
 Total hydrocarbon content  was also  monitored continuously.
                                      31

-------
Sampling Problems
     A few problems were encountered in the sampling of the Battelle  FBC unit.
These, however, were generally isolated events and produced no  threat to the
completion of the sampling task.  The specific problems encountered were:
     •  Small cyclones in Method 5 rigs tended to clog  after several
        minutes of sampling rendering particle size separation  incom-
        plete.
     •  Flue gas temperature at sampling port dropped below that
        desired for good 803 sampling (325° F) for Runs 2 and 3.
     •  Filters would load heavily by end of a 2-hour run.  Some
        had to be replaced during the run (Method 5 rig).
Labeling
     Proper labeling of samples is a very important part of the sampling pro-
gram.  Each sample in each stream listed in Table 3 was labeled so as to
identify the stream sampled, material or sample collected, run number and
date of run.  With proper sample labeling, no confusion will result in re-
lating the analytical results to the appropriate sample.  It is equally im-
portant that starting and finishing times for all processes be noted  and
coordinated with the individual collection processes for each sample  category
so  as to provide valid comparison of all pertinent data.
Analyses of Samples
     Analyses charts were drawn up for each run relating the sample taken from
the FBC unit to the analyses to be made on the sample.  An example chart is
shown in Table 4 for Run No. 2 samples.
     As shown in Table 4 each original sample was divided into a number of
smaller fractions so that sufficient material was available for the different
analyses needed on each sample.   The number of fractions of each sample needed
is indicated by the number of "forks" or divisions after each original sample
(shown in boxes) in Table 4.  Each fraction of sample was weighed to  the near-
est 0.1 gram before distribution for analysis.  In the case of solutions, the
volume of each solution was recorded prior to distribution for analysis.
Additional Considerations in the Analyses of Samples
     Three other analysis areas  not shown in the analyses chart of Table 4
but which should be considered in a FBC sampling program are (1) biological
testing,  (2)  radioactivity measurements, and (3) noise measurements.   Areas

                                      32

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TABLE  4.   SAMPLE IDENTIFICATION AND ANALYSES
Fluid-Bed Sample Number
Material Sample No. Designation

Illinois 16 coal
(-8 M) S-2-1

Grove limestone
• S-2-2

Bed material S-2O

Ash (-325 M) S-S-4

Sludge S-2-5

Flue gas stream
Particulate >27u 2
S-2-1-1 /
-/ S-2-1-2
\ S-2-1- 3
\5-2-l-4
S-2-2-1
\ S-2-2-2
\S-2-2-3
S-2-3-1
x^ s-2-3-'t
\ S-2-3-2
\i-2-1--}
S-2-4-1
-V^ S-2-4-2
\ S-2-4-3
V;_2-it-.l>
• S- 2-5-1
\.. S-2-5-?
\S-2-5-3
S-P-6-1
/ S-2-6-2
^\ S-2-6-3
\ S-2-6-4
Proximate /ultimate
/
^ Sulfur
Na, Ca
Heating value
Trace metals
Particle Size
Ca, Mg, CO" NO"
Trace metals
Particle Size
Trace metals
Organic Classes
SO" , S0j, S=, NO",
Particle Size
NO" NO" s", SO"
Fusion temperature
Trace metals
Organic Classes
C, H. N. S. 0, SO"
Trace Metals
Organic Classes
Ai
C~(l) Moistu
") (2) Ash
1(3) C.H.N.
V, 0(by d
Gl) Total
\(2) Pyrite
NOl
NO;
, and S0~3
, and SO*
Trace metals (approx 60 metals)
__ C, H, N, S, 0
Anione , NO", NO
Organic classes
-. so", so;
                                                           (5) Fixed carbon (by
                                                               difference)
                                                          ;rence)
                                                           (3) Organic
                                                           (4) SO.
                           X
             Partical Size
POM
Organic and reduced sulfur compounds
                                33

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TABLE  4.
Fluid-Bed Sample Number
Material . Sample No. Designation
Flue
Parti
(If t
frac
here
>2.3
sraal
desig
S-2-
yses
Flue
Gases
Cases
ooni

gas stream S-E
culaM? <21\l
rfo particulate
bions involved
, e. g. <2?
, and <2.3 ,
ler fraction is
nated Batch No.
i and same anal-
as S-2-7.)
gas stream S-£

continuoua S-2
:orine

S-2-7-1 Tra
7 ./ S-2-7-2
V
\\ S-2-7-3
C.
Ani
\ S-2-7-4 Orgi
Particle Size
(AL-3) S-2-9-1 s^'
/ ^-~^
-9 ~
-------
1 and 2 are included in the general sampling and analysis plan in Table 9 in
a later section of this report.  Although samples were available for analysis
from our sampling program in areas 1 and 2 above, no testing or measurements
were made in our laboratories.  However, samples were sent to EPA for biologi-
cal testing.  On the other hand, noise measurements were made in the area of
the 6-in. FBC unit used in this program.  The results are included in the
appendix.  Further discussion of noise analyses and areas 1 and 2 above are
given in the "Recommended Sampling and Analysis Plan" section.
Analyses Problems
     No serious problems were encountered in the analysis of samples taken in
this program.  The determination of the concentration of a species "by dif-
ference"  (e.g., the oxygen values in some of the samples in Table 4) is likely
to produce more error  than the direct measurements made on other species.
But this would be expected from the procedure involved.
                                      35

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                                 SECTION 4
                        EVALUATION OF EMISSION DATA

     Three runs were made in the course of this sampling program.  These
are designated Run Nos.  1, 2, and 3.   The firing conditions for each of
these runs differed as indicated in the following tabulation.
                                            Run      Run      Run
                                           No. 1    No.  2    No. 3
        Coal feed rate,  Ib/hr              15.9      8.8      9.3
        Limestone feed rate, Ib/hr         15.4      4.3      8.1
        Air feed rate, Ib/hr              145.0     87.3     84.2
        Bed height: expanded, inches        48       48       48
                    settled, inches        12.6     21.6     21.6
        Bed temperature, F                1538      1655     1490
        Superficial gas  velocity, ft/sec    9.1      6.0      5.3
        Ca/S ratio                         6.7:1    2.9:1    7.1:1
                                3
        Particulate loading, g/m            1.44     1.64     NA
     Sampling procedures were the same for Run Nos. 2 and 3, but different
slightly between Run Nos. 1 and 2, as did also some of the analyses
procedures between these latter two runs.  These differences are brought
out in the list shown in Table 5.  The changes were made to bring about
a more cost effective sampling and analysis plan while at the same time
completely defining the  major pollutants emitted from the FBC unit.
     Two of the three runs, Runs 1 and 2, were selected for analyses.
The results of the analyses of these  samples are presented in the Appendix,
along with the firing conditions for each of the Runs 1, 2, and 3.
     The primary purpose of the Runs  1 and 2 data presented in the Appendix
was to reduce the practice the various sampling and analysis procedures
under actual fluidized-bed operation.  Although FBC emission data are

                                    36

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                             TABLE 5.  CHANGES MADE BETWEEN RUN NOS. 1 AND 2
                    Change Mode
                                                                  Reason for Change
6.


7.
Proximate/ultimate analysis made on bed material -325 M
in Run No. 1; discontinued in Run No. 2

Fe, Al, Si, K, Cl~, F~ analyzed individually (e.g., atomic
absorption, ion electrode, etc.) in bed material samples
in Run No. 1; determined these elements by SSMS in Run
No. 2

NCL, SO , S , and CO  anions added to the analysis of bed
material and particulate samples in Run No. 2

Analysis for POM increased to include bed material,
sludge, and particulate samples in Run No. 2

Organic class analyses increased to include bed material
and sludge samples in Run No. 2

Increased analysis of trace elements to include sludge
samples in Run No. 2

Increased particle size analysis to include bed material
and particulate (both >27 and <27 microns) samples in
Run No. 2
                                                                   Analysis of little use
                                                                   More efficient, eliminate dupli-
                                                                   cation
More completely define anion concen-
trations in solid samples

More completely define the POM levels
in solid samples

More completely define organic classes
in solid samples

To better define trace elements in
effluent waste material

To define particle size ranges more
completely
    Reduced quantity of solid sample for bioassay from 20
    grams in Run No. 1 to 2 grams in Run No. 2
                                                               Only 2 grams of sample needed for
                                                               analysis

-------
currently quite limited, the data obtained in Runs 1 and 2 also merit
some evaluation in terms of other coal burning emissions — both fluidized-
bed and pulverized coal combustion emissions.  Tables 6, 7, and 8 present
s uch comp ar is ons.

General
     In Table 6 some average comparisons are made between the Run 2 FBC emis-
sion data and some small scale pulverized coal (PC) firings  (8).  The  latter1
were data obtained by Battelle on another EPA program, Contract No.
68-02-2119, concerned with the combustion of specially treated coals.  The
pulverized coal (PC) data shown are for raw  (untreated) coals with sulfur
contents of about 2 percent.  (We have directed our attention to Run 2, rather
than Run 1 here, because it was at a higher temperature, about 1655 F.)
     As regards the gaseous emissions, the principal differences are in the
CO and S02 emission levels.  S02 levels are noticeably lower in the FBC
operation, as expected, due to the capture of S02 by the limestone.  The
limestone capture efficiency in Run 2 for a 4.1 percent sulfur coal was about
67 percent.
     The high CO levels in FBC operation compared with pulverized coal firing
is another characteristic, so to speak, of FBC.  The high CO levels in the
FBC run here also go hand-in-hand with high hydrocarbon emissions and
possibly with low NOX emissions.  Hydrocarbon emission in PC firing are
usually quite low and therefore are often not even measured.
     It is sometimes stated that NO emissions from FBC operations are  lower
than from PC firings.  The data in Table 5 neither support nor contradict
that statement.  In a recent study on FBC NOX emissions under Contract No.
68-02-2138  we also point out this disparity (9).
     Particulate loadings (particles <27 microns, particles  that pass  the
first cyclone) appear quite similar for FBC  and PC firings.  The same  can be
said for POM loadings and for the ash analyses - within the  limits that one
can compare data from a single FBC run.
Trace Elements
     Table 7 shows a comparison of trace element data from an Illinois No. 6
coal (the same type coal as used in this study) and its ash.  The analyses
                                      38

-------
             TABLE 6.  COMPARISON OF DATA FROM FLUIDIZED-BED AND
                       PULVERIZED COAL COMBUSTORS
         Gases
           o2, %
           co2, %
           CO, ppm
           S02> ppm
           NO  , ppm
              A
           HC, ppm(C)
         Particulate
           Loading, mg/m"
           POM,  ug/m3
          Ash
            C,  weight percent
            H
            N
            S
    FBC
   Run 2

    3.6
   17.3
   2090
    730
    350
    360
1640 (1500)*
  5 (72)*

   8-20%
    .25%
  0.1-0.3%
    4-6%
    PC

   2-10%
  13-15%
  90-300
 1200-1500
  200-700
    NA

 1000-6000
  0.1-65

high, to 50%
    0.3%
  0.1-0.4%
   1-3%
*  Run 1.
                                   39

-------
            TABLE 7.  COMPARISON OF TRACE ELEMENT DATA
                      FROM COAL AND ASH OF ILLINOIS NO. 6 COAL
PPMW
Element
As
Be
Br
Ce
Co
Cr
Dy
Eu
F
Fe(xlo4)(a)
Hg
K(xl03)(a)
La
Mn
Na(xl02)(a)
Pb
Sc
Sm
Tb
Yb

ANL
2.1
1.6
4.1

3.2
22

0.2
79
1.2
1.2
1.5
3.9
19
3.0
8.0
2.1
0.005

1.4
COAL
BCL
Run
No. 1
2.7
0.17
4.7

4.0
13


110
>1
0.16
1.2
5.0
80
8.9
0.47
1.6
0.71

0.23


Run
No. 2
<3
2
10

10
100

<0.5
*3
*5
<2
•\,6
20
100
200
<1
3
<1

0.5

ANL

13

38
34
800
8.5

5.2
13
0.007
16
40
160
27
46
34

3.1
11
ASH
BCL
Run
No. 1

2.6

15
2.1
15
1.4

290
>1
<0.01
>5
6.4
60
^14
4.3
1.6

0.19
1.6


Run
No. 2

0.20

50
10
100
3

^5
^2
<0.3
M.O
50
200
30
20
30

0.5
1
(a)   Indicates values in  table that are to be multiplied  by  the
     factor  shown, e.g.,  1.2 is 12000 ppm Fe.
                               40

-------
TABLE 8.  COMPARISON OF TRACE ELEMENTS IN COALS AND COAL PRODUCTS  (yg/g)

Element
As
Ba
B
Be
Br
Ce
Cd
Co
Cr
Cu
Dy
Eu
F
4\(d]
Hf
Hg
K(xl03)
La
Li
Mn
Mo
Ka(xl02)
Ni
Pb
Sb
Sc
Se
Sm
Tb
V
Yb
Zn
Zr

ANL BCL
Run . Run "
TR 3^' No.l
5 2.7
35
93
0.7 0.17
13 4.7
9.8
0.10
1.8 4.0
100 13
9.0
0.2 0.70

25 110
1 1 >1
0.18
0.15 0.16
5.8 1.2
4.2 5.0
0.13
26 80
2.9
6.9 8.9
33
29 0.47
0.3 0.56
1.7 1.6
. 0.29
0.8 0.71

20
<1 0.23
37
10
Coal
(b)
Run Power Mean
No. 2 Plant Value (c>
<3 14
200
<0.03
2 1.6
10 15
50
<30
10 0.6
100 14
30 9.6
<1
<0.5
<_3 61
-5 0.37 1.9
<2
<2 0.070 0.2
-6 1.6
20
20
100 49
30 0.99
200 5 '
<10
<1 35
<0.5 1.3
3
<5 1.9
<1
<0.2
500
<0.5
<10 7.3
300 13
Final
Bed
ANL BCL
Run Run
TR 3 No.l
3.5 0.67
180
33
0.8 <0.18
4.5
15
0.14
0.14
12 1.3
78
0.49
0.25
170
55 0.46
96 1.1
<0.005 <0.01
0.66 -1.6
3.7 6.4
5.7
39 26
1.2
13 3.2
2.3
51 1.9
0.7
1.8 0.16

0.1 0.83

7.0
5.2 <0.49
17
390 28
Run
No. 2
1.0
200
5
<0.005
1.0
5.0
<10
0.3
10
3
<0.2
<0.3
£3
-0.10
<0.5
<0.3
-2.0
2
1
20
<3
2
<2
1
<0.2
1.0
<2
<0.5
<0.1
10
<0.2
<3
20

Power
Plant
Sair.ple
BA
15








82



6.6

0.140




3.5





7.7




58
220
                                 41

-------




Primary Cyclone



Element
As
Ba
B
Be
Br
Ce
Cd
Co
Cr
Cu
Dy
Eu
F
Fe(xlOA)
Hf
Hg
K(xl03)
La
Li
Mn
Mo
Na(x!02)
Ni
Pb
Sb
Sc
Se
Sm
Tb
V
Yb
Zn
Zr
(a) Run
(b) Run
coal
(c) Mean

ANL
Run
TR 3
25
350

2.6

19

11
180

1.8

20
(d> 5.9
2.9
0.46
3.7
31

110

41

95
3
9




4



Power
BCL Plant
Run
No.l
4.1
180
500
2.6
6.0
15
0.67
2.1
15
66
1.4
0.50
290
>1
1.8
<0.01
>5
6.4

60
3.3
-14
23
4.3
0.67
1.6
0.94
1.7
0.19
25
1.6
67
35
TR 3 bed temperature
No. 1 bed temperature
used.
analytical
(d) Recorded values

Run Sample
No. 2 MA
1.0 44
500
50
0.20
0.50
50
<3
10
.100
50 150
3
1
<5
-2 7.0
2
<0.3 0.026
-10
50
10
200
20 12
30
200
20
0.2
30
<5 4.1
5
0.5
500
1
<3 100
200 260
1560 F; Arkwright
1560 F; Run No.

values for constituents in
to be multiplied by 104, e




Secondary Cyclone

ANL
Run
TR 3

860

6.0
3
13

19
300

2.9

10
3.6
6
0.46
5
52

140

72

260
6.2
19




7.5




BCL
Run
No.l
6.1
320
2000
6.0
60
44
1.0
14
87
120
2.0
0.94
450
>1
1.8
14
>10
30
57
60
14
>50
99
43
1.4
7.3
9.4
3.6
0.48
140
2.5
140
120
Run
No. 2
3
300
300
2
1
20
<3
10
100
50
2
1
<_20
-2
<0.5
<0.3
-20
30
20
500
10
50
100
100
1
30
<5
3
0.3
1000
1
<3
200
Power
Plant
Sample
PA
120








230



6.9

0.310




41





27




250
210
coal used.
2 bed temperature 1655


101 different
.g. , reported

coals.
value of
F; Illinois


1 is really
ppmw.
                                 42

-------
were determined by Argonne National Laboratory  (ANL)  (10) and BCL.  The
ash from the burned  coals were obtained from different combustion pro-
cesses.  The ash material analyzed by ANL was from an unquenched gasi-
fier ash of the coal while ash analyzed by BCL was from the primary
cyclone of the FBC unit.  The BCL analyses were spark source mass spec-
trometric analyses;  the ANL  group used different analytical techniques
in their analyses; these include wet chemical,  atomic absorption,
fluorimetry, specific ion electrode, and neutron activation analysis.
     Approximately 2/3  of the BCL and ANL  trace element coal analyses agree
within a factor of three.  Those elements  showing deviation greater than a
factor of  three include Be,  Hg, Mn,  Pb,  Sm,  Yb, Cr,  F, La, and  Na.  Manganese
and lead are  the  only elements  showing  large deviations common  to BCL Runs
1 and  2.   The mercury values in the  ANL data are reported as not representa-
tive of  the  coal  seam.
     Considering  the possible difference in  coal samples, the non-statistical
approach to  these analyses,  and the  different analytical techniques used, the
agreement  of data in the majority of the elements is satisfactory.
     Most  of the  elements  reported  in the  ash of BCL Run No. 1  and the ANL
run deviate  by more  than a  factor of three.  The elements showing large de-
viations are Be,  Co, Cr,  Dy, F,  Fe,  La,  Pb,  Tb, and  Yb.  On the other hand,
all but  five of  the  elements reported  in BCL Run No.  2 ash data agree within
a  factor of  three with  the  ANL  data.   Those  elements showing greater than
factor of  three deviation  are Be, Cr, Fe,  Tb, and Yb, all of which are also
common to  the elements  showing  large deviations in  Run No. 1
     One would not necessarily  expect  the  data  from  the various ash samples
to agree as  closely  as  in  the case of coal,  since the ash samples were taken
from two different combustion processes  (as  mentioned above) and probably
are not  comparable in particle  size.  The  BCL ash sample contained particles
greater  than  27 microns.  The ash size  is  not reported for the  ANL data.
Considering  the possible difference  in  ash sample and the different analytical
techniques,  the ANL  and Run  No. 2 data  are in fairly good agreement.
                                    43

-------
     Table 8 offers an interesting comparison of trace element data from
fluidized-bed and pulverized coal combustors.  These data are derived
from the ANL pressurized FBC study (10),  a coal-fired power plant study (11)
and the present FBC study.   The ANL study was carried out in a 6-inch
diameter pressurized fluidized-bed combustor, quite comparable to Battelle's
unit except the ANL unit was operated at  about 8 atm absolute pressure.
The coal-fired power plant data were obtained from samples from the 180
MW Unit No. 5 of Public Service Company of Colorado's Valmont Power
Station near Boulder, Colorado.
     In the Table 8 data, different coals were used by ANL and BCL in
firing the fluidized-bed combustors.   ANL used an Arkwright coal and BCL
an Illinois No. 6 coal.  However, the bed temperatures for ANL Run TR3
and BCL Run No. 1 were the same, 1560 F.   Data from combustors other than
FBC units are also included in Table 8.
     In summary, the comparison of the emission data in these studies
bears out the reduction to practice of the comprehensive sampling and
analytical techniques developed here for  fluidized-bed combustors.  The
data presented here however should only be used at this time for the
purpose of evaluating the sampling and analysis technique.  This program
was not designed for statistical evaluation of the data.   The data
presented in the two reference studies selected here for comparison
should also only be accepted at face value.
                                    44

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                                  SECTION 5
                   RECOMMENDED SAMPLING AND ANALYSIS PLAN

     The generalized S&A plan for fluidized-bed units is presented in Table
9.  This plan is similar to the one presented in Table 3 with appropriate
additions in Table 9 to include those sample streams not covered in sampling
the Battelle FBC unit.  Table 9 lists all the main streams to be considered
in sampling a FBC unit, specific pollutants involved, collection technique,
analysis method and level approach.
     Two areas of analysis shown in Table 9 which may require further brief
comment are the biological testing and radionuclide measurements.  In refer-
ence to biological testing, currently it is felt that five tests of a
screening nature are available to evaluate cytotoxicity, mutagenicity, and
carcinogenicity.  These tests are:
     1.  Ames' bacterial mutagenesis toxicity assays
     2.  BCL - prescreen toxicity assay (Mammalian cells - BALB/c 3T3)
     3.  BALB/c 3T3  clonal transformation assay (mouse fibroblast cell)
     4.  C3H 10T 1/2 mouse prostrate cell assay
     5.  Syrian hamster embroy clonal transformation assay.
A more detailed description of the assay options available is presented in
the Battelle report referenced earlier.
     Radioactive content of samples should be considered in an overall samp-
ling program.  It is suggested that a low background proportional counter be
used to make the measurements.  The proportional counter gives a measure of
the gross a and 3 emissions from thorium, uranium, radium, and their  decay pro-
ducts in the samples being analyzed.  The instrument is highly sensitive and
                                                     	-i r\
can detect radioactivity levels below a picocurie (10 x  curies).
     Some of the procedures involved in the analysis of other components
shown in Table 9 have been discussed previously.  Other analytical procedures
                                      45

-------
 IT1
 W
5
C/3
H
S
X
n
iS
33
M
25
Spaciei, Pollutants Sample Analysis Method^*' System Stream or Material
Collection f ) (Stream Number)
Techniques '

C02 Cw NDIR
S02 Cw Infrared or UV
N0 Cw NDIR or Chemiluminescence
N02 Cw NDIR or Chemi luminescence
CO Cw NDIR
°2 Cw Paramagnetic or Ft. ElectrodP

Integrated CQE Phase MM8,,re«enta
H2S IG GC
COS IG GC
DIsul fides IG GC
S°3 2S°A ^t Goksoyr-Ross/Ion chroma tography
NH3 St Kjeldahl
Cyanides St Coloriraetric
HC1 St Titration

Integrated Specimens Collected for Subsequent Group Analysis
Trace metals SASS/Gs SSHS
Major Elements (Fe, Al, Si, K, Ca) SASS/Cs OES
Organic, by class SASS/Gs Extraction/Liquid Chromatography/IR
Organic-reduced, sulfur compounds SASS/Gs GC/FPD (8 fractions combined)
POM SASS/Gs GC/HS
Proximate Gs ASTM D3172-73


Atmospheric Stack Gaa (la)

>10ti U3u
	

























i











X
X
X
X
X
:
X
Ultimate SASS/CB ASTM PJ176-74 ' ' X
Sulfur forms Cs ASTM D2492-68 ' i
Biological SASS/Gs In vitro

Toxic Elements (Be,Cd,Hg,As ,Pb,Se,Sb,Te) -SASS/Gs AA
Cl SASS/Gs Color imetric |
F~ SASS/Gs Distillation/ Colorimetric
Na Gs AA
X

X
X
X
<3U

















X
X
X
X
X

X
Filter

X
X
X
X
X
X
X

1


X
X
X
X
X



X
X
X











X

X


















!




X









Pressur-
ized
Supply.
f!4)



















X
X
Particulate
Removal
2nd Cyclone

















X
X
X
X
X ' X

X








X

X

x



- 4
X


X
X
X
,X
X
X

: X


X

Bed
(3)

















X
X
X
X
X

X


X

X

X


X
X
X
X
X
X
X

X
X

Fuel
Feed
(16)

















X
X
X
X
X
X
X
X
X
X

X


Sorbent
Feed
(19)

















X
X




X


X

X


X :
X X
X
X
! x
X
i--:—
X
X
X
X

X
; x
x
X
X
X
X
X

X
X


Leachate
from Bed ,
(32)




\
ace
from
2no
cy-
mt '

























X X










X





X
X X
X X





X X
X X
i r
i x
i x





1 	 ?_
J





     M5    - EPA Method 5
(a)   Cw    - Continuous withdrawal  through  non-reactive line with mechanical filtration
     Ci    - i>s'-ade Impuctor  in  flowing  stream.
     Gs    - Grab multiple samples  riffled  to reduce to 100 g representative sample.
     IG    — Integrated grab sample of  gas  in glass bulb.
     St    — Separate wet chemical  train  to collect gas (such as
     SASS  - Source Assessment: Sampling System.  
-------
can be obtained from the reference methods given in the table; some are simply
standard calorimeteric or titration procedures for the listed component.
     One other area to be considered in the environmental assessment of a
FBC unit is the noise generated by the unit and its associated components.
The analysis should include an inventory of all significant noise sources.
Noise emission data would be obtained for each source through direct measure-
ment and/or from available literature.  An integrated noise effect, taking
into account transmission paths and isolation, would be generated from appro-
priate existing computer programs.  One can develop a map of noise intensity
within and exterior to the plant.
     Table 9 is suggested for use in planning an effective sampling and
analysis program for specific fluidized-bed units.  Proper selection of
streams and pollutants to be measured can be obtained from Table 9 (with the
necessary prior information on the FBC unit).  One can then proceed to
sample the FBC unit and develop an analysis scheme, such as shown in Table 4,
for each stream sampled.
AREAS NEEDING FURTHER STUDY AND/OR CONSIDERATION
     In the course of this program, it became apparent that certain areas in-
volving (1) the sampling and analysis of samples,  (2) the associated costs
and timing involved in carrying out a sampling program, and (3) the Level 1,
2, 3 approach to sampling should receive further consideration.  Specific
areas of concern are presented below:
     1.  Two questionable areas were encountered in S03 sampling — (1)
         the accuracy of the Gb'ksoyr-Ross method in determining 803
         levels, and (2) the importance of flue-gas temperature in
         sampling 803.  The wide variation in S03 levels encountered
         in this sampling program suggests that both the collection
         method and flue-gas temperature effects should be examined
         further to assess their relative importance in obtaining
         representative 803 samples.
     2.  Further consideration should be given to the effectiveness
         of sorption solutions in removing trace elements and the
         acidic and basic components from the gas stream.  Also, what
         interference problems exist and how may they be overcome.
     3.  Cyclones were used to separate the particles into different
         size ranges.  The larger cyclone in the flue-gas stream of
         our unit appeared to work properly (removing particulates
         >27 ]i).  The smaller cyclones in the Method 5 rigs produced
         somewhat of a problem in that they tended to plug after

                                      47

-------
several minutes of sampling.  The small cyclones were heated
to about 375 F which should reduce sticking tendencies in the
particles.  Nevertheless, the particles clung to the neck of
the small cyclones making a clean-cut separation impossible.
Enlarging the neck of the cyclone improved the separation but
Changed the size fraction range in the cyclone.  Further con-
sideration should be given to these cyclones if used:.in the
Method 5 rig.
A further look at the effect on the sample of using cold
traps to remove moisture, and pyrex wool filters to retain
particles, would be worthwhile in the gas analysis part of
the sampling.
The use of stainless steel tubing in sampling N02 should re-
ceive careful attention since heated stainless steel can
reduce N02 to NO.
If time requirements for analysis is an important factor in
the sampling and analyses program, the following should be
considered (1) the actual time requirements needed to carry
out a complete analysis of all samples regardless of other
factors, and (2) the time required to have an analysis
carried out taking into consideration other activities of
the contractor's analytical laboratory.  The latter area may
lead to the need of analytical assistance from outside
laboratories.  The contractor should therefore have a clear
understanding of the identity of such laboratories, the
quality and reliability of their work, and the cost for
analysis.

An item requiring serious consideration in a sampling and
analysis program is the cost involved in carrying out the
analyses (as well as the sampling) part of this program.
Cost estimates should be made for each analysis carried
out on each sample.  This requires a detailed analysis plan
such as shown in Table 4.  Consideration of costs prior to
sampling can be an important factor in determining the ex-
tent of sampling and/or analysis carried out in the program.

The Level 1, 2, and 3 approach to sampling and analyzing a
FBC unit was not entirely satisfactory for our program.  It
was felt that a combined Level 1-Level. 2 approach would be
more cost and information effective than strictly adhering
to Level 1 sample and analysis procedure.  This is especially
true for certain group analyses where it would be better to
obtain sufficient and proper samples to analyze for indi-
vidual components in a group (e.g., 803 =, 804 = N02~ N03~)
than to analyze the group as a whole.  Also it appeared
well worthwhile to spend extra time obtaining samples of
specific components, e.g., HCN, NH3, etc., than to return
later for these samples.
                             48

-------
                                REFERENCES
1.    Ackerman, D. G., Ryan, L. E., Maddalone, R. A., and Flegal, C. H.,
      Suggested Approaches for Environmental Assessment Level I Data
      Reviews and Level II Analyses, TRW Defense and Space Systems Group,
      Contract No. 68-01-3152, March, 1977.

2.    Abelson, H. I. and Lowenbach, N. A. , Review of Sampling and Analysis
      Techniques for the Environmental Assessment of Fluidized-Bed
      Combustors, MITRE Corp., 1976, EPA Contract No. 68-02-1859.  (Report
      subsequently issued as EPA 600/7-77-009, January, 1977.)

3.    IERL/RTP Environmental Assessment Guideline Document, First Edition,
      Draft Report, January, 1976.

4.    Allen, J. M., Howes, J. E.,  and Miller, S. E., Planning Study on
      Comprehensive Analysis of Emissions from Fluidized-Bed Combustion
      Units, Battelle's Columbus Laboratories, Contract No. 68-02-2138,
      August, 1976.

5.    IERL/RTP Procedures Manual:  Level I Environmental Assessment, TRW
      Systems Group, Contract No.  68-02-1412, June, 1976.

6.    Standards  of Performance for New Stationary Sources, Federal Register,
      41  (111),  June 8, 1976.

7.    Ibid, December 23, 1971.

8.    Stambaugh, E. P., Giammar, R. D., Merryman, E. L., McNulty, J. S.,
      Sekhar, K. C., Thomas, T. J., Grotta, H. M., Levy, A., and Oxley,
      J. H., Study of the Battelle Hydrothermal Treatment of Coal
      Process, EPA Contract No. 68-02-2119, November 11, 1976.

9.    Creswick,  F. A., Engdahl, R. B., Levy, A., Nack, H., and Weller, A. E.,
      Technical  Program Planning — NO  Formation and Control in Fluidized-
      Bed Combustion Systems, EPA  Contract No. 68-02-2138, September 27,
      1976.

10.   Swift, W. M., Vogel, G. J.,  Panck, A. F., and Jonke, A. A., Trace
      Element Mass Balances Around a Bench-Scale Combustor, Proceedings,
      Fourth International Conference on Fluidized-Bed Combustion, McLean,
      Virginia, December 9-11, 1975.

11.   Kaakinen, J. W., Jorden, R.  M., Lawasani, M. H., and West, R. E.,
      Trace Element Behavior in Coal-Fired Power Plant, Env. Sci. and
      Tech., 9. (9), 862-9, 1975.


                                    49

-------
                  APPENDIX A
FLUIDIZED-BED COMBUSTION SAMPLING AND ANALYSIS
      DATA REPORT - RUN NOS. 1, 2, AND 3
                      50

-------
                                 APPENDIX A
               FLUIDIZED-BED COMBUSTION SAMPLING AND ANALYSIS
                     DATA REPORT - RUN NOS. 1, 2, AND 3
     This appendix presents the sampling and analysis data obtained from
Run Nos. 1 and 2, carried out in January and April, 1976, respectively.
Firing conditions and gaseous components measured in Run No. 3 are also
included.  It is the sole intent here to present the sampling and analysis
data.  It is not the intent of this report to analyze the results in terms
of the overall fluidized-bed combustion process.
     The purpose of this program was to develop comprehensive procedures
for collecting and analyzing fluidized-bed combustion reactants and
emission products.  Battelle's 6-inch fluidized-bed combustion unit was
used to carry out Run Nos. 1, 2, and 3 toward accomplishing the objective
of this program.
     Samples were collected and analyzed in accordance with the original
(Run No. 1) and revised  (Run No. 2) Fluidized-Bed Sampling Plan submitted
to EPA.  Figure A-l shows the sampling locations used to obtain data for
Run Nos. 1, 2, and 3.  The sample  identification numbers associated with
each location are derived as follows.  Each sample is given a three-digit
number, e.g., S-l-6-3, where the first digit represents the run number
(here  #1), the second digit gives  the sample location (position 6 in the
example), and the last digit is the sample number for that location
(sample 3 at location 6 in the example).
     Table A-l in Run Nos. 1 and 2 gives a breakdown of the samples taken
from each location and the analyses performed and is the key for identifying
all samples taken in the runs.  No significant amount of reduced sulfur
compounds, b.P.<450 C, were found  in the Run No. 1 samples.  Therefore,
no table on reduced sulfur compounds is given in Run No. 1  (see Table A-ll
Run No. 2).  Tables A-14 through A-19, Run No. 2, list the appropriate

                                    51

-------
            Cyclone
    n
Bed /,
&
/
Air
             Y
           Participate
            >27tt.  ©
            Cool
        Limestone C?)
                                         Flue Gas Analyzers
                                          I     1     I      I     I     I
                                         CO   C02   ,02  S02   NOX  ,THC
                                                Gas Absofetion
                                                    Trains    C9)
                                                Scrubber
                                                      -TenoxPlug &
                                                      (Pom, He)
                                      Mod. Method 5 Trains
                                          t      I   {
                                          Parficulate
                                      Porticulate
                                     <27jj   >2.3p
       Ash
   FIGURE  A-l.   SCHEMATIC  OUTLINE OF FLUIDIZED BED COMBUSTOR
                 AND SAMPLING LOCATIONS,  RUN NO. 1
                                  52

-------
detection limits for the analysis procedures used in this program.   The
tables in general are self-explanatory.  Noise measurement data are given
in the following section.  An estimated cost breakdown for groups of
samples taken in Run No. 2 are given in Table A-18 at the end of data
presentation.
Noise Measurements
     Some acoustic measurements were made in the laboratory in which the
Battelle's Multisolid Fluidized-Bed Combustor is located.  This particular
unit is very quiet; the support equipment makes more noise than the com-
bustion bed itself.
     The following table shows the sound pressure levels as a function of
center frequency octave bands.  These measurements were taken with the micro-
phone inside the enclosure, one foot away from the bed.

Center Frequency
  Octave Bands
  sec -1          31.5  63    125  250  500    1000  2000  4000   8000  16000
Sound Pressure
  Flat Level, dB  72.5  64.5   68   68   66.5    66  61.5  58.5     56     50

     The present OSHA requirements is to keep the A-weighted level* at 90 dBA
or  less for an  8-hour per day exposure.  The measured levels were well below
this level.
     The sound  pressure level at a distance of 2 ft away from the rotary feed
pump was 78 dBA A-weighted, and 82 dB on the flat scale.  The background noise
was 68 dBA on A-weighted, and 79 dB on the flat side.
     The acoustic radiation from this small model is not a valid indication of
the noise generation  potential of a full-scale model.  However, it is quite
possible that even in full-scale combustion beds, the support equipment will
make more noise than  the combustion bed itself.
*  An adjusted scale taking into account the response of the human ear at var-
   ious frequencies; the A-weighted level (dBA) is always less than the flat
   level  (dB) at a given frequency.
                                    53

-------
                                         TABLE A-l.   SAMPLE  IDENTIFICATION  AND  ANALYSES,  RUN NO.  1
                    Material
                 Illinois tt coal
                  (-8 M)
  Fluid-Bed    Sample Number
_ Sample  No.    Designation
                                                                 S-l-1-1
                                                                 S-l-1-3
                                                                                 Proximate/ultimate
                                                                                                     (1) Moisture  (3) Volatile Batter
                                                                                 Sulfur
                              ' Pa, Ca

                               Heating value

                               Trace metals
                                                                                                     (2) Ash
                                                                   Fixed carbon (by
                                                                    difference)
                                                   (1) Total     (3) Organic
                                                   (2) Pyrites    (4) SO
                                                                                        (5) C, H, N, S,  0 (b
                                                                                            difference)
01
                 Grove limestone
                 Bed material
                Ash (-325 M)
                 Sludge
S-l-2*

S-l-3

S-l-4


\ S-l-2-2
S-l-3-1
\ S-l-3- 2
S-l-4-1
-*^ S-l-4-2
\ S-l-4-3
                                                                                 Ca, Mg,  CO
                                                                                 Trace metals
                                                                                 Trace metals
                               C, H, N,  S, 0, SO.,  and SO,
                                               4       3
                               Fusion temperature

                               Trace metals
                               C, H, N,  S, 0, S04> and
                 Flue gas stream
                 Particulars >27u
                                                                 S-l-6-1
S-l-6*
/ S-l-6-2
\\ S-l-6-3
                                                                 S-l-6-4
                               Trace metals  (approx 60 metals)

                               Cations-Fe, Al, Si, K,  and C, H, N, S,  0
                               Anions Cl~, F~, N0~  S0°
                                                3    4
                               Organic classes
                              "POM
                               Organic and reduced sulfur compounds

-------
                                                                            TABLE  A-l.
                        Material
                     Flue gas stream
                     Particulate <27ii
Fluid-Bed
Sample No




Sample Number
Designation
S-l-7-1
/S-l-7-2
"\\ S-l-7-3
\ S-l-7-4
       Analyses
 Trace metals
 Cations - Fe, Al, Si,  K plus  C,  H,  H, S, 0
 Anions Cl ,  F ,  N0~,  SO,
 Organic classes
''POM
 Organic and  reduced sulfur  compound*
                                                               (AL-3)    S-l-9-1
                     Flue gas stream
                     Gases
Ui
                     Cases,  continuous
                      monitoring

S-l-9*

S-l-10*

-«L S-l-9-2
W\ S-l-9-3
^\ S-l-9- 4
V\ S-l-9-5
\ S-l-9- 6
S-l-10-1
/ S-l-10- 2
4f S-l-10-3
\\ S-l-10-4
\\ S-l-10-5
\ S-l-10-6
^-~.
(AL-2)
(AL-2)
(AL-2)
CAL-4)
(AL-3)






^Org
HC1
HCN
NH3
Tra
so3
°2
co2
CO
so2
NO
X
HC
 Organic classes
 ,POM
 Organ!cs - reduced sulfur
                                                                                         Trace elements (solution)
                                                                                             (Gokaoyr-Ross )
                    *  Composite samples of duplicate runs.

-------
TABLE A-2. SUMMARY OF RUN NO. 1 CONDITIONS
Run Number:
BCL Number:
Coal feed rate, Ib/hr
Limestone feed rate, Ib/hr
Air feed rate, Ib/hr'
Bed height: expanded, inches
settled, inches
Bed temperature, F
Superficial gas velocity,
ft/sec
Ca/S ratio
Particulate loading grams/in
1A
AL-2
15.5
11.2
139.9
48
11.8
1560
8.9
5/1
NA
IB
AL-3
16.9
17.9
144.4
48
13.3
1530
9.0
7.3/1
1.43
1C
AL-4
15.2
17.0
150.6
48
11.8
1525
9.4
7.7/1
1.40
                    56

-------
                           TABLE A-3.  SIEVE ANALYSIS, RUN NO. 1
       Illinois No.  6
 Sieve No.
Wt. Percent
                      Grove Limestone
Sieve No.
Wt. Percent
                                Overflow Bed Material
Sieve No.
Wt. Percent
  -8 + 16
 -16 + 20
 -20 + 50
 -50 + 100
-100 + 200
-200 + 325
-325
   28.0
   17.4
   32.6
    9.7
    4.9
    1.3
    6.1
 -8 + 10
-10 + 12
-12 + 16

-16 + 20
-20
   4.2
  17.0
  37.7

  41.1
     0
 16
-16 + 20
-20 + 30
-30 + 40
-40 + 50
-50 + 100
-100
   44.6
   33.8
   17.1
    4.3
    0.07
    0.02
    0.04
                                          57

-------
TABLE A-4.  PROXIMATE/ULTIMATE ANALYSES OF FLUIDIZED-BED SAMPLES, RUN NO. 1
Material
Illinois id coal
Bed material
Participate >27p
(-325 mesh)
On
00 Sludge
Paniculate >27y
Particulat* <27p
Weight Percent
Sample Volatile Fixed Sulfur
Number HjO Ash Matter Carbon C HNS 0 Total Pyrltic Organic Sulfate SOj
S-l-1-1 3.67 11.2 38.4 46.7 62.9 4.6 1.1 4.47 12.0 4.47 2.41 1.99 0.07 —
and
• S-l-1-2
S- 1-3-2 3.65
S-l-4-1 1.0 72.0 25.0 0.4 0.4 3.29 . 2.84 H.D.
S-l-5-1 1.24 61.7 26.3 0.9 0.4 1.31 8.2 0.45 H.D.
S-l-6-2 <0.05 77.3 20.5 0.3 0.3 4.47 1.20
and
S-l-6-3
S-l-7-2 0.28 88.9 8.2 0.2 0.1 5.93 3.24
and
S-l-7-3

-------
             TABLE A-5.  METAL AND ANION ANALYSES ON FLUIDIZED-BED SAMPLES, RUN NO.  1
Sample Weight Percent
Material
Illinois 86 coal
Grove limestone
Particulate >27p


Number Na Ca Mg CO Fe
S-l-1-1 0.23 0,41 0.06 0.68
S-l-2-1 37.1 0.51 57.7
S-l-6-2 5.42
and
S-l-6-3
Al Si K Cl F NO
________ _ __

2.53 6.00 0.47 0.12 0.005 0.008


Particulate <27p   S-l-7-2                                6.68    7.36   11.0     2.10    0.48    0.019    0.003
                    and
                  S-l-7-3

-------
TABLE A-6.  ANALYSES  OF ACIDIC AND  BASIC  GASES  FROM FLUE
           GAS  SAMPLES WITHDRAWN FROM STACK AT 568 F, RUN NO.  1
Component
HC1
HF
HCN
NH3
so3*
Sample
Number
S-l-9-2
S-l-9-2
S-l-9-3
S-l-9-4
S-l-9-6
Collection
Method
0.01N NaOH
0.01N NaOH
5% KOH
IN H2S04
Goksjfyr-Ross
, 3
mg/m
62.9
0.065
0.077
1.24
58.9
ppm
43.5
0.082
0.070
1.8
18.6
  *   See  page  47, Recommendation  (1).
                        60

-------
TABLE A-7- TRACE ELEMENTS  BY  OPTICAL  EMISSION

          SPECTROSCOPY  SAMPLE  NO.  S-l-9-5

          (Collected  in KMnO,), RUN NO. 1
                                          (a)
Component                             ppmw
   Hg



   Cd                                 <50



   As                                 <50



   Se



   Te



   Pb                                  <5



   Ba
(a)
    All components were near or below minimum

    detection limit.
                     61

-------
                  TABLE A-8.  POM ANALYSIS, RUN NO. 1
NAS(l)
Component Notation
Anthracene/Phenanthrene
Methyl Anthracenes ?
Fluoranthene -
Pyrene
Methyl Pyrene/Fluoranthene ?
Benzo(c)phenanthrene ***
Chrysene/Benz (a) anthracene *
Methyl Chrysenes ?
Benzo Fluoranthenes **
Benz(a)pyrene ***
Benz(e)pyrene
Perylene -
3-Methylcholanthrene ****
Indeno(l,2,3,-cd)pyrene *
Benzo (ghi)perylene -
Dibenzo (a, h) anthracene ***
Diebenzo(c,g)carbazole ***
Dibenz(ai and ah)pyrenes ***
Coronene
Total
3
Sample Weights, yg/m
Sample Number
, S-l-9-1
57.3
9.4
3.2
0.95
0.73
0.17
0.37
0.17











72.2
(1)   Carcinogenicity rating as listed by National Academy of Sciences in
     "Particulate Polycyclic Organic Matter", 1972.
     Not carcinogenic.
 *   Carcinogenic.
**9  *A*S **** Strongly  carcinogenic.
?    Carcinogenicity not indicated by NAS.
                                  62

-------
TABLE A-9. ORGANIC CLASS ANALYSES
           RUN NO. 1
Organic
1
2
3
4
5
6
7
8
Sample Weight ug/gram
Sample No.
S-l-6-4 S
309
10.9
21.8
29.1
4.7
9.6
6.4
13.1
sample
-1-7-4
750
35
55
85
50
75
35
20
                 63

-------
       TABLE A-10.   LEVEL 1 ANALYSES  OF ORGANIC CLASSES,  RUN NO.  1
                    (Refer to  Table A-9 for  total mass of each fraction)
Fraction
        S-l-6-4
         S-l-7-4
   2
   3
   4
   5
   6
Vinyl unsaturated hydrocarbons

Aliphatic esters
Aliphatic esters, ketone
Phthalate ester
                                               Aliphatic hydrocarbons, vinyl
                                                 unsaturated hydrocarbons
Aliphatic esters
Conjugated ketone or quinone
Phthalate ester
                                    64

-------
TABLE A-ll. ANALYSES OF GASEOUS COMPONENT IN
            FLUIDIZED-BED SAMPLES, RUN NO.  1
Sample
Number
S-l-10-1
S-l-10-2
S-l-10-3
S-l-10-4
S-l-10-5
S-l-10-6
Component
0?, percent
C0?, percent
CO , ppm
S02, ppm
N0x, ppm
HC, ppmC
Average
Value
6.5
14.3
790
700
415
85
                    65

-------
TABLE A-12.   TRACE ELEMENT ANALYSIS OF FLUIDIZED-BED SAMPLES,
             RUN NO.  1,  ppmw(a)  (Except where designated percent)
Element
Li
Be
B
F
Na
Mg
Al
Si
P
S
Cl
K
Ca
Sc
Ti
V
Cr
Mn
Fe
Co
Ni
Cu
Zn
Ga
Ge
As
Se
Br
Rb
Sr
Y
Zr
Nb
Mo
Ag
Cd
Sn
Sb
Te
I
(111.
#6 Coal)
S-l-1-3
0.13
0.17
93
110
890
400
>1%
>1%
3.2
>0.5%
= 1100
=1200
=4000
1.6
240
20
13
80
>1%
4.0
33
9.0
37
1.7
2.0
2.7
0.29
4.7
21
80
9.4
10
3.1
2.9
—
0.10
0.28
0.56
<0.37
0.10
(Grove
Lime-
stone)
S-l-2-2
2.9
<0.18
6.2
140
140
>0.5%
= 3000
>1%
140
240
18
>0.5%
>1%
<0.11
87
7
0.87
15
=1200
0.14
0.69
2.2
4.0
0.23
—
<0.61
—
1.2
7.3
470
1.7
7.0
0.32
0.67
—
—
0.12
—
—
2.9
(Bed
Material)
S-l-3-1
5.7
<0.18
33
170
320
>0.5%
=3000
>0.5%
310
>0.5%
120
=1600
>1%
0.16
130
7
1.3
26
= 4600
0.14
23
78
17
1.1
1.4
0.67
—
4.5
7.3
470
3.6
28
0.69
1.2
—
0.14
0.55
—
	
0.29
(Partic-
ulate
>27 p
-325)
S-l-4-3
220
18
710
290
=3200
>0.5%
>1%
>1%
310
310
240
>0.5%
>1%
0.73
870
38
32
210
>1%
14
46
78
80
2.3
3.0
2.0
4.4
12
37
140
8.3
35
3.2
3.3
0.30
0.67
0.92
0.67
	
1.2
(Partic-
ulate
>27 y)
S-l-6-1
NR
2.6
500
290
=1400
>0.5%
>1%
>1%
310
310
240
>0.5%
>1%
1.6
870
25
15
60
>1%
2.1
23
66
67
2.3
3.0
4.1
0.94
6.0
20
470
3.6
35
3.2
3.3

0.67
1.2
0.67
	
0.58
(Partic-
ulate
<27 u)
S-l-7-1
57
6.0
= 2000
450
>0.5%
>0.5%
>1%
>1%
310
310
300
>1%
>1%
7.3
= 2200
140
87
60
>1%
14
99
120
140
11
14
6.1
9.4
60
37
250
29
120
16
14
0.30
1.0
12
1.4

29
                             66

-------
                             TABLE A-12.
Element
Cs
Ba
La
Ce
Pr
Nd
Sm
Eu
Gd
Tb
Dy
Ho
Er
Tm
Yb
Lu
Hf
Ta
W
Hg
Tl
Pb
Bi
Th
U
(111.
#6 Coal)
S-l-1-3
0.65
35
5.0
9.8
2.1
6.6
0.71
—
0.40
—
0.70
—
0.34
—
0.23
—
0.18
0.27
0.31
0.16
0.59
0.47
—
1.7
1.0
(Grove
Lime-
stone)
S-l-2-2
0.19
90
2.2
2.9
0.86
1.7
0.31
—
—
—
0.20
—
—
—
<0.21
<0.15
1.8
0.33
<0.22
<0.01
—
0.86
<0.24
0.34
0.34
(Bed
Material)
S-l-3-1
0.43
180
6.4
15
2.0
3.8
0.83
0.25
—
—
0.49
—
0.11
—
<0.49
<0.15
1.1
0.87
<0.32
<0.01
—
1.9
<0.24
1.1
0.80
(Par tic -
ulate
>27 y
-325)
S-l-4-3
4.4
180
6.4
11
2.0
7.5
1.7
0.50
0.32
0.25
2.0
0.39
0.28
—
1.6
0.38
0.79
0.43
0.36
0.01
1.0
7.2
<0.24
5.7
4.0
(Partic-
ulate
>27 y)
S-l-6-1
1.9
180
6.4
15
2.0
10
1.7
0.50
0.32
0.19
1.4
0.16
0.28
—
1.6
0.50
1.8
0.87
<0.32
<0.01
0.48
4.3
<0.24
2.4
1.7
(Partic-
ulate
<27 y)
S-l-7-1
4.3
320
30
44
15
21
3.6
0.94
0.69
0.48
2.0
0.61
0.56
0.14
2.5
0.50
1.8
0.87
1.1
14
10
43
0.80
11
8.0
(a)   Rhenium  and  Indium used  as internal standards.  Gold, Platinum, Iridium,
     Osmium,  Lutecium, Thullium, Holmium, Palladium, Rhodium, Ruthenium pre-
     sent  at  less  than 0.1  ppm/wt.
                                     67

-------
                                    TABLE A-13.   SAMPLE IDENTIFICATION AND ANALYSES,  RUN NO.  2
cr>
CO
Fluid-Bed Sample Number
Material Sample No. Designation

Illinois 16 coal
(-8 H) S-2-1

Crove limestone
S-2-2

Bed material S-2O

Aah (-325 M) S-2-4

Sludge S-2-5

Flue gas scream ,
Parttculate >27p
S-2-1-1 /
-/ S-2-1-2
\ S-2-1- 3
\;-2-l-4
S-2-2-1
\ S-2-2-2
\S-2-2-3
S-2-3-1
^X 3,2-3-0
\S-2-3-2
^e-2-3-3
S-2-4-1
-*T S-2-4-2
\ S-2-4-3
\<5-'-4-4
• S-2-5-1
\ S-2-5-2
\£-?-5--5
S-2-6-1
/ S-2-6-2
~\V S-2-6-3
\ S-2-6-4
Proximate/ultimate j |;
/ (e
^ Sulfur ||J
^ Na, Ca
Heating value
Trace metals
Particle Size
_ Ca, Mg, CO* NO" NO"
trace metals
Particle Size
Trace metala
Organic Classes
_ SO", so^, S=, NO", NO"
Particle Size
Nor, NO", S*. SO", and
Fusion temperature
Trace metals
Organic Classes
C, H, N, S, 0, SO^, and
Trace Metals
Organic Classes
Trace metals (approx 60
C, H, N, S, 0
Aniona, NO", NO" SO
- 2" 3
Organic classes
A
) Moistu
) Aah
; oW
) Total
j Pyrite
so;
necals)
• «
4' S03
                                                                                             Moisture  (k)  Volatile matter
                                                                                                     (5;  Fixed carbon (by
                                                                                                         difference)
                                                                                                    »rence;
                                                                                                     (3)  Organic
                                                                                                     (4)  SO,
                                                       Partioai Size
                                                                       Organic and reduced sulfur compounds

-------
                                  TABLE A-13.
   Material
Flue gas stream
Participate <27u
                    Fluid-Bed
                    Sample No.
Sample Number
 Designation
                                   S-2-7-1
                                   S-2-7-4
 Particle
                                            Size
      Analyses

Trace metals

 C,  H,  N,  S,  0
Anions, CO",
                                      ,  So , SO
Organic classes
POM
Organic and reduced sulfur compounds
                          (AL-3)   S-2;9-l
                                                     Organic classes
Flue gas stream
Cases
Gaaea, continuous
 monitoring

s-e -9 j-

c j _-in _


/ S-2-9-2 (AL-2)
1\ S-2-9-3 (AL-2)
V\ S-2-9-4 (AL-2)
A S-2-9-5 CAL-4)
Vs-2-9-6 (AL-3)
S-2-10-1
/ S-2- 10- 2
/;/ s-2-10-3
\\ S-2-10-4
\\ s-2- 10- 5
Vs-2-10-6
^Organics - reduced sulfur
HC1, HF
HCN
Trace elements (solution)
SO. (Gokaoyr-Rosa)
°2
co2
CO
so2
NO
X
HC

-------
   TABLE A-14.  SUMMARY OF RUN NO.  2 CONDITIONS
Coal feed rate, Ib/hr                    8.8
Limestone feed rate, Ib/hr               4.3
Air feed rate, Ib/hr                    87.3
Bed height:  expanded, inches           48
             settled, inches            21.6
Bed temperature, F                    1655
Superficial gas velocity ft/sec          6.0
Ca/S ratio                               2.9
Particulate loading g/m                  1.64
                         70

-------
TABLE A-15.  SIEVE ANALYSIS, RUN NO. 2
Illinois Coal # 6
Sieve No.
+ 8
-8 + 12
-12 + 16
-16 + 20
-20 + 30
-30 + 50
-50 + 100
-100 + 200
-200 + 325
-325
Wt. %
0.14
13.93
18.61
14.32
12.91
17.92
9.28
5.14
5.42
2.32
Limestone Overflow Bed Material
Sieve No. wt. % Sieve No.
-8 + 12 32.53 20
-12 + 16 34.26 -20 + 30
-16 + 20 24.69 -30 + 40
-20 8.51 -40 + 50
-50 + 100
-100 + 200
-200



Wt. %
71.10
18.47
7.47
2.16
0.66
0.05
0.12



                  71

-------
     TABLE  A-16.  PROXIMATE/ULTIMATE ANALYSES OF FLUIDIZED-BED  SAMPLES,  RUN  NO.  2
Material
Illinois #6 coal
Sludge

Particulate >27V
Particulate >27y

Sample u n
No. 2
S-2-1-1 8.8
S-2-5-1 1.5

S- 2-6-2 1.6
S-2-7-2 0.6

Volatile
Ash Matter
10.5 36.4
83.9

62.7
88.8
Weight Percent ^

Fixed Sulfur(b)
Carbon C H . N 0 Total SO," Pyrites
44.3 62.5 4.5 2.3 7.3 4.07 — 1.65
— 13.0 0.4 0.3 0.6 0.25 none
detected
32.4 0.4 1.1 0.1 1.66
— 8.7 0.2 0.1 — 1.9
Organic Sulfates
2.10 0.32
0.09

See Table A-17
ditto
(a)  Dashes in Table indicate no analysis made.  Lower limit of detection for each component listed in Table is about 0.10 percent.
(b)  All values reported as sulfur.

-------
                     TABLE  A-17.   METAL AND ANION ANALYSES OF FLUIDIZED-BED SAMPLES, RUN NO. 2
                                                                 Weight Percent
        Material
No.
           NO
                                                                         _/ \
                                                                            C0
                                                                 Na
Ca
Mg
Co
Illinois #6 Coal

Limestone

Overflow bed
  material

Bed material ash,
  -325 mesh

Particulate >27 y

Particulate <27 y
S-2-1-1

S-2-2-1  <0.0003   <0.0003

S-2-2-2   0.0012    0.0007
S-2-4-1   0.012


S-2-6-3   0.006

S-2-7-3   0.002
                                             0.0043
                                                       0.04
                            0.16
                                             0.0008     0.31

                                             0.0006    <0.1
                                    <.01
                                              20.2
                                      0.14    16.4


                                               3.37

                                               5.34
                                                                                 0.11   0.16

                                                                                57.6     —    37.6   0.64
                                                       6.45

                                                       5.97
     (a)   Divide  sulfate values  by 3  for  use in Table  A-16.

-------
TABLE A-18.  ANALYSES OF ACIDIC AND BASIC GASES FROM
             FLUE GAS SAMPLES WITHDRAWN FROM STACK
             AT 260 F, RUN NO. 2
Sample
No.
S-2-9-2
S-2-9-2
S-2-9-3
S-2-9-4
S-2-9-6
Component
HC1
HF
HCN
NH3
so3*
mg/m
55.3
0.57
0.20
4.87
0.46
ppm
37.3
0.70
0.18
7.05
0.14
       *  See page 47, Recommendation (1).
                         74

-------
TABLE A-19.  TRACE ELEMENT ANALYSES OF FLUIDIZED-BED
             SAMPLES BY ATOMIC ABSORPTION AND OPTICAL
             SPECTROSCOPY, RUN NO. 2

                    Sample No. S-2-9-5
Component
Hg
Cd
As
Se
Te
Be
Pb(b)
Ba(b)
ppmw
0.007
<0.04
0.03
<0.03
<0.2
<0.02
<1.0
<1.0
ng/m
9 (a)
<52
39
<39
<260
<26
<1300
<1300
      (a)  Near lower detection limit.  May be
           some contribution from solvent.
      (b)  Determined by optical emission
           spectroscopy; all others by atomic
           absorption.
                          75

-------
                       TABLE A-20.    POM ANALYSES,  RUN  NO.  2

NAS (1) 	 	
Component Notation S-2-3-4
Anthracene/phenanthrene - <"
Methyl anthracenes '
Fluoranthene "

Pyrene
Methyl pyrene/fluoranthene ?
Benzo (c)phenanthrene ***
Chrysene/benz(a)anthracene *
Methyl chrysenes ?
7 , 12-Dimethylbenz (a) anthracene ****
Benzo f luoranthenes **
Benz(a)pyrene **x
Benz(e)pyrene -
Perylene ~
Methylbenzopyrenes ?
3-Methylcholanthrene ****
Indeno(l,2,3,-cd)pyrene *
Benzo (gh i) peryiene
Dibenzo(a,h)anthracene ***
Diebenzo(c,g)carbazole ***
Dibenz(ai and ah)pyrenes ***
Coronene -
(b)
Minimum Detection Limit $
3(a)
	 ng/m 	 	 	
S-2-4-4 S-2-5-3 S-2-6-4
<0.04 470 <4
36.8
511
91 .9

20.4
16.3
81.7
20.4
<0.1
51.0

25.5
1.0
10.2
<0.1
2.0
2.0
<0.1
<0.1
<0.1
<0.1
0.04 o.l 4
(a) Use the following conversion factors to convert from ng/m to ng/gram sample
only, i.e., S-2-9-1 not included)
Sample No: S-2-3-4 S-2-4-4

S-2-5-3 S-2-6-4 S-2-7-4


S-2-7-4 S-
810
73.6
331
36.8

14.7
18.4
73.6
11.0
<0.7
58.9

36.8
<0.7
7.4
<0.7
7.4
7.4
<0.7
<0.7
<0.7
<0.7
0.7
(solid samples




2-9-1
2667
561
1404
211

28.1
14.0
35.1
3.5
<0.4
8.8

3.5
<0.4
1.8
<0.4
3.5
3.5
<0.4
<0.4
<0.4
<0.4
0.4



   Multiply values by:       0.023       11.7        1.42        0.06
                                                                          0.53
(b)   Detection limits vary with sampling conditions encountered, i.E.,  in accordance with amount
     of  sample collected and  gas volume involved.  For solid samp}es the average detection limit
     in  units of ng/gram sample is about 0.27.

(1)   Carcinogenicity rating as listed by National Academy of Sciences In "Particulate Polycyclic
     Organic Matter , 1972.                                                            ' '
     Not carcinogenic.
 *   Carcinogenic.
**,  ***_ **** Strongly  carcinogenic.
 ?   CarcinogCTilcity not indicated by NAS.
                                               76

-------
         TABLE A-21.  ORGANIC CLASS ANALYSES, RUN NO. 2
Organic
Class
1
2
3
4
5
6
7
8
3 (a)
yg/m
S-2-3-4
1288
41
275
170
135
381
381
52.7
S-2-4-4
33.5
2.5
6.3
5.6
3.0
2.3
7.2
3.3
S-2-5-3
247
231
214
184
91.9
150
124
28.7
S-2-6-4
372
422
144
112
73.8
66.8
162
38.7
S-2-7-4
144
83.2
150
118
70.7
141
536
8.1
S-2-9-1
4158
605
2364
1873
610
919
1033
10.9
(a)   Multiplication factors given in Table A-20 can be used here to
     convert from yg/m^ to yg/gram sample (solid samples only).
                                77

-------
        TABLE A-22.  LEVEL 1 ANALYSES OF ORGANIC CLASSES, RUN NO. 2
                     (Refer to Table A-21 for total mass of each
                      fraction)

Sample 2-3-4
     Cut 1 - Aliphatic hydrocarbon containing a significant amount of vinyl
             unsaturation.
     Cut 2 through 6 - Contain only traces of hydrocarbon structure.
             Quantity of material is very low.
     Cut 7 - Material concentration extremely low.  A trace of aliphatic and
             carbonyl structure is present.

Sample 2-4-4
     Cut 1 - Aliphatic hydrocarbon containing a small amount of unsaturation
             including vinyl.
     Cut 2 - Alphatic hydrocarbon containing a small amount of carbonyl.
     Cut 3 - Aliphatic hydrocarbon containing some aliphatic ester.
     Cut 4 - Carboxylic acid ester plus aliphatic ether groups, possibly
             a vinyl ether.
     Cut 5 - A small amount of phthalate ester.
     Cut 6 - Nil
     Cut 7 - Primarily aliphatic - 2 different carbonyls are present, one of
             which is probably a ketone.

Sample 2-5-3
     Cut 1 - Aliphatic and fused ring aromatic hydrocarbons; pyrene and
             benzpyrene types are possible.
     Cut 2 - Similar to 1 but concentration of fused ring aromatics is higher.
     Cut 3 - Some of the fused ring aromatics of cuts //I and #2 but primarily
             an aromatic ketone.  Nitrile* groups are present.  A small amount
             of hydroxyl structure is present.
     Cut 4 - Aromatic ketone and quinone structures.  Small amounts of
             nitrile* and hydroxyl.

     Cut 5 - Aromatic ketone and quinone structures.  A trace of nitrile.  A
             small amount of anhydride or other strained ring carbonyl is
             probable.

     Cut 6 - A complex mixture of many types of carbonyl, aliphatic, aromatic
             structures and with a trace of nitrile*.
     Cut 7 - Same as Cut 6.

     Cut 8 - Only a trace of material; complex carbonyl structures.
                                     78

-------
                           TABLE A-22.  (Continued)
Sample 2-6-4
     Cut 1 - Aliphatic hydrocarbons.
     Cut 2 - Ester (very small amount of material).
     Cut 3 - Trace of ester plus other carbonyl.
     Cut 4 - Trace of material containing several carbonyls.
     Cut 5 - Trace of material containing carbonyl.
     Cut 6 - Trace of material containing carbonyl.
     Cut 7 - Trace of material containing carbonyl.
     Cut 8 - Nil
Sample 2-7-4
     Cut 1 - Aliphatic and fused ring aromatics plus silicone.
     Cut 2 - Aliphatic and fused ring aromatics plus a small amount of ester.
     Cut 3 - A mixture of aliphatic and aromatic esters plus a trace of
             nitrile*.
     Cut 4 - Ester, ketone, and quinone are probable; both aromatic and
             aliphatic structure are present.
     Cut 5 - Aliphatic ester, probably unsaturated.
     Cut 6 - Aromatic strained ring or halogenated carbonyl.
                                      79

-------
                               TABLE A-23.   REDUCED  ORGANIC  SULFUR  ANALYSES,  RUN NO. 2
oo
o
Component
Overflow bed material

-325 mesh overflow
bed material
_

Particulate >27u
Particulate <27u

Tenax


Sludge
Reduced Organic Sulfur
Sample With Retention Time Wit
No. Wt. Gram of Benzothiophene of
S-2-3-4 15.0 None


S-2-4-4 3.9


S-2-6-4 9.5 20
S-2-7-4 5.1 None

S-2-9-1 — 1500


S- 2-5-3 13.8 40
Compounds, ug
h Retention Time
Dibenzothiophene Miscellaneous
None None



1

5
5 2 cpds X. 5 ug
each
800 8 cpd's at 20
to 100 ug each

200 1 cpd — 100 ug
Remarks
No reduced organic sulfur
compounds found in S-2-3-4 or
S-2-4-4 above 5 ug. About one
dozen nonsulf ur compounds .
Major portion in C^& to €22
range; 25 to 500 ug quantities.
50 ug napthalene
10 to 40 u g nonsulf ur cpd's
in C10 t0 C16 range
2 non-sulfur compounds at leve!
of about 5000 V g and 15 at
200 to 1000 ug
About 20 nonsulfur compounds
at levels of 50 to 500 u g
           (a)  ug of material found in total sample weight given in Column 3.  Minimum detection limit is about 0.5 yg for the above samples.

-------
TABLE A-24.  ANALYSES OF GASEOUS COMPONENTS
             IN FLUIDIZED-BED SAMPLES,
             RUN NO. 2
                                Average
    Component                    Value


    0 ,  percent                    3.6

    CO ,  percent                  17.3

    CO,  ppm                     2090

    SO ,  ppm                     730

    NO ,  ppm                     350
      X
    HC,  ppm C                    360
                 81

-------
TABLE A-25.  TRACE ELEMENT ANALYSIS OF FLUIDIZED-BED
             COMBUSTION SAMPLES, RUN NO. 2, ppmw
             (except where designated percent)
Grove -325M
111. Lime- Bed Bed
#6 Coal stone Material Material Sludge
Element S-2-1-3 S-2-2-2 S-2-3-1 S-2-4-3 S-2-5-2
Li
Be
B
F
Na
Mg
Al
Si
P
S
Cl
K
Ca
Sc
Ti
V
Cr
Mn
Fe
Co
Ni
Cu
Zn
Ga(a)
Ge
As
Se (a)
Br
Rb
Sr
Y
Zr
Nb
Mo
Ru
Rh
Pd
Ag (a)
Cd
In (a)
20
2
<0.03
<3
^2%
^2%
^5%
•^20%
100
5000
M3.5!
M).6:
5000
3
5000
500
100
100
^5%
10
<10
30
<10
<5
100
<3
<5
10
20
500
30
300
3
30
<1
<0.5
<3
<3
<30
<10
3
<0.005
1
27y <27y
S-2-6-1 S-2-7-1
10
0.2
50
<5
3000
5000
^5%
^20%
50
1000
800
. -VIZ
•v7%
30
1000
500
100
200
•^2%
10
200
50
<3
<5
3
1
<5
0.5
5
200
30
200
3
20
<0.5
<0.2
<2
<1
<3
<1
20
2
300
<20
5000
^1%
•v-5%
^20%
200
3000
^1%
-v2%
^7%
30
VL%
1000
100
500
•^2%
10
100
50
<3
<10
10
3
<5
1
10
300
200
200
5
10
<0.5
<0.5
<2
<1
<3
<1
                         82

-------
                          TABLE A-25.
Grove -325M
111. Lime- Bed Bed
#6 Coal stone Material Material
Element S-2-1-2 S-2-2-2 S- 2-3-1 S-2-4-3
Sn
Sb
Te
I
Cs
Ba
La
Ce
Pr
Nd
Sm
Eu
Gd
Tb
Dy
Ho
Er
Tm
Yb
Lu
Hf
Ta
W
Re
Os
Ir
Pt
Au
Hg
Tl
Pb
Bi
Th
U
<1
<0.5
<1
3
3
200
20
50
5
^
<1
<0.5
<1
<0.2
<1
<0.3
<0.5
<0.3
<0.5
<0.3
<2
<0.5
<1
<1
<\
<1
<1
<0.5
<2
<1
<1
<0.5
<1
<0.5
<1
<0.1
<0.3
1
<0.3
100
2
2
0.3
0.5
<0.3
<0.3
<0.3
<0.3
<0.2
<0.05
<0.2
<0.05
<0.2
<0.05
<0.5
<0.3
<0.3
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
<0.1
3
<0.1
<0.2
<0.5
<1
<0.2
<0.3
0.5
0.3
200
2
5
0.3
0.5
<0.5
<0.3
<0.3
<0.1
<0.2
<0.05
<0.2
<0.1
<0.2
<0.05
<0.5
<0.3
<0.3
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
<0.2
1 '
<0.1
0.2
0.5
200
2
<0.3
3
5
300
20
50
5
5
5
2
5
0.5
2
0.5
2
0.2
0.2
<0.1
1
<0.3
1
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
5
300
1
10
5
Sludge
S-2-5-2
100
1
<0.3
1
3
5000
200
500
20
50
30
10
20
2
10
3
5
1
5
0.5
10
<1
2
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
10
200
10
50
20
Partic- Partic-
ulate ulate
27 27
S-2-6-1 S-2-7-1
<2
0.2
<0.3
0.5
0.5
500
50
50
5
20
5
1
1
0.5
3
0.5
0.5
0.3
1
<0.1
2
<0.2
0.3 .
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
5
20
<0.1
5
2
10
1
<0.5
5
2
300
30
20
5
20
3
1
3
0.3
2
0.5
1
0.1
1
<0.1
<0.5
<0.2
<0.3
<0.2
<0.2
<0.2
<0.3
<0.1
<0.3
10
100
1
5
2
(a)   Memory from previous sample.
                                83

-------
 TABLE A-26.  APPROXIMATE DETECTION LIMITS FOR  SAMPLES RUN  ON
               SPARK SOURCE MASS SPECTROMETER, RUN NO. 2
               (refer to Table A-25)
Element
Li
Be
B
F
Na
Mg
Al
Si
P
S
Cl
K
Ca
So
Ti
V
Cr
Mn
Fe
Co
Ni
Cu
Zn
Ga
Ge
As
Se
Br
Rb
Si
MDL*
(PPMW)
0.005
0.005
0.03
0.5
0.1
3.0
10.0
2.0
0.3
0.5
0.5
0.5
0.5
0.3
0.3
0.3
0.3
0.3
0.3
0.3
2.0
0.3
1.0
0.3
0.2
0.3
1.0
0.3
0.3
0.3
Element
Y
Zn
Nb
Mo
Ru
Rh
Pd
Ag
Cd
In
Sn
Sb
. Te
I
Cs
Ba
La
Ce
Pr
Nd
Sm
Eu
Gd
Tb
Dy
Ho
Er
Tm
"Yb
Lu
MDL
(PPMW)
0.3
0.3
0.3
0.3
0.3
0.3
0.3
1.0
3.0
1.0
1.0
0.1
0.3
0.3
0.3
0.5
0.3
0.5
0.2
0.5
0.3
0.3
0.3
0.1
0.2
0.05
0.2
0.05
0.2
0.05
Element
Hf
Ta
W
Re
Os
Ir
Pt
Au
Hg
Tl
Pb
Bi
Th
U
















MDL
(PPMW)
0.3
0.2
0.3
0.2
0.2
0.2
0.3
0.1
0.3
0.1
0.2
0.1
0.1
0.1
















Minimum detection limit for samples of approximate composition studied in program.
                                  84

-------
TABLE A-27.  DETECTION LIMITS FOR METALS ANALYSIS
             BY ATOMIC ABSORPTION, RUN NO. 2
             (refer to Table A-19)
Element
Hg
Cd
As
Se
Te
Be
Pb(b)
Ba(b)

ppm
0.005
0.04
0.01
0.03
0.2
0.02
1.0
1.0
MDL(a)
(ng/m )
6.5
52
13
39
260
26
1300
1300
         (a)  Minimum Detection Limit for
              samples of approximate com-
              position analyzed in this
              study

         (b)  Determined by Optical
              Emission Spectroscopy.
                        85

-------
TABLE A-28.  DETECTION LIMITS FOR ACID AND BASIC GASES,
             RUN NO.  2 (refer to Table A-18)

Compound
HC1
HF
HCN
NH,
Solution Analysis
Method of
Analysis
Ion Chromato graph
Ion Chromatograph
Ion Selective Electrode
Ion Selective Electrode

MDL , ppm
0.06
0.06
0.03
0.03
(a)



                 Ion Chromatograph             0.01
     (a)  Minimum Detection Limits for samples
          collected in this program.
                          86

-------
TABLE A-29.  DETECTION LIMITS FOR ANIONS AND METALS,
             RUN NO. 2 (Solid Samples, refer to Table A-17)
Compound
co3=
NO
NO
so4=
so "
Analysis Method
Titration
Colorimetric
Colorimetric
Gravimetric
Titration
MDL
(Wt. Percent)
0.05
0.0003
0.0003
0.05
0.05
  s
  Ca
  Mg
  Na
                     0.01
Atomic  absorption    .01
                      .01
                      .01
                        87

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TABLE A-30.SAMPLES FROM RUN NO. 2 AND ESTIMATED COST FOR ANALYSES
         Analysis
  Run No.  2
Sample Number
Estimated
Cost, 1976
  Particle size
  Trace element
  Minor elements
  Organic classes/POM/
    organic sulfur
  CHNSO
  Anions

  (a) SO^,  S0=3,  S=,  N0~,

        and N0~
  (b)  SO,,  SO,,  S   N0
        t    J    ,

        and NO,,
                                   S-2-1-4
                                   S-2-2-3
                                   S-2-3-3
                                   S-2-6-5
                                   S-2-7-5
                                   S-2-8-5
                                   S-2-1-3
                                   S-2-2-2
                                   S-2-3-1
                                   S-2-4-3
                                   S-2-5-2
                                   S-2-6-1
                                   S-2-7-1
                                   S-2-8-1
   S-2-3-4
   S-2-4-4
   S-2-5-3
   S-2-6-4
   S-2-7-4
   S-2-8-1

   S-2-1-1
   S-2-5-1
   S-2-6-2
   S-2-7-2
   S-2-8-2
                                   S-2-3-2
                                   S-2-5-1
                                   S-2-6-3
                                   S-2-7-3
                                   S-2-8-3
                       $ 400
                        3600
                        1400
                        6240
                                                         750
                         440
                         660
                               88

-------
                      TABLE A-30.
Analysis
(c) SO^, Soij
(d) N0~, N0~, CO^
S03
Elemental Analysis
(AA)
(a) Hg, Cd, As, Pb,
Se, Te, Be
(b) Ca, Mg
(c) Na, Ca
Proximate
Run No. 2
Sample Number
S-2-5-1
S-2-2-1
S-2-9-6

S-2-9-5
S-2-2-1
S-2-1-1
S-2-1-1
Estimated
Cost, 1976
$ 120
150
60

420
120
120
90
Sulfur (total, pyritic,
  organic, and sulfate)                                180
                                 S-2-1-1
                             89

-------
-C
en
QJ
0
^

E
o
   99.8

   99.5

     99

     98
90


80

70

60

50

40

30
     10
    0.5
    0.2
      0.6  08   I
t
                                                
-------
yy
98
95
90
80
? 70
o>
* 60
>.
^ 50
§ 40
£ 30
O)
•| 20
o
1 10
o
5
2
1
0.5
0.2
n i


























^
















-U















y>
















/















3
































/














X
/
j
CS-?-fi-T>






















































































































































































































20    30  40    60   50 100       200    300 400   600 800 1000
                              Particle Diameter, microns (i)

              FIGURE A-3.   PARTICLE  SIZE ANALYSIS, RUN NO. 2
                             (S-2-6-3 Particulate >27  y, Cyclone No.  1

   (1)  Aerodynamic size, i,e., equivalent  spherical particles of unit  density.
2000  3000   5000

-------
TABLE A-31.  SUMMARY OF RUN NO. 3 CONDITIONS




 Coal feed rate, Ib/hr                   9.2

 Limestone feed rate, Ib/hr              8.1

 Air feed rate, Ib/hr                   84.2

 Bed height:   expanded, inches          48.0
              settled, inches           21.6

 Bed temperature, F                   1490.0

 Superficial  gas velocity,  ft/sec        5.3

 Ca/S ratio                              7.1
                     92

-------
TABLE A-32.  SIEVE ANALYSIS, RUN NO. 3
Overflow Bed Material
Illinois No.
Sieve No .
+8
-8 + 12
-12 + 16
-16 + 20
-20 + 30
-30 + 50
-50 + 100
-100 + 200
-200 + 325
-325
6 Coal
Wt. %
0.14
13.93
18.61
14.32
12.91
17.92
9.28
5.14
5.42
2.32
Limestone Run AL8
Sieve No. Wt. % Sieve No.
-8 + 12 32.53 20
-12 + 16 34.26 -20 + 30
-16 + 20 24.69 -30 + 40
-20 8.51 -40 + 50
-50 + 100
-100 + 200
-200




Wt. %
76.80
13.96
5.21
2.36
1.49
0.12
0.07



Run AL9
Sieve No.
20
-20 + 30
-30 + 40
-40 + 50
-50 + 100
-100 + 200
-200




Wt. %
77.68
14.90
4.85
1.79
0.72
0.03
0.03



                   93

-------
TABLE A-33.   ANALYSES OF GASEOUS COMPONENTS IN
             FLUIDIZED-BED SAMPLES, RUN NO. 3
         Component
                    Average
                     Value
02, percent

CO,.,, percent

CO, ppm

S02, ppm

NO , ppm

HC, ppm C
                               3.3

                              18.3

                            4790.0

                             620.0

                             300.0

                             900.0
                     94

-------
                                TECHNICAL REPORT DATA
                          (Please read Instructions on the reverse before completing)
1. REPORT NO.

  EPA-600/7-77-034
2.
                           3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
 Method for Analyzing Emissions from Atmospheric
 Fluidized-Bed Combustor
                           5. REPORT DATE
                            April 1977
                           6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
 E.L. Merry man, A. Levy, G.W.Felton, K.T.Liu,
    J.M.Allen, and H. Nack
                                                      8. PERFORMING ORGANIZATION REPORT NO
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Battelle-Columbus Laboratories
 505 King Avenue
 Columbus,  Ohio 43201
                           10. PROGRAM ELEMENT NO.

                            EHB536
                           11. CONTRACT/GRANT NO.

                            68-02-1409, Task 33
 12. SPONSORING AGENCY NAME AND ADDRESS
 EPA, Office of Research and Development
 Industrial Environmental Research Laboratory
 Research Triangle Park, NC 27711
                           13. TYPE OF REPORT AND PERIOD COVERED
                            Task Final; 9/76-3/77
                           14. SPONSORING AGENCY CODE
                             EPA/600/13
 ^.SUPPLEMENTARY NOTES T£RL-RTP project officer for this report is Walter B. Steen,
 Mail Drop 61,  919/549-8411 Ext 2825.
 16. ABSTRACT Tne repOrj- describes an experimentally developed method to comprehen-
 sively sample and analyze an atmospheric-pressure fluidized-bed combustion (FBC)
 unit.  The method is aimed at providing a cost and information effective environmen-
 tal assessment of FBC units.  The report includes a general discussion of the perti-
 nent areas likely to be encountered in sampling and analyzing specimens from FBC
 units; for example, streams encountered in FBC units, the selection of streams,
 procedures for sampling gaseous, solid, and liquid streams, and the multilevel
 analytical approach to emission characterization defined by EPA for combustion units.
17.
                             KEY WORDS AND DOCUMENT ANALYSIS
                DESCRIPTORS
                                          b.IDENTIFIERS/OPEN ENDED TERMS
                                        c.  COSATI Field/Group
 P Dilution
 Fluidized-Bed Processors
 Atmospheric Pressure
 Sampling
 Analyzing
 Emission
               Pollution Control
               Stationary Sources
               Fluidized-Bed Com-
                 bustion
               Environmental Assess-
                 ment
13B
07A
04B
14B
13. DISTRIBUTION STATEMENT
 Unlimited
               19. SECURITY CLASS (This Report)
               Unclassified
!1. NO. OF PAGES

   97	
               20. SECURITY CLASS (This page)
               Unclassified
                                                                   22. PRICE
EPA Form 2220-1 (9-73)
                                         95

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