EPA-600/2-77-242
December 1977
Environmental Protection Technology Series
                             FLY ASH CONDITIONING
                             WITH SULFUR TRIOXIDE
                                 Industrial Environmental Research Laboratory
                                       Office of Research and Development
                                      U.S. Environmental Protection Agency
                                 Research Triangle Park, North Carolina 27711

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                     RESEARCH REPORTING SERIES
 Research reports of the Office of Research and Development, U.S. Environmental Protec-
 tion Agency, have been grouped into nine series. These nine broad categories were
 established to facilitate further development and application of environmental tech-
 nology. Elimination of traditional grouping was consciously planned to foster technology
 transfer and a maximum interface in related fields. The nine 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. Interegency Energy-Environment Research and Development
           8. "Special" Reports
           9. Miscellaneous Reports

 This report has been assigned to the ENVIRONMENTAL PROTECTION TECHNOLOGY
 series. This series describes research performed to develop and demonstrate instrumen-
 tation, equipment, and methodology to repair or prevent environmental degradation from
 point and non-point sources of pollution. This work provides the new or Improved tech-
 nology required for the control and treatment of pollution sources to meet environmental
 quality standards.
                             REVIEW NOTICE
This report has been reviewed by the participating Federal Agencies, and approved for
publication. Approval does not 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 recommendation for use.

This document is available to the public through  the National Technical Information
Service, Springfield, Virginia 22161.

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                                          EPA-600/2-77-242
                                             December 1977
FLY ASH CONDITIONING
WITH  SULFUR  TRIOXIDE
                   by

         Edward B. Dismukes and John P Gooch

            Southern Research Institute
             2000 Ninth Avenue, South
            Birmingham, Alabama 35205
             Contract No. 68-02-2114
                 Task No. 1
            •  ROAP No. 21ADL-027
           Program Element No. 1AB012
          EPA Task Officer: Leslie E. Sparks

       Industrial Environmental Research Laboratory
        Office of Energy, Minerals, and Industry
          Research Triangle Park, N.C. 27711
                Prepared for

       U.S. ENVIRONMENTAL PROTECTION AGENCY
         Office of Research and Development
             Washington, D.C. 20460

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                        Table of Contents

Section                                                   Page

  I      Introduction and Summary	       1

 II      Background	       5

III      Results from Test Program	       7

 IV      Mass Balance Considerations	      50

  V      Computer Model Projections of Precipitator
           Performance	      59

         Acknowledgements	      63

         References	      64
                               ill

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                         List of Tables

Table No.                                                Page

    1      Mass Train Results Reported by Research
           Cottrell	        16

    2      Mass Train Results Reported by Kin
           Associates	        18

    3      In situ Resistivity from George Neal
           Plant,  Unit 2	        20

    4      George  Neal-Unit 2,  Average voltages
           and currents for 3/27/76	        31

    5      Average voltages and currents  for
           5/17/76	        32

    6      Ultimate Analyses of Coal  Samples	        34

    7      Analyses of Flue Gas	        35

    8      Analyses of Hopper Ash	        40

    9      pH  Values  and Soluble S0i,~2  Concentra-
           tions   of  Hopper Ash	        42

  10      pH  Values  and Soluble Sulfate  Concentra-
           tions of Cyclone Samples of  Ash	        46

  11      pH  Values  and Soluble SO4~2  Concentra-
           tions of Filter  Samples of Ash	        48

  12       Injected S03 Found in Outlet Cyclone
           Samples of Ash	        57

  13       Injected S03 Found in Outlet Filter
          Samples of Ash	        58
                               IV

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                         List of Figures

Figure No.                                                  Page

    1       Inlet Size Distribution (Cumulative
            Percent)  for March 27, 1976 with 90%
            Confidence Intervals .......................       8
    2       Inlet Size Distribution (Cumulative Mass)
            for March 27, 1976 with 90% Confidence
            Intervals ..................................       9

    3       Average Inlet Size Distribution (Cumulative
            Percent) for May 18-21, 1976 with 90%
            Confidence Intervals .......................      10

    4       Average Inlet Size Distribution (Cumulative
            Mass) for May 18-21, 1976 with 90%
            Confidence Intervals .......................      11

    5       Outlet Size Distribution  (Cumulative
            Percent) for May 19, 1976 ..................     13

    6       Outlet Size Distribution  (Cumulative Mass)
            for May 19, 1976 ...........................     14

    7       Fractional Efficiency  for May 19, 1976
             (Based on single outlet sampling point)....     15

    8       Resistivity Probe Voltage -Current
            Characteristics without SO3 Injection ......     21

    9       Resistivity Probe Voltage-Current
            Characteristics with S03  Injection .........     23

    10       Arrangement of Transformer  Rectifier  Sets
            for  George Neal Unit 2 .....................     24

    11       V-I  Characteristics for TR  Set  3 on
            March  27, 1976 .............................     25

    12       V-I  Characteristics for TR  Set  4 on
            March  27, 1976 .............................     26

    13       V-I  Characteristics for TR  Set  7 on
            March  27, 1976 .............................     27

    14       V-I  Characteristics for TR  Set  8 on
            March  27, 1976 .............................     28
                                  v

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                         List of Figures
                           (Continued)

Figure No.                                                  Page

   15       V-I Characteristics for TR Set 3 on
            May 21,  1976	      29

   16       V-I Characteristics for TR Set 8 on
            May 21,  1976	      30

   17       Comparison of Predicted Gas Concentrations
            (Functions of Excess Air)  with Observed
            Concentrations (Displayed by Dashed
            Horizontal Lines)	      36

   18       Hopper Configuration for the Precipitator..      38

   19       Soluble SO.,"2 in Hopper Ash as a Function
            of Hopper Location or Gas Temperature	      43

   20       Locations for Sampling with Series
            Cyclones	      45

   21       Comparison of H2SCK Concentrations at the
            Dew Point with Experimental Results	      53

   22       Relationship between Flue-Gas Temperature
            and Experimental HaSOi, Concentrations	      54

   23       Computer Model Projections of Collection-
            Efficiency without SO3	      60

   24       Computer Model Projections of Collection-
            Efficiency with S03	      62
                                VI

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                   I.   INTRODUCTION AND  SUMMARY

     This report describes a study conducted by Southern Research
Institute for the purpose of evaluating an S03 injection system
for the George Neal Unit 2 Boiler of Iowa Public Service Company
in Sioux City, Iowa.  The SO3 injection system was supplied by
Research Cottrell for the purpose of increasing the collection
efficiency of the electrostatic precipitator installed on the sub-
ject boiler.  The study was sponsored jointly by Iowa Public Service
Company and the Industrial Environmental Research Laboratory of
the Environmental Protection Agency.   Mass loading determinations
were conducted by Research Cottrell and Kin Associates.  EPA's
portion of the study was concerned primarily with accounting for
the fate of the injected conditioning agent with emphasis on stack
losses of SO3, whereas IPS's objective was to determine whether
the injection system would provide a means of reliably increasing
the precipitator collection efficiency to 99% at full load with
normal plant operating conditions.  A second objective of IPS was
to obtain an estimate of the specific collecting area which would
be required to achieve 99.0% collection efficiency without condi-
tioning when the precipitator is collecting fly ash produced from
the low sulfur, low sodium western coal which is used for fuel at
this installation.
     The study consisted of a two-phase test program that was fol-
lowed by appropriate laboratory measurements and analyses.  The
two phases of the test program were:   (1) An evaluation of precipi-
tator performance at full load without S03 injection.  These tests
were conducted on March 27, 1976.  (2) An evaluation of precipita-
tor performance at full load with SO3 injection.  These tests were
conducted during the week of May 17,  1976.
     Results from the baseline tests on March 27 indicated that, as
expected, precipitator performance was limited by the high electrical
resistivity of the collected dust.  The average collection effic-
iency reported by Research Cottrell was 91.3% at a plant load of
                                 1

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 299 megawatts.  Measurements with a point-plane probe indicated a
 dust resistivity value of approximately  6  x 10>2  ohm-cm at 118°C
 (245°F).   Voltage-current relationships obtained from the TR sets
 also exhibited behavior typical  of precipitators collecting high
 resistivity dust.   These voltage-current relationships were used
 to estimate the allowable electrical  operating  conditions which
 could be  maintained without  back corona or  excessive  sparking in
 the absence of S03  conditioning.   The estimated electrical operating
 conditions, the precipitator geometry,  and  the  measured  particle
 size distributions  at  the precipitator inlet were  used as input
 data to a computer  program which simulates  the  operation of the
 precipitator.   The  computer  program was then used  to  estimate the
 specific  collecting area that would be  required to achieve 99 0%
 collecting efficiency.   If it is  assumed that ^  enlarged precipi_
 tator should include a  sufficient  safety margin to allow about  12%
 of the collecting area  to  be de-energized without  decreasing  per-
 formance  below  99%  collection efficiency, the program output  in-
 dicates that a  specific  collecting area of  108  mV(mVsec)  (550 ft2/
 1000  ACFM)  would suffice.
      The  test program with S03 injection was not conducted  in ac-
 cordance with our original test plan because of difficulties with
 the  SO, injection system and the precipitator TR sets  "tripping
 out    it  is our understanding that the cause of the  difficulty
with  the TR sets was ash build-up in the hoppers.  As  a  result of
 these problems, only one efficiency test at a load of  300 MW was
obtained with the S03 injection system operating continually  and
without transformer-rectifier failures.  The results obtained were
as follows:
                           Outlet Dust
    Test at Stack
       ASME             0.0508(.0222)
       EPA              0.0703(.0307)
EPA  with residue from
first impinger          0 .0828 ( .0362)
                              2
                                              PreciPitator Efficient
                                                        9896

                                                        98>78

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These results were obtained from the Kin Associates report concern-
ing the subject test program, and the precipitator efficiencies are
based on an inlet dust concentration of 10.38 gm/DNm3 at 21°C (70°F)
(4.536 gr/DSCF).   Although the above data indicate the performance
of the precipitator was approaching the desired value of 99%, addi-
tional test data taken after the injection system and precipitator
have operated under reasonably steady-state conditions for several
days would be required to determine if 99% collection efficiency can
be consistently maintained.  This will require a solution to the ash
build-up problem and also a turn-down capability for the S03 system.
The reported rate of S03 injection during the test period was about
25 ppm by volume.
     Our conclusions with regard to the effect of S03 injection at
this rate on the flue gas and fly ash properties, and the precipi-
tator performance, may be summarized as follows:
      (1) Dust resistivity values measured with the point-plane probe
indicated that resistivity decreased to approximately 4 x 1010 ohm-
cm at 143°C  (290°F).
      (2) Voltage-current curves obtained from the precipitator power
supplies indicated that the dust resistivity was not limiting the
electrical operating conditions.  The electrical operating conditions
with SO3 conditioning, the precipitator geometry, and the measured
inlet size distribution were used as input data to the mathematical
model.  The results indicated that a collection efficiency of greater
than 99% is theoretically possible with a specific collecting area
of 39.37 m2/(nt3/sec)  (200 ft2/1000 ACFM) and with the improved volt-
ages and currents.
      (3) At the inlet of the precipitator, where the gas temperature
averaged 128°C (262°F), about 2 ppm of the added SO3 was found in  the
gas phase, and about 23 ppm was found on the suspended fly ash.  Ash
samples were collected and fractionated by size in a series  of
cyclones; variations in the  sulfate content of different samples
may have been  caused by fluctuations in either boiler load  (total
gas flow) or S03 injection rate.  Ash of smaller particle  size contained

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higher weight-percentage of sulfate than ash of larger size,  as expected.
     (4) In the precipitator hoppers adjacent to the center line
through the precipitator, about 15 ppm of the injected S03 was
found as sulfate on the ash.  This quantity of S03 was lower than
expected from other data  (S03 injection rate and S03 found as sulfate
on ash at the inlet and outlet).  The discrepancy presumably was
caused by a lower-than-average rate of S03 injection in nozzles
directly upstream from the hoppers in question.
     (5) At the outlet of the precipitator, where the gas tempera-
ture averaged 118°C  (244°F), less than 1 ppm of H2SCK vapor was
found in the gas stream, and only about 2 to 3 ppm of S03 was found as
sulfate on the ash.  The H2S04 vapor concentration was too low to
be distinguished from that occurring without conditioning.  The
total sulfate on the outlet ash was only about 50% of the value
found without conditioning.  Even though the weight fraction of
sulfate on the ash was increased by conditioning, the product of
 (1) sulfate fraction .and  (2) total ash concentration was lower with
conditioning than without, because of the marked  increase in precip-
itation efficiency.  In other words, the decrease in  factor  (2) as
the result of conditioning was more important  than the increase in
factor  (1).
     In summary, the data indicate that an  adequate accounting was
made for the fate of the  injected  S03 and  that the overall rate of
SO3 emission from the  stack  (counting both  E2SO^  vapor and sulfate
on the  ash) was  lower  with conditioning than without.  Additional
testing will be  required  to  determine whether  the injection  system
 can  enable 99%  collection efficiency  of  fly ash  in  the precipitator
 to be  reliably  achieved.

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                         II.  BACKGROUND

     Collection efficiency measurements on the electrostatic pre-
cipitator installed on Unit 2 of the George Neal Station have in-
dicated that the precipitator performance is appreciably below the
design value of 99% at full load conditions.  Although the precip-
itator performance has in the past reportedly been limited by factors
other than dust resistivity  (specifically, a poor gas velocity dis-
tribution and hopper sweepage),  both the electrical readings of
transformer-rectifier sets and in situ resistivity measurements have
shown that the electrical operating characteristics are severely
limited by dust resistivity.
     In order to achieve the design value for collection efficiency
at this installation, two options are feasible:   (a) increase the
plate area of the precipitator,  and (b) lower the dust resistivity
to the extent that it does not limit the performance of the unit.
Option (a) involves a large capital expenditure since it is esti-
mated that the total plate area would have to be increased by a
factor of about 3 in order to achieve 99% collection efficiency.
The precipitator currently is designed for a gas flow of 512.48
m3/sec at 129°C  (1,086,000 ACFM at 263°F), and  the existing plate
area is 19,906 m2  (214,272 ft2).  This gives a  design specific col-
lecting area of 38.84 m2/(m3/sec) or 197  ft2/1000 ACFM.  In view
of the expense required to enlarge the existing unit the required
amount, Iowa Public Service  decided to evaluate the use of an S03
injection system for the purpose of lowering ash resistivity and
increasing the precipitator  performance.
     The SO3 injection system was supplied and  operated by Research
Cottrell.  The system burns  molten sulfur to produce SO2 which is
subsequently oxidized to S03  in a catalytic reactor.  The gas leav-
ing the converter  is transported to the precipitator inlet duct
through an insulated line,  and injection  into the  flue  gas is accom-
plished with an  insulated manifold.  The  system is  designed with  the
objective of maintaining  the temperature  in the transport  line  and
                                 5

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in the manifold above the HaSCK dewpoint.  The design details of
the SO3 system are not provided in this report as a result of a
confidentiality agreement with Research Cottrell.

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                III.  RESULTS FROM TEST PROGRAM

A.  Particle Size Measurements
     Particle size measurements were conducted during both the
baseline and S03 injection tests with cascade impactors and cyclones.
The purpose of the cascade impactor measurements was to provide
size distribution data for subsequent use in a mathematical model
which was employed to simulate the operation of the precipitator
during the test program.  Multistage cyclones were used primarily
to obtain size fractionated samples for chemical analysis, and result:
from these measurements will be presented in the section on chemical
analyses.
     During the baseline test series (March 27), a total of eight
Brink cascade impactor runs were performed at the precipitator in-
let, and two Andersen impactor runs were performed at the outlet.
Useful data were not obtained from the outlet runs because of sub-
strate sticking and stage overloading.   Inlet impactors runs were
made with four-point traverses in which two points were approximately
0.3 meter (1 ft) apart at the top of the duct and the other two
points were the same distance apart at the center of the duct.  The
traverses were conducted in port Nos. 2, 4, 5, and 7  (See Figure 20).
Figure 1 gives the data obtained from the March 27 inlet series on
log probability co-ordinates, and Figure 2 presents the distribution
in terms of cumulative mass loadings as a function of particle di-
ameter.
     The second series of particle size measurements was conducted
the week of May 17, 1976.  A total of sixteen Brink impactor runs
were conducted on May 18, 19, 20, and 21 using the same traversing
procedure described above.  Outlet Andersen impactor runs were also
conducted on May 19, 20, and 21, but only the data obtained on May
19 are of interest because of problems encountered with the preci-
pitator or the injection system on the other test days.  Figures 3
and 4 give the average inlet size distribution on log probability

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 co-ordinates and in terms of cumulative mass loading for the time
 period May 18-21.  Figures 5 and 6 are similar presentations of the
 size distribution obtained on May 19 at the outlet of the precipi-
 tator.  The cumulative percent distribution is based on the total
 outlet mass loading obtained with the impactor (35.45 mg/DNm3).
 Because of the almost 10 meter (32.8 feet)  depth of the outlet
 duct work, full traverses were impractical.   Therefore, single
 point sampling was performed at a depth of 2.4 meters (7.8 feet).
 This single point outlet size distribution,  together with the
 average of the size distributions obtained on May 18-21,  were used
 to compute the fractional collection efficiencies shown in Figure 7.
 Note that a comparison of Figure  1 and 3 shows that essentially
 the same inlet size distribution  was obtained for the March and
 May test series.   The data from Figure 4 were used in the computer
 model projections,  which will be  discussed in a subsequent section.
 B.   Mass Train Results
      Inlet and outlet mass loadings  for the  baseline test were deter-
 mined by Research Cottrell using  the ASME Power Test Code 27 method
 on  March 27 and March 28.   The inlet sampling location was upstream
 of  the injection  manifold (Figure 20),  and outlet data were obtained
 in  the stack.   These data are given  in Table 1.
      Mass train data during the SO3  injection tests in May were
 obtained by Kin Associates,  Inc.  using the following methods:
      (1)  A modified  ASME sampling train at the  inlet location  with
 an  in-stack filter.
      (2)  A modified  ASME  sampling train at the  stack location  with
 an  in-stack Gelman type AE  glass  fiber  filter.
      (3) An  EPA Method 5  sampling train at the  stack.  Four  tests
were conducted with  this  equipment,  but only one  data  set was  con-
 sidered useful due to problems with  the precipitator or the  S03
 injection system.   The tests were designated as follows:
                                 12

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-------
                           Table 1.   Mass Train Results Reported by Research Cottrell
o\
                 Temperature,°C
     Boiler Load       (°F)
Date      MW       in      Out
                                       Gas Volume,
                                          m3/sec
                                          (ACFM)
                                        In
                                  Collecting1
Dust Concentration                   Area
  gm/m3 (gr/ACF)     Efficiency     m2/(m3/sec)
3-27 299
3-282 299

107
(224)
111
(231)
96
(204)
93
(199)
(833

(740
417
,000)
349
,000)
585
(1,240,
386
(819,
000)

000)
6
(2
6
(2
.32
.76)
.04
.64)
\j
0.
(0
0.
(0.
'ui_ •» |
482 92.4
.21)
593 90.2
259)
Itf/lUOO ACFMJ
34.02
(173)
51 .6
(262)
    1.   Based on outlet flow rates
    2.   Gas  flow appears inconsistent with boiler load.

-------
   Date     Test No.                  Description
  5/19/76      2-1        S02  converter temperature fell;  S03
                          injection rate uncertain
  5/19/76      2-2        Normal test
  5/20/76      2-3        Interrupted due to TR set failure
  5/21/76      2-4        Interrupted due to TR set failure

     Table 2 summarizes the data obtained by Kin Associates on
May 19.  The dissolved solids  in the first impinger were obtained
to determine whether any S03 remaining in the gas phase at the stack
would appear in the residue after evaporation of the liquid.  The
results in Table 2 indicate that the outlet mass loading is increased
about 18% if the impinger solids are included.  Chemical analyses
of the impinger wash were also conducted, and these results are
discussed in a subsequent section.
     It is of interest to compare the mass loadings obtained with
the mass trains in the stack with that obtained from the single
point measurement with the Andersen impactor at the precipitator
outlet.  The Andersen impactor obtained a mass loading of 0.0227
gm/m3  (.00992 gr/ACF) which is only  32% of the results indicated
by the EPA train without inclusion of the impinger.  Thus,  the
fractional efficiencies plotted in Figure 7 are not representative
of the overall precipitator performance.  It is probable that most
of the relatively large particles resulting from  rapping reentrain-
ment are concentrated near the bottom of the duct and were, there-
fore,  not captured by the impactor.  The data  in  Figure 7  should,
however, provide  a reasonably accurate  representation of sub-two
micron collection efficiencies.   Similarly, the  total mass  loadings
obtained with the limited impactor  traverses  at  the inlet  will  show
significant  disagreement with the mass  train  results, but  the  smal-
ler  size  fractions should be  represented with sufficient  accuracy
for  use  as  input  data  to  the  precipitator  computer model.
     A comparison of the  ASME-derived  mass  loadings and precipitator
efficiencies in Tables  1  and  2  shows that,  for the brief period when
                                 17

-------
Table 2.  Mass Train Results Reported by Kin Associates
Gas
B . , Temperature, °c Volume
ouiier (°F) m /sec
Date MW m Out in AC™ out
5-19 303
129
(264)
122
(252)
557 476
(1,180,000) (1,009,000)
Dust Concentration
In
6.85
(2.99)
gm/m
ASME
0.0508
(0.0222)
' (gr/ACF)
Out
EPA & First
0.0703 0.0828
(0.0307) (0.0362)
                                                    Efficiency,  %
                                                          EPA  w/o
                                                    ASME   Impinger

                                                   99.27     98.96
    Specific
   Collecting
      Area
  m2/(m3/sec)
(ft'/lOOQ  ACFM)

      41.82
      (212)
Test
 No.

2-2

-------
normal precipitator operation was possible,  the precipitator per-
formance was increased to the extent that outlet mass concentrations
decreased by about a factor of ten as a result of the S03 injection.
This increase in efficiency is consistent with the improvement in
power supply performance and the decrease in dust resistivity, as
discussed below.
C.  Resistivity Measurements
     In situ resistivity data were obtained with a point-plane
probe1 during both the baseline and S03 injection test series.  These
data are given in Table 3, and it is apparent that dust resistivity
during the S03 injection tests is about two decades lower than it
was during the baseline series.  The data in Table 3 are obtained
with parallel plate cell geometry with an applied electric field
slightly lower than the value which is sufficient to cause spark-
over.  It is also possible to obtain resistivity data from the
voltage-current characteristics of the apparatus with and without
dust on the collecting electrode as illustrated in Figure 8.  The
collecting area of the measurement cell is  5 cm2, and resistivity
may be calculated from the dust  layer thickness  0.09 cm, the  volt-
age difference between the  "clean" and  "dirty"  voltage-current
curves  (5600 volts),  a selected  current  (0.5 x  10~6A), and  the cell
area.  Thus,

             n =   (5600V) (5cm2)       = 6>2 x 1Qn ohm-cm
             p   (0.5 x 10~6A)0.09 cm
at  an  applied  field  strength of  62.2  kV/cm  with a  current density
of  100 nA/cm2.   In  contrast, the parallel plate data were obtained
with  an  applied field of 16.6 kV/cm at a current density of 2 nA/cm
and the  resistivity  obtained under these conditions  was  8.3x1012
ohm-cm.   The  resistivity value derived from the voltage-current
curves is expected to be lower than the parallel plate  data under
these conditions as  a result of electrical  breakdown (back corona)
in  the deposited dust layer.
                                 19
2

-------
     Table 3.  In situ Resistivity from George Neal Plant, Unit 2
 Baseline Test Series (3/27/76)
                   Resistivity
Temperature °C(°F)   ohm-cm
    110(230)

    118(244)

    118(244)

    121(250)
8.3 x 1012

5.7 x 1012

5.9 x 1012

6.8 x 1012
                  S03 Injection Test Series
               Temperature         Resistivity
                  °C(°F)     Date     ohm-cm   '
127(261)  5/17/76  4.4 x 1010

132(270)  5/19/76  3.1 x 10l°

138(280)  5/19/76  l.OxlO11

142(288)  5/19/76  4.1 x 1010

143(289)  5/20/76  3.5 x 1010

143(289)  5/20/76  4.1 x 10x°
                               20

-------
                         I   '    I   '    I
                         _ (5600X5.0) =C23t1011
Figure 8.  Resistivity Probe Voltage-Current Characteristics
           without SO3 Injection
                            21

-------
      Figure  9  shows  the  resistivity probe  voltage-current  relation-
 ships with SO3  injection.   Note  that  the resistivity derived  from
 the  voltage-current  curve  at  100 nA/cm2 is higher than  the parallel
 plate data because,  with the  relatively low dust resistivity, elec-
 trical breakdown  is  not  occurring in  the deposited dust layer at
 this  current density.  In  general, the parallel plate data are con-
 sidered more reliable than that  derived from the voltage-current
 curves.
 D.  Voltage-Current  Characteristics of the Precipitator
      Figure 10  illustrates the arrangement of the transformer-rect-
 ifier sets on the precipitator.   The  power supplies are not equipped
 with  secondary  voltage meters, and therefore voltage divider resis-
 tors  were attached to selected TR sets for the purpose of obtaining
 secondary voltage readings.   Figures  11 through 14 present the
 secondary voltage-current  relationships for the indicated TR sets
 obtained during the  baseline  test on March 27.  These curves in-
 dicate that back corona  and/or severe sparking occur at low values
 of current density, which  is  indicative of high dust resistivity.
 Note  that the automatic  operating point location is such that much
 of the power input is not  useful power for the precipitation process,
 Figures 15 and 16 show the secondary voltage-current relationships
 for TR sets 3 and 8 with S03  injection on May 21.  The shape of
 these  curves, in contrast  to  Figures 11, 12, 13, and 14, indicates
 that  dust resistivity is not  limiting the electrical operating condi-
 tions.  This conclusion  is consistent with the in situ resistivity
measurements.  However,   as stated previously, TR sets were tripping
our during this test series due to dust removal problems.   Average
electrical readings from the panel meters for March 27 and for May
19 are given in Tables 4 and  5, respectively.
                                22

-------
        SO
        Q_
          0.5
                1   I    '    I   '    T"7
                      >SPARK=4.1x1010
                      1400 (5)
                   (0.5x10-6)(0.1)


                 = 1.4x 10^ ohm-cm
                           10      12

                                  kV
                                               CLEAN
                                          DIRTY
                                      .    I    .   I   .
14
16      18
Figure  9.  Resistivity Probe Voltage-Current Characteristics
            with  SO3 Injection
                            23

-------
                            t  Gas Flow
                                CTD
CTD
                                    r<
Figure  10.  Arrangement of Transformer Rectifier Sets  for
           George Neal Unit 2
                           24

-------
0.6
0.5


0.4

| 0.3
0.2

0.1

0
I
O
- OA -
AVERAGE OPERATING^
POINT o
	 0 —
0

	 O —
o
o
	 o —
o
la I ' !
15 20 25 30 35 40
ou
13.4


10.8 ™
o
<
H
8.1 1
Ul
Q
en
i»
CURRENT

2.7


                               kV
Figure 11.  V-I Characteristics for TR Set 3 on March 27, 1976
                             25

-------
         0.4
         0.3
      CO
      &
         0.2
         0.1
       ~~i	r~

       AVERAGE OPERATING
       POINT
                                  _O_
15
                    20
25
                           30
                                  kV
                   J	L
                                                             10.8
                                                             8.1
                                                             5.4
                                                             2.7
                                                                 E
                                                                 u

                                    Z
                                    Ul
                                    cc
                                    cc
                                    D
                                    U
                                               35
                             40
Figure  12.   V-I Characteristics for TR  Set 4 on March 27, 1976
                                26

-------
0.4


0.3





1 0.2
^





0.1
ft

AVERAGE OPERATING 	 *-£
POINT
	 O —


O


— O 	


o



	 o —
o
I



24.1 N
E
o
c
>."
t
16.0 |
UJ
Q
I-
Z
UJ
CC
cc
8.1 3

15 20 25 30 35 40
                                  kV
Figure 13.  V-I Characteristics for TR Set 7 on March 27, 1976
                             27

-------
        to
        Q.
U.O

0.4

0.3

0.2
0.1
0
1
I I I I
AVERAGE OPERATING 	 ».* o
POINT U
— o —
O
— 0 —
0
— 0 —
o
— 0 —
I c I I I
40.2

32.2
M
O
24.1 1
1— .
P~
Z
UJ
Q
o>
b
CURREN1
8.1

5 20 25 30 35 40
                                kV
Figure 14.  V-I Characteristics for TR  Set  8  on March 27,  1976
                              28

-------
   co
   a.
1.4
1.3
1.2
1.1
1.0
0.9
0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.
	 r- , . ,
_ CURRENT LIMIT 	 *••-
	 • —
	 • • —
^^•M
AVERAGE OPERATING 	 »-£ —
POINT FOR 5/19/76
_ —
— —
• A ^^^~


— •
— • *
I " '
0 " 20 30 40
kV
/.o

32.2

26.8

21.4

16.1

10.7


2.68
50
                                                             CM




                                                              I
V)

HI
o
I-

UJ
cc.
a.

u
Figure 15.   V-I Characteristics for TR Set  3  on May 21, 1976
                                29

-------
     Q.




     <
I.O
1.2

1.1
1.0
0.9
0.8
0.7

0.6

0.5
0.4
0.3
0.2
0.1
11
i • i • i •— r-
CURRENT LIMIT
AVERAGE OPERATING-^ • —
POINT FOR 5/19/76 ^^*^
~"~ • • — —
— , 	
_ _
-
0 ^HIBH



^^•M* _ A
-
-
-
I - I
104.5

88.4


CM
O
64.3 <
I—
V)
LU
48.2 Q
z
111
DC
QC
D
U
32.2


8.0

> 20 30 40 50
kV
Figure 16.  V-I Characteristics for TR Set 8 on May 21, 1976
                              30

-------
TRtt1
  7
  8
  4
  3
                  Table 4.  George Neal - Unit 2
            Average voltages and currents for 3/27/76
Primary amps  Primary volts  Secondary amps
     76
     93
     80
    105
    213
    230
    205
    220
    0.36
    0.45
    0.34
    0.5
 Current
 Density
 nA/cm2
   29.0
   36.2
    9.2
   13.4
  1
  2

  5
  6
     40
  30 to 40

    140
    145

    110
    170
150 to 200

    280
    275

    225
    0.07
0.06 to 0.14

    0.8
    0.82

    0.43
    1.8
 ( sparking,
  meters
  swinging)
    64.3
    65.9
no sparking
    34.6
  sparking
1  TRs 1, 2, 3, and 4 each have 40,176 ft2 collecting surface.
   TRs 5, 6, 7, and 8 each have 13, 392 ft2 collecting surface,
   for 214,272 ft2 total.
2. Average readings during sparking.
                                31

-------
         Table  5.  Average  voltages  and currents  for  5/17/76




                                                            Current
TR No.

71
8
4
3
1
2
5
6
Primary Amps
86.1
191
199
164
137
220
195
193
Primary volts
215
346
295
328
306
312
353
349
Secondary
.474
1.156
1.137
.917
.728
1.397
1.234
1.248
"diO4_-£
amps nA/cm2
38.1
92.9
30.5
24.6
19.5
37.4
99.2
100.0
1.   Declined from 1.18 amps to 0.15 amps at end of day.
                                32

-------
E.  Chemical Analyses
1.  Coal
     Ultimate analyses of four coal samples (one collected during
the baseline test and three during the conditioning tests) are
given for the "as received" condition in Table 6.  The data show
a reasonable degree of uniformity, as desired.  The aspect of the
coal composition that is of primary interest is the sulfur concen-
tration, which is around 0.6% by weight.
2.  Flue gases
     The vapors of S02 and H2SOi» were determined with a sampling
train in which the H2SOif was first condensed around 70°C  (160°F)
and the S02 was absorbed in a bubbler filled with aqueous H202.
Each sample was titrated as dilute HaSOi* with Ba(ClO^)2 and Thorin
as the endpoint indicator.2  The concentration of H20 vapor was
determined by condensing part as the liquid and absorbing the re-
mainder with silica gel.  Concentrations of C02 and 02 were deter-
mined by Orsat analysis.
     Theoretical concentrations of C02, HaO, Oa/ and S02 were com-
puted by using the coal analysis in Table 6 and assuming the com-
bustion air contained 2% of H20 vapor.  The percentage of excess
air was not known; hence, predicted concentrations of the flue gases
were displayed in a graph as functions of excess air to permit a
comparison with the experimental results.
     Table 7 gives the results of the experimental determinations,
and Figure 17 compares these results  (except for H2S(K) with the
computed curves for varying percentages of excess air.  The data
in the table indicate that during the conditioning tests the con-
centrations averaged 11.9% C02, 7.2% H20, 5.6% 02, and 431 ppm S02.
No reliable data were obtained for the first three of these gases
during the baseline test; however, the somewhat higher result for
SO2 during the baseline test indicates that a lower excess air
level was used during this test.  The data for H2S04 were higher
                                 33

-------
             Table 6.  Ultimate Analyses of Coal Samples


Moisture1
Carbon
Hydrogen2
Nitrogen
Sulfur
Ash
Oxygen2
Btu/lb
Baseline Test
3/27
6.86
60.83
4.88
1.26
0.66
10.45
15.06
10,949
                                      Conditioning Tests
                               5/19N


                                6.28


                               62.24


                                5.56


                                0.65


                                0.57


                               10.66


                               14.05


                              11,047
5/19PM


  5.91


 59.72


  4.60


  0.88


  0.61


 13.84


 14.44


10,579
 5/21N   Average


  5.89     6.03


 60.89    60.96


  4.37


  1.26
  0.57


 11.52


 15.50
 4.84


 0.93


 0.57


12.00


14.67
11,008   10,878
Determined by air drying.
n

 Elements assumed  to be present  as  chemically-bound  water  (all  of

 the oxygen and an equivalent  amount  of  the  hydrogen -  less  than
 the total of hydrogen,  of  course).
                                 34

-------
                  Table 7.   Analyses of Flue Gas


                      Baseline
                        Test     	Conditioning Tests	

Sampling Conditions

    Date                3/27      5/19   5/19   5/20   5/20    5/21   5/21

    Location           Inlet     Inlet  Outlet Inlet  Outlet Inlet  Outlet

    Temperature, °F     250       265    250    285    250    285    250

                 °C     121       129    121    141    121    141    121

Flue-gas Concentration

    C02, %              	       11.7   11.6   11.2   11.0    12.9   12.9

    02, %               	        6.0    6.0    6.3    6.2     4.6    4.5

    H20, %              	        6.6    7.6    6.7    8.1     7.1    7.3

    S02, ppm            521       473    419    446    391    428    	

    H2SO^r ppm          0.4        1.2    0.9   10.6    0.6     8.0   	
                                 35

-------
cc
o
8"
LL
O
3?
IU
5
D
O
    16
    12
    10
                             C02
                                            (C02)
H20
          (H20)
                                                            1800
                                                            1600
                                                            1400
                                                            1200
                                                            1000
                              oo
                            800
                                                            600
                                                           400
                                                           200
                           EXCESS AIR,%
 Figure  17.   Comparison of Predicted Gas Concentrations
              (Functions of Excess Air)  with Observed
              Concentrations  (Displayed  by Dashed
              Horizontal Lines)
                            36

-------
during conditioning as expected;  no average of these data is mean-
ingful, however, because of the variation in the sampling temperature
(a point later discussed in greater detail).
     The comparison of observed and predicted concentrations in
Figure 17 shows the experimental results lying on the predicted
curves at excess air levels as follows: 02, 40% excess air; H2O,
>50% excess; C02, 42% excess; and S02, 38% excess.  These comparisons
lead to two observations:   (1) the experimental concentrations of
C02, 02, and S02 are consistent with the same excess air level
(about 40%) but  (2) the concentration of H20 indicates a consider-
ably higher air level and is thus probably lower than the true
value  (the estimated true concentration of H20 is about 8.5%) .
3.  Fly ash
     a.  Overall oxide composition
     Samples of fly ash were collected from selected hopper loca-
tions  under the precipitator to be analyzed for overall composition
as expressed by oxide concentrations.  The configuration of the hop-
per system is  shown in Figure 18.  The hoppers used in sampling
during the baseline test were Nos. 16  (inlet  row) and 8  (outlet row);
those  used in  the  conditioning tests were  Nos.  17  (inlet)  and 9
 (outlet).  All of  the samples were thus  taken from  hoppers  adjacent
to  the midline of  the precipitator.
     For each  inlet and  outlet  sample  taken at a  given time,  a
composite  was  prepared  to  represent  the  appropriate amounts  from
each source.   The  ratio  of inlet sample  to outlet sample  in the
composite  was  3.6:1.0  for  the baseline test or 10.0:1.0  for the
conditioning  tests.
     The appropriate  ratios were computed by  assuming that for each
test mode  (with conditioning or without)  the  effective migration
velocity w in the  Deutsch  equation was constant through  the precip-
itator from inlet  to outlet.  In view of the  fact that the electrode
area  over  the inlet hoppers is one-half of the total, equations in-
volving the total  precipitation efficiency Et and the inlet
                                 37

-------
                        GAS OUT

5
13
6
14
7
15
8
16

9
17
10
18
11
19
12
20
                        GAS IN
Figure 18.  Hopper Configuration  for  the  Precipitator
                        38

-------
precipitation efficiency E.  can be written in terms of the respec-
tive electrode areas A  and A.  as follows:
                     ln(l - E )  = -Atw/V
                     ln(l - E±)  = -A..W/V
                                = -0.5 Atw/V

Therefore,
= 0.5 ln(l - Et)
                         Ei =  (1 - Et) °'5
                         E± =  1 -  (1 - Et)°-5
The fractions of ash received by the inlet and outlet hoppers, res
pectively, are E± and  (Efc - EI) .  Hence, the ratio of masses is
given by
                 Inlet mass _   Ei  _  1 -  (1 - Et)
                Outlet mass ~ Et-E±   Efc-l +  (l-Et) ° • 5

With Et taken as 0.924 for the baseline test, the  computed mass
ratio  is  3.6.  Similarly, with Efc taken as  0.990 for the condi-
tioning tests, the  result is 10.0.
     A portion of each composite sample was ignited to  determine
the weight  loss during ignition and then  it was divided into  three
final  fractions that  were separately  dissolved  in  (a)  a mixture of
HF and H2SO,,  (b) fused  NaOH,  and  (c)  fused Na2C03.  The fraction
dissolved by acid was analyzed for Li,  Na,  K, Mg,  Ca, Fe,  and Ti
by atomic absorption  spectroscopy  and for P by  a  colorimetric pro-
cedure.   The fraction dissolved in  fused NaOH was  analyzed color-
imetrically for Al  and Si,  and the  fraction dissolved in fused car-
bonate was  used  for turbidimetric  determination of S as SO 3.
      The  results  of the analyses expressed as oxide weight per-
 centages  are given in Table 8.  These data indicate that the major
 difference   (on a relative basis)  in the samples from the baseline
 and conditioning tests was in % S03;  the difference was a gain of
 about 0.67% as the result of S03 injection during  the conditioning
 tests.
                                 39

-------
         Table 8.  Analyses of Hopper Ash
Weight %, Baseline Test
Weight %, Conditioning Tests
Component
Li20
Na2O
K20
MgO
CaO
Fe203
A1203
SiO2
Ti02
PiOs
S03
LOI
3/27AM
0.
0.
1.
2.
13.
6.
17.
53.
1.
0.
0.
0.
01
39
9
6
6
7
9
0
3
2
78
39
3/27AM
0.01
0.34
1.9
3.0
15.0
6.5
19.6
48.7
1.0
1.1
0.75
0.18
3/27PM
0.01
0.34
2.0
2.3
14.4
6.4
19.5
51.9
0.9
0.9
0.75
0.21
Avg.
0.01
0.36
1. 9
2.7
14. 3
6.5
19.0
51.1
1.1
0.7
0.76
0.33
5/19AM
0.
0.
1.
2.
15.
5.
17.
50.
0.
0.
1.
0.
01
45
9
9
0
7
9
3
9
7
38
51
5/19PM
0.01
0.45
2.0
2.9
13.1
5.9
17.9
51.7
0.9
0.7
1.66
0.58
5/20
0.01
0.39
1.8
2.4
13.2
5.9
17.2
53.0
0.8
0.6
1.26
0.50
5/20
0.01
0.46
1.7
3.0
14.6
6.0
18. 3
53.4
1.1
0.7
1.42
0.44
Avg.
0.01
0.44
1.9
2.8
14.0
5.9
17.8
52.1
0.9
0.7
1.43
0.51

-------
     b.  pH and soluble sulfate concentration
     Determinations of the pH values of fly-ash slurries in dis-
tilled water and the concentrations of SO.*"2 dissolved in the
slurries were made for ash samples from several sources:  (1) pre-
cipitator hoppers, (2) cyclones used for sampling from the flue-gas
ducts, and  (3) filters used for sampling from the stack.  For the
determination of pH and soluble SOi*"2 values, 0.1 g of ash was
mixed with 30 ml of distilled water and stirred until the pH
reached a stable value.  This pH value was then recorded; the
liquid phase was separated from the suspended solids and analyzed
for S04~2
      (1) Hopper samples.  The data for hopper samples are given
in Table 9.  The pH values listed are in the highly alkaline
range; all are above pH 11 and show no significant variation with
hopper source or with sampling conditions  (with or with S03 in-
jection) .  Within the first minute or so after addition of fly
ash to water, however, the samples taken during S03 injection
showed evidence of free H2SO.t on the ash surfaces.  Minima in the
range pH 4-5 occurred with the conditioned samples, but such pro-
nounced minima with unconditioned samples were not usually observed.
The eventual rise in pH to values above 11 is attributed to the
excess of  soluble base toward the interior of the ash particles.
      The data for SCK"2 in ash samples taken across the inlet to
the precipitator are plotted in Figure 19.  Across the bottom of
the horizontal axis, hopper numbers  are shown to identify the
locations  within the precipitator where the samples originated;
across  the top, temperatures measured  in  the inlet duct upstream
from  the hoppers are  given to show  the temperature gradient result-
ing from the  Ljungstrom air preheater.  The data for  two complete
sets  of  hopper  samples  taken  during S03 injection  are plotted  and
connected  by  line  segments; averages of results  for  individual
hopper samples  taken  with and without injection  are  also plotted.

                                 41

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                 Table 9.  pH Values and  Soluble SO.,'2  Concentrations1 of Hopper Ash






                       	Baseline Test	  	Conditioning Tests	



      Hopper No.         3/27 AM       3/27  PM      5/19 N       5/19 PM      5/20        5/21




    Inlet    Outlet     pjl   SO.."2   pj_   SO.T2    pJJ  SOi."2   PJL   SO.."2   pj^   SO.."2  pH   SOt
 to
     13                                                                     11.7   0.7
     14                                                                     11.5   1.6
     15                                                                     11.5   1.3
                                                                                       11.3   2.0
                                                                                       11.3   1.6
               7                                                                       11.4   1.7



    16                11.6   0.7   11.5    0.3                              11.7   0.7



               8      11.7   0.5   11.7    0.5                                          11.4   1.4




    17                                          11.6    1.1   11.5   1.2   11.7   0.4



               9                                11.6    1.3   11.5   1.3               11.5   i.o



    18                                                                     11.6   1.3




              10                                                                       11.6   0.7



    19                                                                     11.6   1.1




              H                                                                       11.6   0.7



    20                                                                     11.6   0.7




              12                                                                        11.6   0.7
1Weight percentage

-------
     3?
     N
     it
     O
     GO
     UJ
     _J
     CQ
     O
     CO
                        GAS TEMPERATURE
        °C  138
        °F  281
         139
         283
136
276
129
265
123
254
121
249
118
244
116
241
        2.0
        1.6
1.:
0.8
         0.4
                                            a
                                            o
                                            A
                                      3/27
                                      5/19
                                      5/20
                                      5/21
              13
           14
                          15
       16     17
     HOPPER NUMBER
                                            18
                                                 19
Figure 19.   Soluble SOiT2 in Hopper Ash  as a Function of
              Hopper Location  or Gas  Temperature
                           43

-------
      The variation in SO,  2 across the precipitator inlet shows an
 essentially continuous, downward trend with decreasing gas tempera-
 ture during SO3 injection on May 21, but show no consistent trend
 during injection on May 20.  A possible explanation of either vari-
 ation is a lack of uniformity in the rate of flow of S03 into the
 inlet gas duct.  Another possible explanation for the more or less
 regular trend on May 21 is the effect of temperature.  However, the
 observed direction of the trend (simultaneous decreases in both SO^-2
 and temperature)  is opposite to that expected from previous data in
 another study of S03  conditioning3  or expected from the observed H2so
 concentrations in the gas  phase at  different temperatures (Table 7).
      (2)  Cyclone samples.   Locations in the gas ducts where the
 series cyclones were  used for  sampling fly ash during conditioning
 tests are indicated in Figure  20.   The numbers circled in this
 diagram are subsequently used  to identify the different samples.
 It may be seen from the  diagram that two  samples were taken upstream
 from the  line  of  S03  injection  nozzles on opposite  sides  of the
 duct at estimated  temperatures  of 138°C (280°F)  and 115°C (240°F),
 another three  samples  were  taken between  the nozzles  and  the pre-
 cipitator  (again at different temperature extremes),  and  a  final
 set of  three  samples were taken at  one  location  in  the  outlet  duct
 near the  stack.
      The  results of determinations  of  pH  and soluble  SO.T2  are
 given in Table  10.  Data are given  for  each  size fraction and  for
 weighted  composites of the  inlet samples,  but only  for composites
 of the  outlet  samples  (which were of such limited quantity to pre-
 vent study of each fraction).
      The pH data, in general, show  increasing acidity with decreas-
 ing  particle size or with increasing available S03 as the result of
 injection.  The SO.,'2 data show the same effects.
     The only location in the flue-gas train where cyclone samples
were collected during the baseline test was at the outlet of the
precipitator.   A composite of different size ranges of this sample
gave these results:  pH = 10.8;  % SO^-2 = 2.6.
                                44

-------
                   PRECIPITATOR
                         t
                     GAS FLOW
                S03 INJECTION NOZZLES
                2345678
                    PORT NUMBER
Figure  20.   Locations  for Sampling with Series  Cyclones
                          45

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             Table 10.  pH Values and Soluble Sulfate
             Concentrations of Cyclone Samples of Ash
 Sample
  3a
  3b
  5a

  5b

  5c
   Source

Inlet before
 injection
            Inlet before
             injection
Inlet after
 injection
Inlet after
 injection
            Inlet after
             injection
Outlet

Outlet

Outlet
  Relative       Size
Temperature1 Fraction2
                                                              Soluble
pH
High



Low



High



High



Low






C
M
F
Comp.
C
M
F
Comp.
C
M
F
Comp.
C
M
F
Comp.
C
M
F
Comp.
Comp.
Comp.
Comp.
11.2
9.8
8.7

11.2
9.6
8.7

11.1
11.1
10.9

11.3
9.5
6.7

11.1
11.2
10.8

7.8
8.2
8.7
0.27
0.92
1.5
0.30
0.34
0.84
1.6
0.37
1.2
2.0
3.7
1.6
0.82
3.4
6.6
1.1
1.2
1.4
2.8
T74
6.4
6.3
7.6
'High temperature, ca 138°C (280°F), Low Temperature, ca 115°C  (240°F)

2C, M, and F correspond to DBO values of 2.2, 0.8, and 0.5
 um, respectively.  Comp. indicates a composite of all size
 ranges.
                                46

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     (3)  Filter samples.   Samples of the fly ash collected on the
filters that were used at the precipitator outlet (in the stack)
during the efficiency tests were analyzed.  These samples were from
both the ASME and EPA sampling trains.  The results are given in
Table 11.
4.  Gases absorbed in the EPA mass-sampling train
     Analyses were conducted to determine whether nonvolatile
material was collected in the impingers of the EPA mass-sampling
train at the outlet of the precipitator.  Weights of solid material
in the first impinger catches were taken into account in calculating
the mass concentrations.   These weights were determined by drying
aliquots of the material caught by use of a temperature high enough
to evaporate water rapidly.  However, a less vigorous drying pro-
cedure could leave a residue of absorbed gases-specifically includ-
ing H2SCU absorbed from the filtered  flue gas or H2SCH produced by
absorption of S02 from the flue gas and oxidation of the S02 in
the absorption medium.
     In  view of this possibility, we  performed  analyses  for absorbed
gases in aliquots of the first  impinger catches and in composites
of the second and third impinger  catches.  One  analytical method
employed with a few  samples was to  titrate absorbed acid with NaOH;
the results indicate that  comparable  amounts of two acids were
present:  HzSOi, and  H2SO3  (sulfurous  acid, or absorbed but un-
oxidized S02).  Reasoning  that  the  H2SO3  would  be  lost during any
drying procedure, we then  removed the H2S03  and determined the
remaining quantity of  SO,'2  (not  only the H2SCH evidently present
but also any  SCK"2 leached from solid material) .
     The results  of  the  SOiT2  determinations indicated that  vir-
tually  equal  quantities  appeared in the first impinger catch  and
in  the  composite  of  the  second and  third impinger  catches.   The
total  amount  of  SO,'2  found was equivalent to about 5  ppm of HzSO*
vapor,  which  could  give  a  particulate concentration of about
 .02  gm/m3  (0.01 gr/CF) *  as H2SOi, mist in the plume.  As such, the

* Concentration at 21°C and  1  atm.
                                47

-------
           Table 11.  pH Values and Soluble SO,, 2
           Concentrations of Filter Samples of Ash
Test
2-1
2-2
2-3
2-4
Sampling
Train
AS ME
EPA
AS ME
EPA
AS ME
EPA
AS ME
EPA
pj
10.
10.
9.
9.
10.
9.
[
4
4
9
6
5
_ i
5
_ i
Soluble
5.1
4.9
5.6
3.4
4.2
	 i
6.2
	 i
aFilter sample not available for analyses.
                            48

-------
SOi*"2 found would be significant.  However, the finding of S0i*~2
concentrations in the second and third impingers that were nearly
equivalent to those in the first impinger suggests that much of
the SO.*"2 found was from absorbed and oxidized S02 , and not from
H2SCU vapor.  As S02 in the flue gas, the material found would not
be logically included in the particulate emission.
                                 49

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                 IV.   MASS BALANCE CONSIDERATIONS

 A.   Sulfur Excluding Injected SOa  (Conditioning Test)
      It is possible  to use the analytical data given in Section III.E
 to  compare the rate  of combustion  of sulfur in the coal with the rates
 of  production of sulfur compounds  in the flue gas and in the fly ash.
 We  made this comparison by using the data from the conditioning tests
 with carbon as a basis for comparison.   In other words,  we assumed
 that all of the carbon in the coal appeared as C02 in the flue gas
 and then compared the mole ratio to sulfur to carbon in the fuel
 against the mole ratio in the combination of flue gas and fly ash.
      For the fuel, the average weight ratio of sulfur to carbon is
 0.57/60.96 (Table 6),  which corresponds  to a mole ratio of:
                        0.57/32.07  _ 3 c    ln-3
                       60.96/12.01  ~        U
      For the flue gas,  the average concentrations of SOa and COa
 are approximately 430  ppm and 12%  by volume, respectively (Table 7) .
 The concentration of SOa  in the gas phase prior to injection of this
 compound is negligible  (less than  1 ppm).   However,  the concentration
 of  SO 3  in the fly ash  is  not small enough to be ignored.  If the
 weight  percentage of S03  in the ash prior to treatment with this gas
 from the conditioning  system is taken as 0.76% (Table 8) and the fly
 ash concentration entering the precipitator is computed on an abso-
 lute basis (that is,  for  moist flue gas)  as 9.00  mg/m3,* then the
 SO3 in  the ash corresponds to a gas-phase composition of:

              0.0076  x  9.00 gm/m3   n oc    .rt_3   . .  3
              - 80         *    = 0.85  x 10   mol/m3
This concentration is  added  to  the  concentration of  SO^,  which is

              430 x 10"6 m3/m3   _  ,_      ,  -3
             24.1 x 10-3         ~  17<8 X  10
* This concentration represents the average of several inlet
  determinations, expressed for a temperature of 21°C at a
  pressure of 1 atm with water vapor present.
                                50

-------
The concentration of COz is:
                      0.12 mVm3      = 5 0 mol/m
                                        b-U mol/m
                   24.1 x 10-3 m'/mol

Thus, the mole ratio of sulfur to carbon in the combination of
flue gas and fly ash is given by:

                   (17.8 + 0.85) x 10"3 _ o -7 v irr3
                  - 57o—          3'7 x 1U
     Three conclusions are now evident.  First, the sulfur/carbon
ratio in the combustion products  (3.7 x 10" 3) agrees remarkably
well with the ratio in the fuel  (3.5 x 10~3).  Second, there is
evidently little of the sulfur in the fuel that is discharged from
the boiler as bottom ash.  Third, if it is assumed that all of the
sulfur in the fuel is initially oxidized to S02 but that subsequent
partial oxidation of S02 to S03 occurs in the flue-gas train as
the temperature is lowered, then  the conversion factor of  S02 to
SO 3 is best represented by the concentration of S03 in the fly ash
 (not in the flue gas).  The computed conversion factor is:

             _ °-85 x 1?"3  1n-TX 100 = 4.4%
              (17.8 + 0.85) x  10-3
B.   Injected SO 3:  Quantity Accounted  for at the  Inlet of  the
     Precipitator
1.   S03 present as H2SCH vapor in the  gas phase
     Data on inlet concentrations of H2SCK vapor  are  necessarily
limited to  the  results that could be obtained  at  the  only  two  sam-
pling  ports available between the injection  nozzles and  the  pre-
cipitator.  The data  (given previously in  Table  7) were  for  dif-
ferent temperatures,  around 130°C (265°F)  toward  one  side  of the
duct and  around 143 °C  (290°F) on the other side.   They  show  higher
concentrations  of  H2SCH  at the higher gas  temperature,  as  expected.
     To obtain  a  reasonable  approximation of the  average H2SCU con-
 centration  at  the  precipitator inlet,  the following approach was

                                  51

-------
 taken:  First, Figure 21 was prepared to compare the H2SOi, concen-
 trations found at different sampling temperatures with the concen-
 trations predicted from the data of Banchero and Verhoff1*  at the
 dew point (theoretically, the maximum vapor concentrations attain-
 able) .  As expected,  the experimental results are portrayed by a
 curve  falling substantially below the dew point curve.   Next,  Figure
 22 was prepared to show average gas temperatures at different  dis-
 tances across the inlet duct (these temperatures were computed from
 the data of  Kin Associates  that were obtained in pitot traverses).
 Also plotted in Figure  22 were  H2SO» concentrations at these tem-
 peratures as obtained by interpolation of the previous  curve
 (Figure 21)  for the experimental values.   Finally,  the  average H2SCH
 concentration across  the duct was computed from the relationship
 between apparent experimental concentration and location in the
 duct.
     The  value  of  the average thus  obtained is  1.8  ppm.  It repre-
 sents  the approximate increase  in the  H2SOif  vapor concentration as
 the  result of S03  injection  (the  concentration  during the  baseline
 test has  been reported  as 0.4 ppm but  is  not large  enough  to be
 clearly distinguished from zero).
 2-   SO3 present  as SCK"2  in  the  fly  ash
     Data based  on hopper samples.   Average  values  for the  total
 percentage of S03  in  fly ash  collected in hoppers adjacent  to  the
 midline of the precipitator  are  0.76% without conditioning  and
 1.43% with conditioning  (Table  8).   Using the difference of
 0.67% as  a measure of the effect  of  S03 injection and taking the
 value of  9.00 gm/m3 as representative of  the  fly-ash  concentration
 at the inlet of  the precipitator,* one calculates as  follows to
obtain the concentration of injected S03 thus accounted for:
* This concentration represents the average of several inlet
  determinations, expressed for a temperature of 21°C at a
  pressure of 1 atm with water vapor.
                                52

-------
        a
        a

        *
        O



        X*
           16
           14
           12
           10
8
             110
              230
       116
240
121
                                    TEMP °C


                                  127     132
                                     138
                              143
                                                   149
                            _L
                                   T
                              T
                     DEW POINT CURVE


                     (8.5% H20)
                              °/
                                /
                                                    /

                                                   /  EXPERIMENTAL


                                                  /   RESULTS
                                                  »o
                                                w

 250
                       260      270


                         TEMP°F
                                                  280
                                             290
                                                                 300
                           * u cr»  r-nnr-^nf-rations  at the  Dew Point
Figure 21.  Comparison of H2SOi»  Concenrratiuaa

             with Experimental  Results
                                 53

-------
    160
          320
   104
Figure 22.  Relationship between  Flue-Gas  Temperature and
            Experimental H2SO^ Concentrations
                            54

-------
              0.0067  x 9.00  gm/m3  =         1Q_3  mol/m3
                  80  gm/mol
     0.75 x 10~3  mol/m3 x 24.1  x 10~3  m3/mol =18.0  x 10'6  m3/m3

In other words, VL8 ppm or about 75% of the 25 ppm of injected S03
is accounted for.  In connection with this result, it is necessary
to point out that the composition of fly ash collected near the
middle of the precipitator may not be representative of the total
collected, particularly in view of the erratic nature of results
for soluble SO.,"2 in ash across the entire inlet of the precipi-
tator  (Figure 19).
     Data based on cyclone samples.  Results of determinations of
soluble SO,"2 in fly ash collected in cyclones during S03 injection
give another basis for calculating the fraction of the conditioning
agent  found in the fly ash.  Two composite samples taken upstream
from the injection nozzles were found to contain an average of
about  0.34% soluble SO,'2 (Table 10).  Corresponding samples  taken
between the nozzles and the precipitator contained individually
1.6, 1.1, and  1.4% soluble S04"2 or averaged  1.37%.  The difference
in the averages, 1.03%, upstream and downstream of the nozzles
corresponds to the following concentration  of injected S03:

     0.0103 x  9.00 gm/m3  x  24  L x 10-s m3/moi = 23 x  10~6  m3/m3
          96 gm/mol
The  result, 23 ppm,  is very close to  the  nominal  value  of  the in-
jected concentration.
C.   Injected  SQ3;  Quantity Accounted for in Stack  Emissions
1.   Emission  as  H2SQi»  vapor
     Concentrations  of HZSO»  found  in the outlet  duct during  con-
ditioning tests  were all less  than  1 ppm.   Such low values are to
be expected as a result of  the low gas temperature recorded at the
 sampling point 120'C  (about 250°F), if one consults the dew point
 concentrations predicted by Banchero and Verhoff (Figure 21).  It
 is therefore evident that if  S03 injection significantly increases
                                 55

-------
SOi, 2 emissions, the increase must be found in the composition
of emitted particulates.
2.  Emission of S0it~2 in particulates
     Data from cyclone samples.  The soluble SO^2 concentrations
in particulate collected in cyclones at the outlet duct during con-
ditioning tests were individually 6.4, 6.3, and 7.6% or the average
was 6.8% (Table 10).  The average value was used with outlet parti-
culate concentrations calculated from efficiency tests to compute
equivalent concentrations of S03 lost to the stack in the solid
phase as summarized in Table 12.
     The soluble S0i»~2 content of outlet ash during the baseline
test was 2.6%.  The particulate concentration at this time was about
0.63 mg/1.*  Thus,  the corresponding S03 concentration without con-
ditioning was 4.4 ppm, a value that exceeded each emission level
given in Table 12 except those for Test 2-3, which is known to have
given a faulty indication of the precipitator performance during
conditioning.  It is evident,  therefore, that the total amount of
SO3 emitted in particulates was lower with conditioning than without
as a result of the  marked reduction in the mass concentration of
particulates.
     Data from filter samples.  Computations of stack losses of
SO3 as particulate  SOi,"2 found on the filters used in the efficiency
tests gave the results summarized in Table 13.   These results con-
firm the conclusion just given:  an insignificant fraction of the
injected S03 escapes to the stack as SOi,"2 in particulates.
* This concentration is the average of two outlet determinations,
  expressed for a temperature of 21°C at a pressure of 1 atm, with
  water vapor present.
                               56

-------
                 Table 12.   Injected S03 Found
                In Outlet Cyclone Samples of Ash


                Sampling     Particulate Con-    Corresponding S03
  Test           Train1     centration2. gm/m3   Concentration, ppm

  2-1             ASME            0.092                 1.6
                  EPA             0.163                 2.8

  2-2             ASME            0.071                 1.2
                  EPA             0.098                 1.7

  2-3             ASME            0.318                 5.4
                  EPA             0.556                 9.5

  2-4             ASME            0.205                 3.5
                  EPA             0.210                 3.6
1.   Used for determination of total particulate
    concentration given in next column.

2.   At 21°C and 1 atm. with water vapor present,
                                 57

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               Table 13.  Injected SO3 Found
              In Outlet Filter Samples of Ash


            Sampling    Particulate Con-    Corresponding S03
Test         Train     centration1, gm/m3   Concentration/ ppm

2-1           ASME           0.092                  1.2
              EPA            0.163                  2.0

2-2           ASME           0-071                  1.0
              EPA            0.098                  0.8

2-3           ASME           0.318                  3.3
              EPA            0.556                  	2

2-4           ASME           0.205                  3.3
              EPA            0.210                  	z
1.  At 21°C and 1 atiru with H20 present.

2.  Filter sample not available for analysis.
                              58

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     V.  COMPUTER MODEL PROJECTIONS OF PRECIPITATOR PERFORMANCE

     The SRI-EPA mathematical model6 was used to analyze the perform-
ance of the precipitator during the test program and to estimate
the plate area required for 99% collection efficiency without the
aid of conditioning agent.  In order to use the model to simulate
the precipitator operation with high dust resistivity, it is neces-
sary to estimate a "useful" input power from the voltage-current
relationships.  This is required because the model is based on the
assumption that the input values of current and voltage represent
a unipolar particle charging process in which all of the charge
transported to the collecting electrode from the corona wires is
carried by either corona current or the charged dust particles.
The average conditions used were estimated from the voltage-current
relationships obtained on March 27.  The averages of the values
selected for the TR sets are:  35kV applied voltage, 3.5 nA/cm2
current density.  Figure 23 presents results from the computer pro-
gram in terms of overall collection efficiency as a function of
specific collecting area.  The theoretical performance  is clearly
much greater than the measured performance obtained by  Research
Cottrell on March 27.  However, if  the overall collection efficiency
is reduced by empirical relationships which are intended to esti-
mate the effects of gas sneakage, particle reentrainment, and  non-
uniform gas velocity distribution,  fair agreement can  be obtained
by assuming a gas velocity distribution with a normalized standard
deviation of 25%, and by  further assuming  that reentrainment and
gas sneakage losses amount to  20%  of  the mass collected in  each
stage  over three effective stages.  The computer projection based
on these assumptions is labeled curve 2 on Figure  23.   These assump-
tions  indicate  that a specific collecting  area of  78.8 m2/(m3/sec)
 (400 ftVlOOO ACFM) would result in 99.0%  overall  collection effic-
iency.  However, this projection does not  contain  a safety  factor
for TR set failures, nor  does  it consider  the  possibility  that the
                                 59

-------
         s?



         u


         LU

         o

         il
         o
         HI
         o
         u
              99.9 —
Figure 23.
                          FROM RESEARCH COTTRELL TEST OF 3/27
                                                            700  ft2/1000ACFM

                                                            138  m2/(m3/sec)
Pr°jections  of Collection-Efficiency
                                   60

-------
assumed electrical operating conditions may be degraded if dust
resistivity increases.  The latter consideration constitutes a
major uncertainty since the electrical operating characteristics
of the precipitator will be critically influenced by dust resis-
tivity changes.
     In an effort to obtain an estimate of specific collecting
area which includes a safety margin, the following procedure was
employed to obtain curve 3 on Figure 23:  (1)  The model was used
to calculate the overall efficiency if the SCA were effectively
reduced from 78.8 to 59.0 m2/(m3/sec)   (400 to 350 ft2/1000 ACFM) in
1/2 of the precipitator.   (2) The model was used to calculate over-
all efficiency if the SCA were reduced from 118 to 88 m2/(m3/sec)
(600 to 450 ft2/1000 ACFM) in 1/2 of the precipitator.   (3) The
results from (1) were plotted at 78.8 m2/(m3/sec)  {400 ft2/1000 ACFM),
and the results from  (2) were plotted at 118 m2/(ra3/sec)  (600 ft2/1000
ACFM).  This procedure results in an estimated requirement of 108
m2/(m3/sec), or 550 ft2/1000 ACFM, to achieve 99% collection effi-
ciency with a safety margin for transformer-rectifier failures as
specified above.
     Figure 24 gives the theoretical model projections and the
reduced projections (using the same parameters for gas velocity
distribution and reentrainment and sneakage as were used  in Figure
23) with the average electrical operating conditions achieved with
S03 conditioning.  These results indicate that, with the  measured
size distribution and electrical operating parameters achieved dur-
ing the SO3 injection test,  99% collection efficiency is  theoret-
ically possible at the existing SCA.  However, as  stated  earlier,
additional testing is required to determine whether the  S03 system
will allow precipitator performance to remain at the 99%  level  for
extended periods with a boiler load of 300 MW.
                                61

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          99.99
       (J
       z
       LLJ


       O


       o
       O
       u
          99.90
           99,5
           99.0
           95.0
                ASME ON TEST 2-2
                 EPA ON TEST 2-2
a = 0.25

S = 0.2

N = 3.0
                                                      I
              100     200     300      400      500      600   ft2/1000 ACFM
              19.7     39.4     59.1      78.7     98.4     118   m2/(m3/sec)



Figure  24.  Computer Model  Projections of  Collection-Efficiency

              with SO3
                                  62

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                        ACKNOWLEDGEMENTS

     Appreciation is expressed to Research Cottrell and Kin
Associates, for assistance in obtaining mass loading measurements,
and to Iowa Public Service Company for financial and technical
assistance.  Mr. G. H. Marchant, Jr., supervised the Institute
personnel in the field, who consisted of several members of the
Physics Section and the Physical Chemistry Section.
                                Submitted by:
                                Edward B. Dismukes,
                                Senior Research Advisor
                                John P.  Gooch,  Head
                                Control  Device  Research Division
                                63

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                        REFERENCES
 Grady B. Nichols,  "Techniques  for  Measuring Ply Ash Heals-
 tivity", EPA-650/2-74-079, August  1974.
 J. S. Fritz and S. S. Yamamura, Anal.  Chem.  27,  9
 (1955).                             "
 E. B. Dismukes, "Conditioning of Fly Ash with Sulfur
 Trioxide and Ammonia", EPA-600/2-75-015, August  1975.
J. T. Banchero and F. H. Verhoff, J. Inst. Fuel  48, 76
 (1975).
                         64

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                                TECHNICAL REPORT DATA     .
                         (Please read Inuructivns on the reverse before completing!
1. REPORT NO.
 E PA- 600/2-
             77-242
4. TITLE AND SUBTITLE
Fly Ash Conditioning with Sulfur Trioxide
                                                       December 1977
                                                       PERFORMING ORGANIZATION CODE
7. AUTHOR(S)

Edward B. Dismukes and John P. Gooch
                                                       . PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Southern Research Institute
2000 Ninth Avenue, South
Birmingham, Alabama  35205
                                                       1AB012; ROAP 21ADL-027
                                                       11. CONTRACT/GRANT NO.

                                                       68-02-2114, Task6
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 PER
                                                       Task Final; 3-11/76
                                                       14. SPONSORING AGENCY CODE
                                                        EPA/600/13
T5. SUPPLEMENTARY NOTES IERL_RXP project officer is Leslie E. Sparks,  Mail Drop 61,  919/
541-2925.
 l.
bi
i6. ABSTRACT The report describes an evaluation of an SO3 injection system for the Georg
Neal Unit 2 boiler of the Iowa Public Service Co. in Sioux City, Iowa. Results of base
line tests without conditioning indicate a dust resistivity of 6 x 10 to the 12th power
ohm-cm at 118 C: the precipitator's average collection efficiency was 91.3% at a
specific collecting area of 42.8 sq m/(cu m/sec). Because transformer-rectifier sets
tripped out, apparently due to ash buildup in the hoppers, only one precipitator effi-
ciency test was  conducted with the SOS system operating continuously with all T-R
sets operating.  Results of this test were: (1) specific collecting area = 41.8 sq m/(cu
m/sec); (2) collection efficiencies = 99.27% (ASME method), 98.96% (EPA method),
and 98.78% (EPA method, including first impinger residue); and (3)  4x 10 to the 10th
power ohm-cm  dust resistivity at 143 C. An adequate accounting was made for the fate
of the injected SOS.
 17.
                               KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                            b.lDENTIFIERS/OPEN ENDED TERMS
                                                                     .  COSATI Field/Group
Air Pollution
|Fly Ash
Treatment
Sulfur Trioxide
Dust
Electrostatic
         itators
                          Electrical Resis-
                           tivity
                                            Air Pollution Control
                                            Stationary Sources
13B
2 IB

07B
11G
20C
  18. DISTRIBUTION STATEMENT

  Unlimited
                                            19. SECURITY CLASS
                                            Unclassified
                                            20. SECURITY CLASS (This page)
                                            Unclassified
                                                                     22. PRICE
  EPA Form 2220-1 (9-73)
                                            65

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