EPA-650/2-74-026


 March 1974
                             Environmental Protection  Technology Series
                                                                        m
                                                                        m
                                                                        m
                                                                        •m
                                                                        i*
                                                                        ii
                                                                        II
A me r i c a n Pet r oJeum;i:

1801 K SU««t>
llpilliiililiiilli;

-------
                                                       I/O
                                   EPA-650/2-74-026
INVESTIGATION OF  PARTICULATE
   EMISSIONS FROM OIL-FIRED
  RESIDENTIAL  HEATING  UNITS
                     by
       R. E. Barrett, D. W. Locklin, and S. E. Miller

            Battelle, Columbus Laboratories
                 505 King Avenue
               Columbus, Ohio 43201
           Contract No. 68-02-0230 (Task 9)
                ROAP No. 21AFE-07
             Program Element No. 1AB015
            Project Officer: Robert E. Hall

             Control Systems Laboratory
         National Environmental Research Center
       Research Triangle Park, North Carolina 27711
                  Prepared for
          AMERICAN PETROLEUM INSTITUTE
      COMMITTEE ON AIR AND WATER CONSERVATION
                1801 K STREET, NW
             WASHINGTON, D. C. 20006
                     and
        OFFICE OF RESEARCH AND DEVELOPMENT
       U.S. ENVIRONMENTAL PROTECTION AGENCY
             WASHINGTON, D. C. 20460
                  March 1974

-------
This report has been reviewed by the Environmental Protection Agency
and approved for publication.  Approval does not signify that the
contents necessarily reflect the views and policies of the Agency,
nor does mention of trade names or commercial products constitute
endorsement or recommendation for use.
                                  11

-------
                          ABSTRACT

          Two residential oil-fired heating units  (a warm-air
 furnace and a boiler) were fired  in the laboratory while
 Bacharach smoke and  filterable particulate emissions were
 measured at several  excess-air levels for both cyclic and
 steady-state runs.   In addition,  particle-size distributions
 were measured during runs on the  boiler to determine if particle-
 size variations might help explain the lack of correlation be-
 tween  smoke and particulate emissions, based on earlier field
 measurements.
          One unit was found to produce essentially no ex-
 cessive smoke or particulate on startup; smoke one minute
 after  startup was equal to steady-state smoke, and particulate
 emissions for cyclic and steady-state firing were equal.  The
 second unit produced high smoke on startup (relative to the
 steady-state smoke)  and produced  higher particulate emissions
 for cyclic runs than for steady-state runs, suggesting that
 this unit had a significant "on puff" on startup.
          It was determined that  particulate  emissions  varied
with excess air in the same pattern as smoke  number,  being
higher at low excess air levels for both units.   Correlations
between smoke and particuJate emissions  appeared  practical  for
individual units firing at specific operating conditions.   How-
ever, the data did  not suggest  that a  general correlation between
smoke and filterable particulate  emissions  exists for cyclic
operation.   For the two units examined here,  particle-size dis-
tributions indicated that  over  80  percent of  the  particles were
below 1.0 micron and that  the particle-size distributions were
nearly identical for all  runs.
                             ill

-------
                           ACKNOWLEDGMENT

         The s-jchors v ish to acknowledge the assiscancs and helpful  comments
of the EPA Project OHlcci', Kchert fi. Hal J, .ir.d the API SS-5 Task Force
during the course- of this puuj,i'dm.  Membjrship on the SS-5 Task Force
was as follows:
     E. Landau (Chairman). . .  .  Asiatic  Petroleum Corporation
     R. C. Amero	Gulf Res&irch 6. Development Company
     S. P. Cauley	Mobil t.il Corporation
     H. E. Leikkanen	Texaco Inc.
     B. L. Mickel	American Oil Company
     R. E. Pater son	Chevron Research Company
     C. W. Siegnund	Esso Research ft Engineering Company
     R. A. Seals	National Oil Fu*l Institute, Inc.
     J. R. GouJd 	  American Petroleum Institute
                                   IV

-------
                        TABLE OF CONTENTS







                                                             Page




OBJECTIVE 	       1




BACKGROUND  	       1




APPROACH	       2





     Heating Equipment Studied	       2




     Measurement Techniques and Equipment 	       3




     Particle Sizing	       3




     Conditions at Which Measurements Were Made 	       4




COMMENTS ON FILTER MEDIA	       5




RESULTS 	       6




     Data Summary	        6




     Smoke Versus Time During Cycle	        6




     Smoke Versus Excess Air	         9




     Particulate Emissions Versus Excess Ait	        10




     Particulate Loading Versus Smoke 	        11




     Particle Size	        12




CONCLUSIONS	        13




     Additional Information Koeded	        14




REFERENCES	         16

-------
                          FIGURES
No.
1   Schematic Diagram Showing Principle of the
       Cascade Impactor                                   17
2   Smoke Versus Time During Cycle -- Unit 36             18
3   Smoke Versus Time During Cycle -- Unit 37             19
4   Smoke Versus Excess Air -- Unit 36                    20
5   Smoke Versus Excess Air -- Unit 37                    21
6   Filterable Particulate Emissions Versus Excess
       Air -- Unit 36                                      22
7   Filterable Particulate Emissions Versus Excess
       Air -- Unit 37                                      23
8   Filter Catch Versus Excess Air -- Unit 36               24
9   Filter Catch Versus Excess Air -- Unit 37               25
10  Filterable Particulate Loading Versus Smoke  --
       Unit 36                                             26
11   Filterable Particulate Loading Versus Smoke  --
       Unit 37                                             27
12  Particulate Loading (Based on Filter Catch)
       Versus Smoke -- Unit 36                            28
13  Particulate Loading (Based on Filter Catch)
       Versus Smoke -- Unit 37                            29
14  Particulate Loading (Based on Filter Catch) Versus
       Smoke at 1.0 Minute for Cyclic Runs                  30
15  Filterable Particulate Loading Versus Smoke  --
       Cyclic Operation of Units 36 and 37                   31
16  Particle-Size Distribution for Unit 37 at 35  Percent
       Excess Air                                         32
17  Particle-Size Distribution for Unit 37 at 29  Percent
       Excess Air                                         33
18  Particle-Size Distribution for Unit 37 at 27  Percent
       Excess Air                                         34
19  Particle-Size Distribution for Unit 37 at 26  Percent
       Excess Air                                         35
20  Particle-Size Distribution for Unit 37 at 23  Percent
       Excess Air                                         36
                           vi

-------
                       Figures (Cont)

No.
21  Particle-Size Distribution for Unit 37 at 18 Percent
       Excess Air                                          37
22  Part iculate on Fiberglass Filter                         38
23  Clean Silver Filter (1000X)                              38
24  Clean Silver Filter (5000X)                             39
25  Parti culate on Silver Filter (20X)                        39
26  Particulate on Silver Filter QOOX)                       40
27  Particulate on Silver Filter (500X)                       40
28  Particulate on Silver Filter (1000X)                      41
29  Particulate on Silver Filter (5000X)                      41
                             vii

-------
            INVESTIGATION OF PARTICULATE EMISSIONS FROM
                OIL-FIRED RESIDENTIAL HEATING UNITS
                                 by
                 R. E. Barrett, D.  W.  Locklin, and
                            S.  E. Miller
                             OBJECTIVE

          The objective of this limited laboratory study was to investi-
gate the relationship between particulate emissions and excess air and
the relationship between particulate emissions and Barharach smoke number
from oil-fired residential heating units.
                             BACKGROUND

          Battelle-Columbus has conducted a two-year field study of
emissions from 33 oil-fired residential heating units and 13 commercial
       (1 2)*
boilers  '  . During the course of that study, gaseous emissions (CO,
hydrocarbons, SO , and NO ) were measured at many different operating
conditions.  However, due to the time and cost associated with particu-
late sampling, data were collected on particulate emissions at only a
few operating conditions.  Consequently, several questions remained un-
answered after completion of the field study.  These questions included:
          (1)  What is the relationship between particulate emissions
               and excess air?  (During the field study,  particulate
               emissions were measured at only one excess-air level
               for each burner condition.)
          (2)  Is there a relation between particulate emissions and
               Bacharach smoke number?  (The field study  data showed
               no satisfactory correlation between particulate emis-
               sions measured during cyclic operation and smoke
               measured near the end of a 10-minute "on"  time, as
               normally measured by burner servicemen.)
*  References are given on page 16.

-------
          (3)  Do particle-size variations explain the lack of
               suitable correlation between participate emissions
               and smoke reading?
          (4)  How much do transients at startup and shutdown con-
               tribute to particulate emissions?

          In an  effort  to obtain data that might answer some of  the
 above  questions,  the American  Petroleum Institute and the U.S. Environ-
 mental Protection Agency sponsored this laboratory  study to measure par-
 ticulate  emissions, smoke, and particle size while  firing two residential
 oil-fired heating units at several operating conditions.

                               APPROACH

          Battelle's approach  to this study was to  install two typical
 oil-fired heating units within the laboratory and to fire these units
 at  a range of conditions while collecting data on filterable particulate
 emissions, Bacharach smoke, and particle-size.

 Heating Equipment Studied

          The two heating units that were selected  for this study were
 intended  to  be representative of different types of oil-fired heating
 units:  a warm-air furnace and a hot-water boiler.  The furnace was
 equipped  with a  light-weight ceramic combustion chamber liner and a
 conventional gun burner, while the  boiler was  equipped with  a heavy  re-
 fractory  (firebrick) liner and a flame-retention gun burner.  The speci-
 fic units were as follows:
     Unit 36'
       Up-flow oil furnace with ceramic-felt  liner and  1.0  gph conven-
       tional high-pressure gun burner.   (This  unit was identified  as
       Unit 35 in the  Phase II studies^2^.
     Unit 37*
       Dry base,  vertical fire-tube steel  boiler with a dense cast-
       refractory combustion chamber and a 1.0  gph high-pressure,
       flame-retention-type oil burner with  3450 rpm motor.
*  Unit numbers were continued sequentially from numbers used  in the Phase I
   and II reports.   Unit 36 was given a new number as the air  damper had  been
   modified since it was run as Unit 35.

-------
The units were equipped with solenoid shut-off valves (nondelay type)

to eliminate possible variations due to pump shut-off.

          To increase the variety of equipment included in this study,

the burner was interchanged and one run was made witli the flame-retention

burner firing in the warm-air furnace.   The combination of the flame-

retention burner firing in the warm-air furnace is identified  as Unit  38.


Measurement Techniques and Equipment


          Measurement techniques and equipment used in conducting this
study were identical to those described in Reference 2 with the follow-
ing exceptions:

          (1)  NO and NOX were not measured as most of the data from
               the field study showed fairly consistent levels of
               NOX emissions from oil-fired residential heating units.

          (2)  A back-up filter was used on the EPA particulate
               sampling train to catch any material not collected
               by the first filter.  Particulate weights are based
               on the sum of the mass collected on the two filters.

          (3)  The material collected in the impingers of the EPA
               particulate sampling train was not dried and weighed,
               as the interest was in correlation with filterable
               particulate.

          (4)  For the runs on the first units examined (Units 36
               and 38), fiberglas filters wore used in the EPA
               sampling train [as specified by the EPA Method 5
               procedure^)]. However, due Lo problems associated
               with the hygroscopic nature of the fiberglas filter
               and its fragility, silver LLiters were used for
               runs on Unit 37.   (Silver filters were used for the
               Phase I and Phase II field studies.)


Particle Sizing


          Particle-size measurements were made for six runs in Unit  37
using the Battelle Cascade Impactor.  The design of the impactor is  based

on the principle of particles in a moving aerosol impacting on a slide

placed in the air stream.  The impactor classifies particles in the

-------
 range of  0.25  -  16.0 microns  into  seven categories.  If a particle is
 sufficiently large  it will  impact  on the  first stage; the smaller
 particles will continue  to  travel  around  the  slide to subsequent
 stages.   The jet diameter of  each  succeeding  stage decreases.  Thus,
 the particle will increase  in velocity for various stages until it
                                                               (4)
 obtains  sufficient  inertia  to impact as illustrated  in Figure 1

          Procedure.  Flue-gas was sampled from the  center of the stack.
 For the  sampling done for this study, a 5/8-inch-diameter sample probe
 about 20  inches  in  length (from probe tip to  impactor inlet) was used,
 It  had a  90-degree, 6-inch  radius  bend such that the probe tip pointed
 upstream.  The impactor  was operated horizontally and was heated to
 stack gas temperature (about  400 F) prior to  probe insertion in the
 stack.   Sampling at the  required 12.3 liters  per minute was initiated
 immediately on probe insertion into the stack.  Due  to the small parti-
 cle size  measured in some preliminary runs, it was decided that the
 particle  size was so low as to not require isokinetic sampling and so
 sampling  was conducted at greater  than isokinetic velocities.  (Also,
 the very  low gas velocities in the stafk  would have  required an ex-
 cessively large  nozzle to obtain isokinetic sampling.)  Sampling times
 were 30 and 60 minutes.  The  impactor slides  were covered with a disk
 of  2-mil  stainless  steel shim stock so i:hat the entire glass slide did
 not have  to be weighed.  Immediately after sampling, the impactor
 slides were removed and  returned to a constant temperature and humidity
 room to  equilibrate and  for weighing.

Conditions at Which Measurements Were Made

         Particulate emissions and  smoke were  measured  at  a  range  of
excess-air levels for  two types  of  runs:   cyclic  runs with repeated cycles
of  10-min on and  20-min  off  cycles  (the  same cycle  as used  in the  field
program)  and steady-state runs at  thermal  equilibrium.   In addition,  CO.,
0«,  CO, and  HC  were  continuously monitored for all  runs  and  particle-
size measurements were made  during  steady-state runs  on  Unit  37.

-------
 Particulate  emissions for the cyclic runs were collected during the
 firing  portion of  six cycles, giving one hour of sampling during burner
 operation.   To assure obtaining samples during startup and shutdown
 puffs,  sampling was initiated about 30 seconds before burner startup
 and was continued  until about 30 seconds after burner shutdown.  For the
 steady-state runs, sampling was begun about 30 minutes after startup
 and was continued  for about two hours.  Smoke readings were taken at the
 1-, 2-,  3-,  5-, 7-, and 9.5-minute points during the 10-minute "on"
 period  for cyclic  runs and at the 10-, 30-, 50-, 70-, and 100-minute
 points  for the steady-state runs.
          The fuel fired during this investigation was identical to
                                                        (1 2)
 the No.  2 reference fuel oil used during the field study  '  .
                       COMMENTS ON FILTER MEDIA

          The particulate emission measurements in this study were com-
plicated by the problems associated with weighing the very small quan-
tities of particulate accumulated on the filters during these experi-
ments with residential oil burners having relatively low particulate
emission levels.  For example, for most of the runs, three hours of
sampling during cyclic operation (one hour of firing time) or two hours
sampling during steady-state operation resulted in collection of less
than 10 mg of particulate; for many runs, less than five mg of particulate
was collected.  Moreover, no filter is completely satisfactory when attempt-
ing to measure these small quantities of materials as indicated by the
following:
          •  Fiberglas filters (as required by EPA Method 5)  are
             highly hygroscopic,  are somewhat fragile,  and contain
             significant impurities which make them less suitable
              for detailed chemical analyses of particulate catch.
          •  Quartz filters (compared to fiberglas)  contain lesser
             quantities of background elements but are  even more
             fragile and also are hygroscopic.
          •  Silver filters are rugged and, essentially, not  hygro-
             scopic.  However, the silver does react with sulfur
              compounds to a greater extent than fiberglas.

-------
         Fiberglas filters were chosen initially for use in conducting
the measurements for this study, primarily because of their being speci-
fied by the EPA Method 5 for sampling large sources.  However, weighings
of fiberglas filters from runs on Units 36 and 38 sometimes produced
negative values for filter catch.  These negative values were attributed
to one of two causes:  (1) the hygroscopic nature of the filter, or (2)
the loss of small pieces of filter that stick to the glass filter holder
or break off when the filter is removed at the completion of the run.
         At this point it was decided that the silver filters should be
used for runs on Unit 37, even though there was the possibility of re-
action with sulfur.  Hence, silver filters were used as the filters for
the Unit 37 runs and as back-up filters for the particle-size runs on
the same unit.

                               RESULTS

Data Summary

         Tables 1 and 2 give detailed data resulting from this investi-
gation.  Table 1 lists operational conditions and emissions.  Table 2
gives detailed smoke data.  The data presented in these tables are plotted
in Figures 2 through 15,  and their significance  is discussed below.

Smoke Versus Time During Cycle

         For the cyclic runs,  smoke readings were taken at the 1-,
3-, 5-, 7-,  and 9.5-minute points in the ]0-minute "on" period.   These
data are plotted in Figures 2  and 3 for runs in Unit 36 and 37,  respec-
tively.  For Unit 36,  the smoke readings during the first few minutes
of the cycle were usually high; that is,  this unit had  an appreciable
start-up transient.   The  CCL and CL data indicated a richer flame (com-
pared to steady state)  immediately after startup of this unit,  probably
related to nozzle characteristics.   In contrast, the 1-minute smoke

-------
                                               TABLE 1.  SUMMARY OF EMISSIONS AND EMISSION  FACTORS
Operational

Unit 36







Unit 37






Unit 38
Unit 36







Unit 37






Unit 38
Firing C02'
Cycle %
10/20(b) 9.7
11.0
12.1
12.3
12.3
12.9
13.3
13.6
10/20 11.3
11.7
11.8
11.8
12.0
12.3
12.9
10/20 12.5
steady-state 9.7
11.0
11.9
12.3
12.2
12.8
13.3
13.5
steady-state 11.3
11.8
11.9
11.8
12.0
12.3
12.9
steady-state 12.5

0.3
0.3
0.3
0.3
0.5
0.3
0.7
1.8
4.0
0.2
0.7
0.7
0.9
1.0
2.3
5.8
0.3
611
610
596
579
595
567
551
542
580
546
547
543
528
540
529
570
630
624
610
593
582
580
566
560
584
547
552
550
552
542
538
590
10.2
11.1
11.8
10.7
10.8
11. 1
17.9
37.4
25.9
24.5
23.0
25.3
28.8
26.9
65.7
17.5
8.0
8.0
10.0
12.0
12.0
10.0
11.0
11.0
18.0
27.0
20.0
20.0
22.0
27.0
52.0
11.0
HC
1.9
3.2
4.2
2.0
2.9
1.9
2.2
2.4
7.0
3.5
3.5
2.6
2.4
3.1
2.8
3.0
<1.0

0.85
0.86
0.95
1.12
1.70
1.13
3.27
4.09
0.46
0.66
0.58
1.39
0.97
1.89
2.48
0.90
0.97
0.64
0.47
0.84
0.25
0.35
0.83
1.27
0.47
1.06
0.5?
1.07
0.56
0.78
3.35
0.14
(a)   Background  levels  were measured and found to Le less than 0.25 mg/snv*.
(b)   Cycle of 10 minutes  on and  20 minutes off.
(c)   Data at 7 minutes.
(d)  Negative value obtained, considered as zero when determining total filterable partlculate.
(e)  Filter catch only.
(f)  Filter catch plus probe wash (reported aa "filterable" partlculate In reports covering Phaaea I and TT»

-------
                                                               TABLE  2.   SMOKE  DATA

Unit 36







Unit 37






Unit 38
Unit 36







Unit 37






Unit 38
Operational
Firing Cycle C°2' *
10/20(a) 9.7
11.0
12.1
12.3
12.3
12.9
13.3
13.6
10/20 11.3
11 7
11.8
11.8
12.0
12.3
12.9
10/20 12.5
Steady state 9.7
11.0
11.9
12.3
12.2
12.8
13.3
13.5
Steady state 11.3
11.8
11.9
11.8
12.0
12.3
12.9
Steady state 12.5
Data
o2. %
7.5
5.8
4.2
3.9
3.8
3.3
2.6
2.3
5.8
5.0
4.6
4.5
4.4
4.0
3.2
3.8
7.6
5.9
4.3
4.0
3.9
3.4
2.7
2.4
5.8
5.0
4.6
4.5
4.4
3.9
3.3
3.7

Excess Air. TL
54
37
25
23
23
18
14
12
35
30
28
27
26
23
18
22
55
38
26
23
23
19
15
13
35
29
27
27
26
23
18
21

1 mm
0.3
0.7
2.9
1.9
4.3
7.9
8.1
8.3
0.2
0.8
0.6
1.0
1.0
1.9
5.2
0.3

















3 mm
0.3
0.6
0.6
0.6
1.0
1.7
5.4
4.7
0.2
0.8
0.6
1.0
0.9
1.7
5.4
0.3

















5 mm
0.3
0.3
0.3
0.5
0.7
1.0
3.9
4.8
0.2
0.8
0.5
0.9
0.8
1.6
5.4
0.3

















7 mm
0.3
0.3
0.3
0.5
0.6
1.0
3.0
4.1
0.2
0.7
0.5
0.7
0.8
1.5
5.4
0.3
















Smoke .
Bacharach
N umbe r
9.5 mm 10 nun 30 mm
0.3
0.3
0.3
0.5
0.6
0.3
3.0
4.0
0.2
0.8
0.5
0.7
0.7
1.5
--
0.3
































0.3
0.3
0.3
0.5
0.3
0.7
1.8
4.0
0.2
0.7
0.7
0.9
1.0
2.3
5.8
0.3
















0.3
0.3
0.3
0.5
0.3
0.6
2.1
3.9
0.2
0.8
0.7
0.8
1.0
2.2
5.8
0.3

50 mm
















0.3
0.3
0.3
0.5
0.3
0.6
2.1
4.0
0.2
0.7
0.6
0.8
1.0
2.3
5.6
0.3

70 nun
















0.3
0.5
0.3
--
0.3
0.7
?.l
4.1
0.2
0.7
0.7
0.9
1.0
2.3
5.4
0.3

100 mm
















_.
0.3
0.3
--
0.3
--
?. 1
--
0.2
--
0.7
0.8
1.0
2.2
--
0.3
                                                                                                                                                             00
(a)   Cycle of 10 minutes on and 20-mlnutes off.

-------
readings for Unit 37 were nearly as low as the steady-state values and,
hence, it appears that this unit stabilizes relatively quickly from a
cold start.  The shorter start-up transient for Unit 37  was somewhat
unexpected  in  that  it was the unit having the heavier refractory com-
bustion chamber and, thus, was expected to have slower temperature
response.  The excellent start-up properties of Unit 37 are apparently
due to superior burner design and/or nozzle characteristics.

Smoke Versus Excess Air

         Figures 4 and 5 show plots of Bacharach smoke number versus
air for runs with Units 36 and 37, respectively.  Data plotted in these
figures are 9.5-minute smoke data for the cyclic runs and 100-minute
smoke data for the steady-state runs.  By the 9.5-minute point in the
cyclic runs, the smoke levels were essentially equal to the steady-
state values.
         Both units demonstrated low smoke at relatively low excess air
levels.  Units 36 and 37 reached No.  1 smoke at about 18 and 26 percent
excess air (12.9 and 12.0 percent CO.), respectively.  No field units
from the Phase II study exhibited smoke levels as low as No. 1 Bacharach
at such low excess-air levels.  (Data at lower excess-air values were ob-
tained on Unit 37 during these runs than when this unit was investigated
during the Phase II study; this was accomplished by modifying the air
gate to reduce leakage in the closed  position.)
         For Unit 38, the flame-retention burner from Unit 37 firing
into the furnace, a 0.3 smoke number  was obtained at 22 percent excess
air.  This smoke reading agrees more  with the observed smoke versus
excess air characteristics of the Unit 36 data than with that for Unit 37.
The flame-retention burner produced low start-up smoke at relatively low
excess air when fired in the furnace  (0.3 smoke  number at both 1.0 minute
and steady state), similar to its performance when fired into the boiler.

-------
                                  10
Particulate Emissions Versus Excess Air

         Figures 6 and 7 show plots of filterable participate emissions
(probe wash plus filter) versus excess air for runs on Units 36 and 37,
respectively.  Figures 8 and 9 show similar plots but based on filter
catch alone, which is the portion of the total particulate catch that
should relate best to smoke data.  Particulate emissions were collected
                       *
using the EPA Method 5,  but only filterable particulate was dried and
weighed.
         For Unit 36 (Figures 6 and 8), particulate emissions were
appreciably less for the steady-state runs than for the cyclic runs,
suggesting that cycling (probably startup) contributes significant
quantities of particulate to particulate measurements "integrated" over
the cycle.  The ratio of cyclic particulate to steady-state particulate
was nearly four to one at low excess air; this ratio decreased as excess
air was increased so that, at 40 to 50 percent excess air, cyclic partic-
ulate emissions were less than twice the level of steady-state emissions.
         The difference in particulate emissions between the cyclic and
steady-state runs is attributed to particulate generated during burner
startup and shutdown.  Hence, for this unit, it appears that the startup
and shutdown "puffs" contribute between 30 and 75 percent of the partic-
ulate emissions measured while operating a burner on a 10-minute-on/
20-minute-off cycle.  Because this unit also exhibited high smoke levels
during startup, it is concluded that high startup smoke may be an indica-
tion of high levels of particulate emissions during startup.

         Both cyclic and steady-state particulate emissions increased
significantly as excess air was reduced below 20 percent.
         For Unit 37 (Figures 7 and 9), the cyclic and steady-state runs
produced about the same particulate emission levels at given excess air
levels. These data, combined with the low smoke early in the cyclic runs,
*  Silver filters were used for runs on Unit 37;  whereas,  EPA Method 5
   specified fiberglas.

-------
                                  11
suggest  that start-up transients are minor for this unit.  Again, both
cyclic and steady-state particulate emissions increased significantly as
excess air was reduced below about 20 to 30 percent.
         The filter loadings and particulate emissions for runs on both
units are in the same range of values as the data from the Phase I and II
field studies(1'2).

_Part_iculate Loading. Versus Smoke

         Figures 10 and 11 show the correlations between filterable partic-
ulate loading (probe wash plus tiltcr catch) and the 9.5-minute smoke
reading for cyclic runs or 10--.iinute smoko reading for steady-state runs
for Units 36 and 37, respectively.  Figures 12 and 13 show similar data
for filter catch alone (without probe wash).  For both units, there is
considerable scatter of data below No. 1 smoke, but a correlation between
particulate emissions and smoki- appears piactical above this smoke level
for a given unit operating on a given cycle.
         Figures 10 and 11 show that, for both units, the rycli.c runs
gave a different correlation between filterable partirulatc emissions
and smoke than did tbc steady-stai.e runs.  Figures 12 and 13 show that
the correlations between filter catch and smoke number tor the steady-
state run for Unit 36 and both runs for Unit 37 were similar.  However,
the cyclic run for Unit 36 produced H qnitr: different correlation.
         Figure 14 shows the correlation between particulate based on
filter catch only an.3 smoke- at the 1 ,0-irinute point for cyclic runs in
both units.   The correlations between particulate emissions and smoke for
Units 36 and 37 arc inore nearly similar when the 1.0-minute smoke reading
is used as the data base.  However, ther^ is considerable scatter in these
data for Unit 36.
         Comparing the cyclic-run results shown in Figures 10 and 11, it
can be seen that Unit 37 emitted l(.v-:s parL jculate at a No. 5 smoke than
did Unit 36 at a No. 2 smoke.  This illustrates the difficulty of con-
trolling air pollution emissions from residential heating by basing regu-
lations on smoke reading alone.

-------
                                  12
         Figure 15 shows participate emissions plotted against smoke
number  (at 9.5 minutes) for cyclic runs and for steady-state runs for
all three units.  The data are too few to draw certain conclusions about
a general relationship of particulate emissions and smoke.  The scatter
in the data do not suggest that a strong correlation between particulate
emissions and smoke exists for the total of the cyclic data from these
two units. It appears that different start-up characteristics of the two
units are the primary factor preventing correlation of smoke number and
particulate emissions.  This helps to explain why such correlations were
not possible with the field data from Phases I and II.  However, within
limits of the available data, Figure 15 does show a fairly definite re-
lationship between steady-state particulate emissions and smoke.

Particle Size

         Figures 16 through 21 show plots of paLticle-size distribution
for samples collected by a Battalle Cascade Impactor during six steady-
state runs on Unit 37 with excess air ranging from 18 to 35 percent.
Runs were made at smoke levels from 0.2 to 5.8 Bacbarach smoke numbers,
with duplicate samples collected during each run.  All runs were for 60
minutes except Runs B in Figures 16 and 21 which were for 30 minutes.  A
particle specific gravity of 2.0 was assumed for calculating the cutoff
particle size for each impactor sta^e.
         These data indicate that 80- to 90-veight percent of the partic-
ulate was below 0.25 microns in size, even with the higher smoke levels.
Little difference in partLcle-size distribution Is evident for the various
runs.
         An electron-microscope examination of selected particulate filters
was made to provide an alternative determination of particle size (an opti-
cal microscope cannot see below about 0.25 microns).  Figures 22 through
29 show electron microscope photographs as follows:

-------
                                 13
          •   Figure  22         -   1000X view of a  fiberglas  filter
                                with collected participate  (Unit  36
                                run at  14 percent excess air)
          •   Figures 23-24     -  1000X and 5000X  views of clean
                                 (unused) silver  filters
          •   Figures 25-29     -  ?OX, 100X, 50QX, 1000X, and 5000X
                                views of silver  filters with
                                collected particulate  (Unit 37
                                run at  23 percent excess air).

Although these electron-microscope photographs (particularly Figures 25
through 28)  show the presence or some larye particles,  Figures 22  and
29 suggest that a significant portion of i:he collected  material  is well
below one micron in particle: size.  The possible  presence of agglomerations
makes determination of the size of individual particler-. difficult.  How-
ever, these photographs appear to confirm the facf.  that most of  the
particles emitted by the furnace and boiler were  quite  small,  below one
micron, placing them withjn the respirable size range which is consid-
ered to be below about 3.5 ricrons  ' ''.

                             CONCT I'S I0\'?

          Although the conclusions of this invoscigacion must  be con-
sidered in the context, of data limited to only two  units,  the  following
conclusions can be made::
          •  Filterable particalato emissions vary  with excess
             air in approximately the sam3 manner as smoke: readings;
             that is,  particular emi3Sions are telatively low at
             high excens air anJ increase significanrl >r as excess
             air is reduced. Thus, smoke readings arc indicative
             of particulace enissiim trencs for a gi >;rn unit and
             operating condition.

-------
                                  14
         o  Correlations of particulate emissions and smoke appear
            possible for given operating cycles for particular units
            and possibly for different units at steady-state conditions,.
            However, data for cyclic conditions of the two units ex-
            amined do not suggest that a general relationship between
            particulate emissions and smoke exists when considering
            more than one unit, primarily due to differences in start-
            up characteristics.  This observation confirms the results
            of the Phase I and II studies where no general relationship
            between particulate emissions arid smoke was found.

         o  A greater difference between cyclic and steady-state partic-
            ulate emissions was observed for the unit that had high
            start-up smoke than for the unit that did not have high
            start-up smoke.  Hence, high start-up smoke appears to be
            an indicator of nha startup contributing a disproportionately
            large quantity of particulace emissions.

         o  Particle-size distribution did not change significantly for
            a given unit aw excels air and smoke were varied.

         o  Particle-size measurements indicated that most particulate
            emitted by these units was below one micron,  and in the
            respirable range.  (The respirable range is not precisely
            defined but is roughly below 3.5 microns.)
Additional  Information Needed


          Although the results do not show a firm correlation between

particulate emissions arid smoke when different cycles and equipment are

considered, the results show that there is a trend toward lower  partic-
 ulate emission with  lower  smoke  numbera.   Thus,  if the  desired  partic-

 ulate emission control  level  falls  in  the  range  of data observed for

low smoke number values, the smoke number might be used as a satis-

factory control.   To do this, it: would be necessary to accumulate con-
                         v
 siderably more data  on  the?  relationship between  smoke number and partic-

 ulate emission for a large  number of oil-fired units under different
operating conditions.

          The  following information that is presently not available

would contribute to a better understanding of this subject:

-------
                                 15
          •  Particulate data versus excess air and smoke for a
             variety of burners and applications

          •  Effect of nozzle firing-rate characteristic on starting
             (including consideration of nozzle temperature)

          •  Cycles other than 10-on and 20-off, especially shorfor
             cycles

          •  Effect of pump cut-off characteristics

          •  Particular characterization versus particle size
                Chemical composition:  carbon, hydrogen, and
                nitrogen contents aa.d polycyclic organic matter (POM).

          •  Effect of filter material on particulate measurement
             (roact-ion of silver filters with sulfur).
This latter work uould he- justified CMly if particulate emissions from
domestic oil-fired equipment are considered to be a significant contri-
bution in the overall particula-jt anatem^nt problem.

-------
                                  16
                              REFERENCES
(1)   Levy, A.,  Miller,  S.  E.,  Barrett,  R.  E.,  et al.,  "A Field Investiga-
     tion of Emissions  from Fuel Oil Combustion for Space Heating",  API
     Publication 4099,  November 1,  1971,  available from the API Publi-
     cations Section,  1801 K Street, N.W.,  Washington,  D.  C.   20006.

(2)   Barrett, R.  E., Miller,  S.  E.,  and Locklin, D.  W., "Field Investi-
     gation of Emissions from Combustion  Equipment for  Space Heating".
     This report is  identified as API Publication 4180  (available from
     API); PB-223148  (available from NTIS); and as EPA  Publication
     EPA-R2-73-084a, all June, 1973.

(3)   "Standards of Performance for  New  Stationary Sources",  Federal
     Register,  Vol.  36,  No.  139, Part II,  pp 24876-24895,  December 23,
     1971.

(4)   Pilcher, J.  M., Mitchell, R. I., and  Thomas, R.  E.,  "The Cascade
     Impactor for Particle-Size Analysis  of Aerosols",  presented  to  the
     Chemical Specialists  Manufacturers Assoc., Inc., New York City,
     December 6 and  7,  1955.

(5)   Dunmore, J.  H., Hamilton, R.J., and  Smith, D.S.G., "Instrument  for
     the Sampling of Respirable Dust for  Subsequent Gravimetric Assess-
     ment", J.  Scientific  Instruments,  41.  669 (1964).

(6)   Lippman, M., and Harris,  W. B.."Size-Selective Sampling for Esti-
     mating 'Respirable1 Dust  Concentrations", Health  Physics, 8, 155  (1962)

-------
                           17
Large particle-**
          Impaction slide
                  "*-Small particle
                                         First Stage:
                                              Large  jet
                                              Low  velocity
                                              Large  particles  impact
                                         Succeeding Stages:

                                              Smaller  jets
                                              Higher  velocities
                                              Smaller  particles  impact
      FIGURE  1.  SCHEMATIC DIAGRAM SHOWING PRINCIPLE
                 OF THE  CASCADE  IMPACTOR

-------
                                         18
CO
u
o


I
u
o
CD
                             25 % Excess air


                               23% Excess air
                            I
                            34567


                              Time From Start of Cycle,  minutes
8
10
              FIGURE 2.   SMOKE VERSUS TIME DURING CYCLE -

                           UNIT 36

-------
en


u
o



I  «
                                              19
                                18% Excess air
                26% Excess air

         28 % Excess air
(cess air—i
                             23% Excess air
                            1	a-



                      27 % Excess air
                     _L
       , 35 % Excess oir  -

       T       I         T
                                                                    30 % Excess air
                                                   ±
JL
             i
                                                 8
         234567


                   Time From Start of Cycle,  minutes



FIGURE 3.   SMOKE VERSUS TIME DURING CYCLE -  UNIT 37
         10

-------
                                      20
o
o
en
o
o
o
                                             Operation
                                     x - Cyclic (smoke at 9 5 mm)
                                     o - Steady  state (smoke at 100min)
                        Cyclic and steady state
              Unit 38
             Cyclic
             Steady state

                I
       xo
             I
1
                10
20          30          40
    Excess Air, percent
            50
60
        FIGURE 4.  SMOKE VERSUS EXCESS AIR - UNIT 36

-------
                                       21
                                            Operation

                                    x - Cyclic (smoke at 9 5 min)
                                    o - Steady state (smoke at 100 min)
o
z
a>
o
o
o
o
u

-------
                                       22
      4.5
      3.5
      30
   O
   O
   g

   £  25

2.0
   6
   UJ

   a>
   o
   0.
  I   I*
   0)
       10
      05
                  Steady state
                                I
                                     I
                                                       Operation

                                                    x - Cyclic

                                                    o - Steady state
                    10
                         20         30          40

                             Excess Air,  percent
50
60
FIGURE 6.   FILTERABLE PARTICULATE EMISSIONS VERSUS EXCESS

              AIR  - UNIT 36

-------
                                       23
    3.5
    30
    25
O
O
g

£  2.0
 in

 o
o>
B
o

I
il
    15
    10
    0.5
                  10
                                                       Operation

                                                    x - Cyclic

                                                    o - Steady  state
                                   Cyclic and steady state
                                       o  o
                                      x
                                      °oX
                              1
                        1
20          30          40


    Excess Air, percent
50
60
   FIGURE 7.  FILTERABLE  PARTICULATE EMISSIONS VERSUS EXCESS

                AIR - UNIT 37

-------
    4.0
    3.5
    30
 0)
 o
 on
025
O
O
O  2.0
jC
o

3
—  1.5
en
tf>
'E
UJ


    1.0
    0.5
                              Cyclic
                                                         Operation

                                                      x - Cyclic
                                                      o - Steady state
                                            1
                                                        1
                   10
                               20          30          40

                                   Excess Air, percent
50
60
       FIGURE 8.  FILTER  CATCH VERSUS EXCESS AIR - UNIT 36

-------
                                        25
    4.0
    3.5
                                                           Operation
                                                        x - Cyclic
                                                        o -Seady state
    3.0
 o
"55
 o
~  2-5
O
O
O
I 2-0
JC
o
o
O
0)
E
UJ
    1.5
    1.0
   0.5
Cyclic \ \Steady state

                 o
                   I
      1
                                   I
I
                   10
                                           50
                      20          30           40
                          Excess Air,  percent

FIGURE 9.  FILTER CATCH VERSUS EXCESS AIR -  UNIT 37
                        60

-------
                                      26
     45
     40
     35
     30
   (A
  >^

   a*
  I 25
  o
  9)

  O
  0)
  r>
  o

  v
     15
     10
                              I
I
                                                            Operation


                                                         x  - Cyclic

                                                         o  - Steady  state
I
                              234

                          Bacharach Smoke No (at 9 5 or 10 min)
FIGURE  10.   FILTERABLE PARTICULATE LOADING VERSUS SMOKE

               UNIT 36

-------
   35
                                      27
   30
                                                     Operation


                                                 x - Cyclic

                                                 o - Steady state
'   20
o
o
5
3
O
o
a.
a

a3
    15
   10
                 12345


                        Bacharach Smoke No. (at 9.5 or 10 min)



       FIGURE 11.   FILTERABLE PARTICULATE LOADING VERSUS

                     SMOKE - UNIT 37

-------
                                   28
40
35
30
25
20
 15
 10
                                                        Operation
                                                     x  - Cyclic
                                                     o  - Steady state
                         I
I
1
                         234
                     Bacharach Smoke No. (at 9 5 or 10 min)
  FIGURE 12.   PARTICULATE LOADING (BASED ON FILTER CATCH)
                VERSUS SMOKE -  UNIT 36

-------
                                      29
   30
   25
10
 
-------
                                 30
"E
 en
   40
   35
 o>
 E 30
_
 c
O

 o
 o
O
25
S 20
•§  '5
 O
    10
                                   Unit
                              x - Unit 36
                              o - Unit 37
                           I
                                      I
I
I
                           34567

                        Bacharach Smoke No. (at 1.0 min)
                                                            6
 FIGURE 14.  PARTICULATE LOADING (BASED ON FILTER  CATCH)
              VERSUS SMOKE AT  1. 0 MINUTE FOR CYCLIC RUNS

-------
                                     31
 8
 o>
 o
 jQ
 O
      45
      35
      30
      25
      15
      10
Cyclic  runs
  n  Unit  36
  o  Unit  37
  A  Unit  38
Steady-state runs
  •  Unit  36
  •  Unit  37
  A  Unit  38
                              I
                                        I
                              234

                         Bacharach Smoke No (at 95 or  10 mm)
FIGURE  15.   FILTERABLE PARTICULATE LOADING  VERSUS SMOKE
               CYCLIC OPERATION OF UNITS 36 AND  37

-------
                             32
99
OQ
yo
95
an
ftft
O\J
£ en
o» WJ
'a;
> KH
& DU
S* ^in
•Q «»U
c -in
QJ OU
e
n o/^
Q- 20
V
_>
n iu
3 R
O 5


0.5
0.2
.1
f\ /NC
O.O5
0^\i
.01


X"

-x — •














).2 0.




— x~














3 0




. •










.



4



















0



















6



rfM















c



















1.8



^

















RunAx

Run BX
	 	 x*^









.





*•
/
X
/
/















> •



















5 "



















J



















(



















k



















(



















J



















l(



















D 2C
                 Equivalent Particle Diameter, microns
FIGURE 16.   PAPTICLE-SIZE DISTRIBUTION FOR UNIT 37
              AT 35 PERCENT EXCESS AIR

-------
                                      33
   99
   98

   95
   90

   80
   70
I, 60
'o>
$ 50
o 40
   30
       Run B
Run A

   20
    10
<§  5
   0.5
   0.2
   O.I
 0.05
  0.01
     0.2   0.3   0.4    0.6  0.8 I          2346
                          Equivalent Particle Diameter, microns
                            8   10
20
        FIGURE  17.  PARTICLE-SIZE DISTRIBUTION FOR  UNIT 37
                      AT 29 PERCENT EXCESS AIR

-------
                           34
99
98
95
90
80
70
1, 60
o>
$ 50
.0 40
§30
£ 20
0)
>
| 10
1 5
2
1
0.5
02
O.I
005
O.OI(


v
fi^

















X**"
^
^o-

















— -—
*• •*

















-. •
•• ••

















«
^^t
— <

















t
>^

















•*
—•
















»i
^"
















Run AX
^****'*
RunB^.
	 •**'>















X
S
/
^
















f
/






















































































































































)2 0.3 0.4 06 0.8 2 3 4 6 8 10 2C
Equivalent Particle Diameter, microns
FIGURE 18.   PARTICLE-SIZE DISTRIBUTION FOR UNIT 37
             AT 27 PERCENT EXCESS AIR

-------
                                35
99
98
95
90
80
70
1. 60
'
>
5 10
I 5
2
1
05
02
O.I
005
n r»i


^
(
/
/















X^.
r»X
s
















~~~
^

















~* -
^-

















•^»J
>
















^>
w
>^
















X
^

















X1
X
















Run^x
x/
x^Run B



























































































































































































02   0.3  04
FIGURE 19.
               0.6  08  I          2      34      6
                   Equivalent Particle Diameter, microns
8  10
20
                PARTICLE-SIZE DISTRIBUTION FOR UNIT 37
                AT 26 PERCENT EXCESS AIR

-------
                                       36
   99
   98

   95
   90

   80
   70
I. 60
'o>
$ 50
£ 40
§30
   20
 0)
 >
|  10
o
   05
   0.2
   O.I
  0.05
  0.01
0.2   0.3   0.4
0.6  0.8 I           2346
    Equivalent Particle Diameter, microns
                                                                 8  10
20
        FIGURE 20.  PARTICLE-SIZE DISTRIBUTION FOR  UNIT 37
                      AT 23 PERCENT EXCESS AIR

-------
                                       37
   99
   98

   95

   90

   80

   70
I. 60
'55
$ 50
n 40
£ 30
u
0-  20

|   10

J   5

    2
     I
   05
   0.2
   O.I
 005
 /
  0.01
0.2   0.3  0.4
0.6   0.8  I           2346
    Equivalent Particle Diameter, microns
                                                                8   10
20
         FIGURE 21.  PARTICLE-SIZE DISTRIBUTION  FOR UNIT 37
                       AT 18 PERCENT EXCESS AIR

-------
    1000X
             Scale
'4-
1 Micron
FIGURE 22. PARTICULATE ON FIBERGLASS FILTER
    1000X
             Scale
-4-
1 Micron
      FIGURE 23.  CLEAN SILVER FILTER


-------
                    39
   5000X
             Scale:  ~*j  r«—  1 Micron




     FIGURE 24.  CLEAN  SILVER FILTER

   2 OX
FIGURE 25.  PARTICULATE ON SILVER FILTER

-------
    100X
FIGURE 26.  PARTICULATE ON SILVER FILTER

   500X
              Scale
1 Micron
FIGURE 27.  PARTICULATE ON SILVER FILTER

-------
                     41
    1000X
Scale:
                           1 Micron
FIGURE 28.  PARTICULATE ON SILVER FILTER
    5000X
                         •*—  1 Micron
FIGURE 29.  PARTICULATE ON SILVER FILTER

-------
                                      42
                                TECHNICAL REPORT DATA
                          (I'lcaw read liiwuc Horn 
-------