EPA-650/2-73-002
June 1973
Environmental Protection Technology Series

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                                 EPA-650/2-73-1
  CHEMICAL AND  PHYSICAL


      CHARACTERIZATION


  OF AUTOMOTIVE EXHAUST


     PARTICULATE  MATTER


     IN  THE  ATMOSPHERE


(Year  ending  June  30,  1973)

                  by

         J. F. Foster, D. A.  Trayser,
        C, W. Melton, and R. I. Mitchell

        Battelle Columbus Laboratories
      505 King Avenue, Columbus, Ohio  43201

          Contract No. 68-02-0279
          Program Element No. 1A1010

      EPA Project Officer:  Dr. Jack Wagman

        Chemistry and 'Physics  Laboratory
     National Environmental Research Center
    Research Triangle Park, North Carolina  27711

               Prepared for

       COORDINATING RESEARCH COUNCIL INC.
            30 ROCKEFELLER PLAZA
            NEW YORK, NY 10020
          APRAC PROJECT CAPE-19-70

                  and

        OFFICE OF RESEARCH AND MDNITORING
     U. S. ENVIRONMENTAL PROTECTION AGENCY
            WASHINGTON, DC  20460

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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

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                     MANAGEMENT SUMMARY
The purpose of the program is to determine the physical and
chemical characteristics of exhaust particulate matter from
internal combustion engines as a function of sampling proce-
dure, engine operating conditions  (including emission control
systems), fuel composition, and residence time in the atmos-
phere.  Emphasis will be placed on predicting the fate of
exhaust particulate matter in the atmosphere.

The scope of the project work covers the generation of auto-
mobile particulate matter with specially chosen, measured
engines.  The auto exhaust is diluted in two stages:  first
in a mixing tunnel, then in a large residence chamber with
relatively small wall loss.  The properties of exhaust parti-
cles are being studied from their initial formation to their
ultimate remo'val from the chamber atmosphere.

A major experimental study has been necessary to develop test
procedures which give as true as possible values of the
particulate emissions.  This has been a consequence of the
very small weights of the particulate matter and the very
large dilutions necessary to simulate the way they exist in
the atmosphere, as well as the fact that the collection of
particulate material is strongly affected by the techniques
used to collect them.  Thus the geometry, temperature, and
velocity of the sample stream had to be set to optimums, as
well as the size, weight, and type of filter used, weighing
techniques, and the many car operating variables.

In the study thus far, two identical 1970 Fords with matched
standard 1971 engines (engine modification emission controls)
were conditioned similarly for 5,000 miles on unleaded fuel,
and shown to have equivalent emission characteristics.  The
vehicles then were operated for an additional 8,000 miles, one
on unleaded fuel, the other on the same base fuel to which
had been added 2.5 grams lead per gallon measured as TEL Motor
Mix.  During this phase, exhaust gas emissions and particulate
matter were measured at preselected intervals.  The gaseous
measurements enabled a detailed assessment of vehicle opera-
tion to be made.  The particulate matter was sampled from the
dilution tunnel and the residence chamber in each run.  The
material collected from the dilution tunnel is considered
representative for fresh auto exhaust as it is emitted into
the atmosphere.  The particles sampled from the residence
chamber inidcafe the nature of the air-suspended fraction
after aging for periods  up to 24 hours.

In this contract year two major problem areas were encountered
and significant efforts were devoted to solving them.  The

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first relates to reproducible day-to-day operation of vehicles
for particle generation.  Vehicle operation during the cold
start portion of the cycle and  the operation of  the choke
were found to be critical.  These problems have  been identi-
fied and the procedures have been standardized for reproduci-
ttlity.

The second problem relates to the measurement by filtration
of the carbonaceous particulate matter in vehicle exhaust.
A filter sampling system and filter media have been selected
that show reproducible weight gain.  Work on the filtration
problem continues with the aim of establishing a procedure
for absolute measurements.

The total particulate emission rate from the nonleaded car is
in the range .0.04-0.075 gram per mile for the 1972 FTP (Federal
Test Procedures) Cycle.  There  is a correlation  between  the
particulate and the hydrocarbon emission rates.  The parti-
culate emissions from leaded fuel were 0.05 to 0.15 g/mile
more than those from unleaded fuel, or from 60 to 100*percent
higher when compared at the same hydrocarbon emission level.
For both fuels the mass median equivalent diameter of the
exhaust particles sus.pended in the dilution tunnel and in the
residence chamber were in the submicron size range.  Measure-
ments with the Minnesota Aerosol-Analyzing System indicate
a bimodal size distribution.

Electron microscope studies of  the exhaust particles suggest
four possible, mechanisms of particle growth; agglomeration,
condensation, crystal growth, deposition and ablation of exhaust
system deposits.

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                           TABLE OF CONTENTS
MANAGEMENT SUMMARY .........................      i

INTRODUCTION ............................      1

OBJECTIVE .......... „ ..................      2

EXPERIMENTAL APPARATUS AND PROCEDURES ...............      2

     Fuels .............................      4

     Project Cars . . .......................      4

     Conditioning of Cars .....................      4

     Test Cycles ..........................      5

     Test Run Procedure ......................      5

          Preconditioning .............. .  ......      5

          Test Run. ........................      6

          Post-Cycle Operation Check ................      6

     Engine Air Flow Measurements .................      6

     Choke Operation ................... .....      7

     Dilution Tunnel ........................      8

     Residence Chamber .......................      8

     Instrumentation ........................      8

     Filtration and Weighing ....................      9

EXPERIMENTAL RESULTS ...... . .................     12

     Exhaust Emission Rates  ....................     12

     Reproducibility of Mass of Particulate Emissions .......     14

     Correlation of Light Scattering with Mass ...........     18

     Addition of Foreign Materials to the Residence' Chamber ....     18

     Size Distribution of Auto Exhaust Particles
       with the Cascade Impactor ..................     22


                                 iii

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                           TABLE OF CONTENTS
                              (Continued)
     Size Distribution of Particles with the
       Minnesota Aerosol-Analyzing System 	    22

     Correlation of Particulate Mass with
       Hydrocarbon Emissions	    26

     Morphological Characteristics of Particles 	    28

CONCLUSIONS	  .  .	    31

          Emission Levels ..............  	  .    31

          Particulate Characteristics	 .  .  .  .    34

          Morphological Analysis	    34


                               APPENDIX


     Fuels	A-l

     Air Flow Measurements	A-4

     Car Maintenance	f .  .  .  .   A-4

     Oil Consumption	A-7

     Development of Acceptable Choke Operation	   A-7

          Apparatus	A-7

          Characteristic Stages in Choke Schedules	A-10

          Experimental Studies of Choke Schedules  	   A-ll

     Choke Schedules and Starting Sequences 	   A-14

          Choke Schedule I (Modified LA-4 Cycle)	A-14

          Choke Schedule I-S (Standard LA-4 Cycle)	A-14

          Choke Schedule II (Modified LA-4 Cycle)	A-16

          Choke Schedule II-S (Standard LA-4 Cycle)	A-16

          Periods of Choke Schedule Use	A-16
                                IV

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                      TABLE OF CONTENTS
                         (Continued)

                                                                Page

Summary of Test Conditions in Experimental Runs	A-18

Dilution Tunnel	A-18

     Sample Probes	»	.	A-18

     Tunnel Sample-Point Pressure	A-23

     Tunnel-Bag Sample	A-23

     Calculation of Exhaust Mass Emissions
       from Tunnel-Bag Sample.	A-26

     Lead Deposits in Pipe to Residence Chamber	A-26

     Test for Uniformity of Mixing in the Tunnel ........ A-27

     Gaseous Contaminant Injection System	A-27

     Solid Contaminant Injection System	A-29

     Dust Contaminant	   A-29

Residence Chamber	A-32

     Chamber Configuration 	   A-32

     Dilution Ratio Experiments	A-35

     Chamber Mixing Experiments	   A-37

     Chamber Humidification.  .... 	   A-38

     Dilution Ratio Definition and Method of Calculation . .  .   A-41

Instrumentation.	„	   A-42

     Gas Analysis	.	   A-42

     Speed Controller	A-46

     Minnesota Aerosol-Analyzing System	A-46

Studies of Filtration and Weighing  Procedures	A-47

     Microbalance in Controlled Atmosphere Balance Room. . .  .   A-47

     Repeatability of Weighings with the Microbalance	   A-47

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                           TABLE OF CONTENTS
                              (Concluded)

                                                                     Page

          Filter Media	  .   A-49

          Pattern of Sampling for Particulate Matter	A-51

     Experimental Results — Supplementary Data	A-51

          Test Conditions	A-rSl


                            LIST OF TABLES


Table 1.  Summary of Test Results	  .    13

Table 2.  Mass Emissions of Particles Collected
          From Tunnel by Filtration	    15

Table 3.  Mass Concentrations of Particles Collected from
          Tunnel and Residence Chamber	•.    16

Table 4.  Correlation of Light Scattering with Aerosol
          Mass in the Residence Chamber	    19

Table 5.  Studies of Environmental Variables	    21

Table 6.  Comparison of Automobile Particulate Data	    23



Table A-l.  Characteristics of Fuels. ........  	   A-l

Table A-2.  Oil Consumption During Test Series	A-8

Table A-3.  Test Data Relating to Choke Schedule Development.  .  .  .   A-13

Table A-4.  Summary of Experimental Studies of Exhaust Emission .  .   A-19

Table A-5.  Chemical Composition of Fine Arizona Dust	A-32

Table A-6.  Summary of Initial Tunnel-to-Chamber
            Dilution Ratio Experiments	A-36

Table A-7.  Gas Analysis Instruments	A-43

Table A-8.  Repetitive Weighings of Blank Filters and
            Other Materials	   A-48

Table A-9.  Laboratory and Operating Data for Modified and
            Standard LA-4 Cycle Runs	   A-52
                                  vi

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                            LIST OF TABLES
                              (Continued)
                                                                   Page

Table A-LO.  Air-Fuel Ratios Determined from Steady-State
             Exhaust-Gas Analyses After Each Run	  A-53

Table A-ll.  Dilution Ratios of Diluted Exhaust in
             Residence Chamber for Modified and Standard
             LA-4 Cycle Runs	A-55
                            LIST OF FIGURES
Figure 1.  Perspective View of Test Apparatus and
           Auxiliary Instrumentation	   3

Figure 2.  Correlation Between Light Scattering and
           Aerosol Mass Concentration	 .  19

Figure 3.  Volume Distribution of Unleaded Particles	24

Figure 4.  Volume Distribution of Leaded Particles	25

Figure 5.  Correlation Between Particle Emissions and
           Hydrocarbon Emissions	  27

Figure 6.  An Electron Micrograph of Unleaded Exhaust
           Particulate Collected at the 0.5 u.m Impactor Stage
           After 4 Hours Residence (Run 4-17)	29

Figure 7.  An Electron Micrograph of Leaded Exhaust Particulate
           Collected at the 0.5 um Impactor Stage After 4
           Hours Residence (Run 4-25)	29

Figure 8.  Electron Micrographs Showing Nonleaded Exhaust
           Particulate From Run 12-15	30

Figure 9.  Electron Micrographs Showing Leaded Exhaust
           Particulate From Selected Experiments. ........  32

Figure 10. Electron Micrographs Showing Effects of Dust,
           Ammonia, and Humidity from Selected Experiments. ...  33
Figure A-l.  Variation of Engine Air Flow and Road Horsepower
             with Vehicle Speed Using Unleaded Fuel 	  A-5

Figure A-2.  Air-Fuel Ratio Versus Carburetor Air Flow
             With Unleaded Fuel	  A-6

Figure A-3.  Device  for Controlled Choke Opening on a
             Reproducible Time Schedule	  A-9
                                VI1

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                            LIST OF FIGURES
                              (Continued)
Figure A-4.  Idealized Choke Opening Schedules for
             Modified Cold-Start LA-4 Cycle	    A-12

Figure A-5.  Choke Schedule I	    A-15

Figure A-6.  Choke Schedule I-S	    A-15

Figure A-7.  Choke Schedule II	    A-17

Figure A-8.  Choke Schedule II-S	    A-17

Figure A-9.  Pattern of Probe Inlets in Cross-Section
             of Dilution Tunnel at Sampling Point	    A-21

Figure A-10. Connection at Tunnel of Pipe to Carry Diluted
             Exhaust to Residence Chamber	    A-22

Figure A-11. Recorded Differential Pressure Between Tunnel and
             Residence Chamber During a Modified LA-4 Cycle. . .    A-24

Figure A-12. Tunnel-Bag Sampling System	    A-25

Figure A-13. Gaseous Contaminant Injection System	    A-28

Figure A-14. Schematic of Dust Feeder	    A-30

Figure A-15. Particle Size Distribution of Classified
             Arizona Road Dust	    A-31

Figure A-16. Layout of Residence Chamber and Purge-
             Circulation System	    A-33

Figure A-17. Tunnel-To-Chamber Sample-Pipe Discharge Nozzle. . .    A-34

Figure A-18. Time To Mix Propane in Residence Chamber with
             Sample Inlet Nozzle Shown in Figure A-17	    A-39

Figure A-19. Schematic of Wick-Type Humidifier in Residence
             Chamber Purge Duct	    A-40
                                 Vlll

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                    FOURTH ANNUAL SUMMARY REPORT
                                  on
              CHEMICAL AND PHYSICAL CHARACTERIZATION OF
                AUTOMOTIVE EXHAUST PARTICUIATE  MATTER.
                          IN THE ATMOSPHERE
                                  to
                    COORDINATING RESEARCH COUNCIL
                  (CRC-APRAC PROJECT NO.  CAPE-19-70)

                                 and

                   ENVIRONMENTAL PROTECTION AGENCY
                      CONTRACT NO.  68-02-0279)

                                 from

                               BATTELLE
                        Columbus Laboratories

                            July 25, 1974
                             INTRODUCTION



          This report describes a fourth year  '  '    of studies directed

toward determining the fate of auto exhaust particles in the atmosphere.
During this year two preconditioned cars have been operated on test cycles
under controlled conditions to generate particulate matter for detailed
(1)  C. W. Melton,et al, "Physical-Chemical Characteristics of Particles
     Associated with Polynuclear Aromatic Hydrocarbons Present in Automo-
     bile Exhaust", Final Summary Technical Report for the period Janu-
     ary 24, 1969, to March 31, 1970, to Coordinating Research Council
     (APRAC-CAPE-12-68-Neg. 59), January 29, 1970.

(2)  J. F. Foster, et al, "Chemical and Physical Characterization of Auto-
     motive Exhaust Particulate Matter in the Atmosphere", Final Summary
     Report for the period July 1, 1970, to June 24, 1971, to Coordinating
     Research Council (CAPE-12-68-Neg. 59 and CAPE-19-70), October 6, 1972.

(3)  C. W. Melton, R. I. Mitchell, D. A. Trayser, J. F. Foster, "Chemical
     and Physical Characterization of Automotive Exhaust Particulate Matter
     in the Atmosphere", Final Summary Report for the period June 25,
     1971, to June 30, 1972, to Coordinating Research Council (CAPE-19-70)
     and Environmental Protection Agency (Contract No. 68-02-0205),
     June 14, 1973.

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study.  In this report are presented descriptions of the apparatus, includ-
ing cars, exhaust-dilution tunnel, residence chamber for aging particulate
matter in suspension, and instrumentation; and procedures, including pre-
paration and maintenance of the cars, test cycles, and measurements of the
properties of generated particulate matter.  Development and standardization
of apparatus and procedures was carried out during the early part of the
year by operation of the cars, as well as by tests on indi-vidual segments
of the associated apparatus.
          Subsequently a total of 58 runs was  completed in the integrated
test system in which particles were generated from both leaded and unleaded
fuels.  Results from the 58 tests are 'tabulated in the experimental section.

                               OBJECTIVE

          The objective of the program is to determine the physical and
chemical characteristics of exhaust particulate matter from internal-
combustion engines as a function of sampling procedure, engine operating
conditions, lead content of the fuel, and the length of residence in the
atmosphere under various conditions.

                 EXPERIMENTAL APPARATUS AND PROCEDURES

          In this project, automobile exhaust particulates are generated
from  leaded or unleaded fuels used separately in each of two otherwise
identical automobiles having  specially chosen, measured engines selected
for similarity.  The auto exhaust  is diluted and mixed with  air  passing
through a 36-foot-long tube (the "dilution tunnel"), then passed  into  a
2100-cubic-foot residence chamber  large enough  to minimize wall  losses.
Figure  1  is a perspective view of  the test apparatus with  the  test car
positioned on the chassis dynamometer.  Exhaust is directed into  the  dilution
tunnel, from which a portion is taken into the residence chamber.

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                            SAMPLING POINTS:
                                     CHAMBER
                                     TUNNEL-
RESIDENCE CHAMBER
                                                             INSTRUMENTATION
                                                                                        u>
 FIGURE 1.  PERSPECTIVE VIEW OF TEST APPARATUS AND AUXILIARY INSTRUMENTATION

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                                 Fuels
          Two fuels were purchased from Mobil Research and Development
Corporation in January, 1972.  These gasolines were identical except for
lead content.  Fuel RE-141B was unleaded and RE-141C had 2.49 g Pb/gal.
Measured characteristics of the two fuels are reported in the Appendix,
Table A-l, pages A-l to A-3.

                             Project Cars

          Two 1970 Fairlane Fords with 1971 engines were prepared last
year for exhaust-gas generation.  The engines were 351 CID V-8's with
2-barrel carburetors and automatic transmissions.  In order to make
the two automobiles closely comparable, specially matched and measured
1971 engines were made available by the Ford Motor Company and were
installed in the two vehicles by project personnel at Battelle.  There
is no significant difference between the two cars, although one is
color coded white (Car W) and the other blue (Car B) for identification.
Only unleaded fuel has been used in the white car.  Only leaded fuel
has been used in the blue car, following a 4000-mile conditioning on
unleaded fuel.

                         Conditioning of Cars

          Each car was operated 8,000 miles to stabilize deposits.  Be-
ginning at 0 miles, each car was driven on a chassis dynamometer for 4000
miles with unleaded fuel, using a (modified) Durability Driving Schedule    .
Periodic measurements of volatile emissions were made during the 4000
miles to compare emission characteristics.  Car W continued for another
4000 miles on the modified Durability Driving Schedule with RE-141B unleaded
fuel, but Car B was operated for the second 4000 miles on leaded fuel
RE-141C.
 (1)  Standard Durability Driving Schedule as described in the Federal Register.
     Volume 35, No. 136, Part II, July  15,  1970, without the 70 mph lap.

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                              Test Cycles

          A modified Standard Urban Driving Cycle    was used during most
of the test runs, in which 35 seconds was added to the standard 20 seconds
of idle after engine start to give a total of 55 seconds idle time before
the first acceleration mode.  This cycle is designated the "modified
LA-4" cycle.
          In some test runs the standard cycle, with the specified initial
20-second idle, was used.  This cycle is designated as the "IA-4" cycle.

                          Test Run Procedure

          In cooperation with the CAPE-19 Project Group the following pre-
conditioning and particulate-emissions test procedure was established:

Prec ond it ioning

                                  (2)
          •  100 miles  on modified  '  MVMA Durability  Schedule
                         (3)
          •  Two modified    EPA (LA-4)  Urban Driving  Cycles  immediately
             after the  100-mile durability run
          o  Record tailpipe CO during EPA cycles
          •  Check tailpipe CO at  idle and adjust,  if  necessary,  to
             1.0 * 0.2  percent.
          a  Record tailpipe CO and 0   at idle and  50  mph  cruise  before
             shutdown for overnight soak
          •  Overnight  soak period of  at least 16 hours  at  70 F * 2 F.
(1)   Federal Register,  Volume 35,  No.  136,  Part  II,  July  15,  1970.
(2)   Standard Durability Driving Schedule as  described  in the  Federal
     Register. Volume 35,  No. 136, Part II, July 15,  1970, without  the
     70 mph lap.
(3)   Standard Urban Driving Cycle  as described  in July  15,  1970  Federal
     Register modified as  described in Test Cycles above  (basically
     35 seconds additional time at idle before  first acceleration mode).

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Test Run
           e  Actuate throttle, set choke to closed, adjust choke drive
              system to starting position
           ©  Simultaneously start particulate-filter sample pump, open
              sample-pipe valve to chamber, start tunnel-bag sampling
           9  After 15 seconds start car
           9  15 seconds after engine start "kick down" off high idle
           9  25 seconds after engine start put car in gear
           9  35 seconds after engine start, start speed controller tape
              (first acceleration mode begins 20 seconds later)
           9  5 seconds after full stop at end of last mode of cycle close
              sample-pipe valve and stop tunnel-bag and particulate sampling
              pumps.

 Post-Cycle Operation Check

           9  Operate car at idle, 35 mph cruise, and 50 mph cruise.
           •  Record tailpipe CO (Runs 12-1 to 1-15, Appendix, Table A-4) for
              evidence of change since preconditioning, and for check on
              emissions plus calculation of air/fuel ratio.  Supporting
              data on tailpipe oxygen, and on C07 and HC in diluted exhaust
              of tunnel were found to be less reliable for emissions and
              air/fuel ratio determinations, so improved instrumentation
              was employed in the next experimental phase.
           »  Record tailpipe CO, CO   0 ,  and HC for operation check,
              emissions, and air/fuel ratio.  (Runs 4-4 to 5-22, Table A-4)
           0  Shut off engine.

                      Engine Air Flow Measurements

           A  laminar  flow meter and  a differential  pressure  transducer were
  installed on the unleaded-fuel white car  prior  to  the regular test runs  to
  measure engine air flow during both the LA-4 cycles  and  steady cruise
  operation under the  above operating procedures.

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          With the laminar flow meter connected to the engine air cleaner
inlet, it was not feasible to preheat the carburetor air as in the normal
configuration.  Consequently, carburetor inlet air temperatures were slightly
lower during the air flow measurement runs than during regular test runs.
The effect of this departure from normal engine air flow is negligible.
          One run was made to measure engine air flow during a cold-start
LA-4 cycle, and another run to measure engine air flow during a hot-start
IA-4 cycle.  The average flow rate during the cold-start run was 28.2 scfm,
and during the hot-start run was 27.2 scfm.  These carburetor air rates
are converted to exhaust-gas flow rates, including water vapor, by multi-
plying by a factor of 1.07.  Thus, the average exhaust gas  flow during  the
cold-start modified IA-4 driving cycle was 28.2 x 1.07 = 30.2 scfm.  This
value represents a tunnel dilution ratio of 30 for a  tunnel flow of 905 cfm.
Measured variations of engine air flow with road speed and  of air-fuel  ratio
with engine air flow are given  in the Appendix, pages A-4  to A-6.

                            Choke Operation

          It was necessary to repeat for each run in a series  the  same
choke opening schedule because it was found that choke operation influenced
strongly the particle emissions.  In addition,  slower choke opening  than
would normally occur at laboratory ambient temperature was  needed  in
conjunction with the programmed throttle controller to reduce  the  chance
of stumble and stall in the first minute or so, which occurred with  the
regular vehicle choke.  However, decreasing the rate at which  the  choke
opens increased exhaust emissions, and the extent to which  the choke
schedule could be modified was limited by the maximum acceptable HC  and
CO composite (tunnel-bag) emissions from the cycle.   The tunnel-bag emissions
considered acceptable for the 1971 project cars on the LA-4 driving
schedule were:  4.6 g/mile HC, 47.0 g/mile CO,  and 3 g/mile NO.   The
small amounts of particulate matter generated in the single modified
or standard LA-4 cycle required that these limits be approached closely
in order to collect weighable amounts.  Four different choke schedules
were used in the course of the experimental program to accommodate
operating requirements and other limitations.  Details of the  experimen-
tal development of 'acceptable choke operation are given in the Appendix,
pages A-10 to A-17.

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                            Dilution Tunnel

          A dilution tunnel simulates the real environment by inducing
rapid dilution of the exhaust as it issues from the tailpipe.  Mixing with
constant proportions of filtered atmospheric air under reproducible experi-
mental conditions permits accurate sampling of the dilute mixture (usually
diluted 30:1).  The dilution tunnel used in these studies was constructed
according to the design developed at the Du Pont Petroleum Laboratory   .
The dilution tunnel residence chamber, and sampling apparatus are shown in
Figure 1, page 3.  Details of configuration, operation, and arrangement of
auxiliary apparatus are given in the Appendix, pages A-18 to A-32.

                           Residence Chamber

          A rectangular residence chamber with flexible walls of black
polyethylene sheeting on a supporting frame was used to contain a composite
sample of the diluted exhaust taken from the tunnel and further diluted by
filtered air in the chamber.  The overall dilution of the exhaust by tunnel
and chamber air was nominally 300:1, and the volume of the twice diluted
sample was about 2100 cu ft.  Details of the sampling probes, procedures for
mixing and sampling, and measurement of dilution ratio in each run are
presented in the Appendix, pages A-32 to A-42.

                            Instrumentation

          A critically important part of the facility are the instruments
for indicating and recording the composition of samples of exhaust and
diluted exhaust, the ambient conditions, the operation of the cars,  and
the characteristics of the particles suspended in the exhaust gases.  All
instruments were selected with the objective of providing reliable and
accurate analyses, checked periodically, given maintenance service as
necessary, calibrated before each run, and then checked after each run to
(1)  Habibi, Kamran, "Characterization of Particulate Lead in Vehicle
     Exhaust-Experimental Techniques", Environmental Science and Tech-
     nology, Vol. 4, No. 3, March 1970, pp 239-253.

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insure against unacceptable performance.  Measurement techniques were
evaluated and improved when possible throughout the experimental program.
The carbon monoxide meter indicated carbon monoxide concentrations lower
than the true values for Runs 4-11 to 4-26, (Table A-4), so that the cars
Lad CO emissions above the limits specified for the modified LA-4
cycle.  Experimental data in this report give the true values for carbon
monoxide concentration, corrected to compensate for the instrument: error.  The
series of runs was repeated under conditions to give acceptable CO emissions,
so that two sets of valid data were obtained for interpretation.
          Three different oxygen meters of one type were used in the first
half of the test program with recurring difficulties in achieving reliable
operation and rapid response.  After investigation a different type was
substituted and used with completely satisfactory results.
          In ten runs  the size distribution of the aerosol particles in
diluted exhaust in the residence chamber was measured with the Minnesota
Aerosol Analyzing System  (MAAS), a group of prototype instruments which
quantitatively characterize aerosol particles in submicron size ranges
and at low concentrations not accessible to other quantitative methods of
measurements.  Appropriate calibration procedures to standardize the data
have not yet been worked  out, so that the results given in this report are
interpreted in relative terms to indicate the changes that occur in size
distribution during aging of an aerosol by interaction of the particles with
each other and with the walls of the residence chamber.
          Two speed controllers were used during the experimental runs for
automatic control of  the  driving cycle after the car was placed in gear.
The first instrument was  programmed by a punched paper tape, which was less
precise  than  the magnetic tape program used in the later instrument, which
resulted in a marked  improvement in reliability and reproducibility.
          Specific details of the  instruments used and the calibration pro-
cedures  are given in  the  Appendix, pages A-42 to A-47.

                        Filtration and Weighing

          The mass concentration of solid particles in auto exhaust was
measured by  passing a measured volume of the diluted exhaust from the tunnel

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                                  10
through an absolute filter.  If the filter retains only  solid particles  on
its upstream face and passes all gaseous components,  the  increase  in
weight, AW, of the filter  is then the weight  of  suspended particles collected
from the filtered sample.  AW is used to calculate the emission  rate,  R,  of
the car, as follows:

                       R =  AW     x V(tunnel)
                           D(IA-4)    V (sample)

          where  R is  the  rate of  solid  emissions,  g/mile

                 AW is the  weight  gain of the  filter  when a
                 constant  sample stream  is  maintained during
                 one LA-4  cycle

                 D is  the  distance  driven during  one  IA-4 cycle,  7.5 miles

                 V(sample)  is  the  rate of flow through the filter
                 of a  sample  stream from the  tunnel,  cu ft/min

                 V(tunnel)  is  the  rate of flow of diluted exhaust in
                 the dilution  tunnel, cu ft/min.

          Ideally, sampling for particulates  should  be done isokinetically,
i.e.,  the flow velocity entering the sample probe should  be equal  to  the
flow velocity in the  tunnel.  To accomplish this, the ratio rr?	;—r-
            J                         v          '           V(sample)
should equal the ratio of  the cross-sectional areas  of the  tunnel  and
the sample probe.  However, when dealing with particulates  in the  sub-
micron range such as  normally found in auto exhaust,  large  deviations
from isokinetic  sampling can be tolerated  (such  as 10 to  1) without
appreciable effect on the  collection efficiency^ ' .   The  deviation
from isokinetic  sampling,  expressed as a ratio (Sampling  Ratio)  is given
by  the following equation:
 (1)  "Subisokinetic  Sampling  of  Particles  in an Air  Stream",  G.  A.  Sehmel,
     AEC Contract  No.  AT(45-1)-1830,  Battelle-Northwest, March  1,  1966.

-------
                                   11
             .,   . .    „          Actual  Sample Velocity
             Sampling Ratio = Isokinetic Sample Velocity   =

                    V(sample)    Area (tunnel)	
                    V(tunnel)    Area (sample probe)

The sampling ratios  actually used in this program were 1.3 for the
tunnel-to-chamber sampling, and 2.2 and 6.5 for the particu'late sampling
from the tunnel.
          Experience  in  this study and  discussions with other  investigators
have indicated  that  the weight change of a  filter  after  filtration  of dilute
samples  of  auto exhaust  can  be  affected by several experimental  variables,
such as  the size of the  sample  line, the temperature  of the  sample  stream
at  the  filter,  the  face  velocity  of  the sample stream,  the  size  and type of
filter,  and the gross weight of filter  relative to the weight  of solid  par-
ticles.  Thus  the  real system used in  these studies has required a  major
experimental study  to develop and specify  procedures  that  give a true value
of  AW.
          This study has necessarily dealt with very  small weights  of
collected particulate matter because of relatively large dilution  ratios of
about 30:1  in the  tunnel and about 300:1 in the residence  chamber.  The size
of  the  samples has  been  limited by controlling the flow rate through the
filter  to avoid excessive pressure drop,  and by the short  sampling  time of
23  minutes  during  one LA-4 cycle.  The  weights of particles  collected have
ranged  from a  few milligrams down to less  than a  hundred micrograms.  Par-
ticles  were collected on two sizes of  filters  which weighed  about  500 rag
in  142-mm diameter, and  about 70  mg  in 47-mm diameter.  A  standardized
technique had to be developed to measure weight gains that truly represented
 the amounts of solid particulate matter removed from  the  filtered  air.
The following requirements were included in the standard  technique after
development studies were completed.
           •  Microbalance with a sensitivity of better than 2  ng
           o  Control of atmospheric  temperature and humidity in
              the weighing area

-------
                                   12
          »  Selection of abrasion resistant filter  material
          •  Checks  on operator technique by reweighing items  of
             constant mass
          9  Discharge of static electricity from filters  before
             weighing
          e  Duplicate simultaneous samples to detect and  eliminate
             uncontrolled variables
          9  Parallel samples  with two different membrane  filter
             materials to detect any effects of filter medium
             composition
          a  A backup  filter  held in the same filter holder  in
             contact with the  primary filter and weighed after
             exposure to the same sample conditions, but without
             collection of the solid particles retained by the face
             of the  primary filter.  The weight change of the  back-
             up filter is applied as a correction to the weight
             change  of the primary filter.
          The use of a backup  filter is an important feature of the pro-
cedure used in these CRC studies.  The data that support its  use  are reported
in the experimental  section.  Details of application of other parts of the
standard  technique  itemized above  are given in  the Appendix,  pages A-47  to
A-51.

                          EXPERIMENTAL RESULTS

                         Exhaust  Emission  Rates

           The  results  of two  series  of  runs are  summarized in Table  1.
These were carried  out  to examine  reproducibility of  the  emissions with  un-
leaded and leaded fuels.   In  the first  series  (Runs 4-11  to 4-26)  a  low
reading caused by a malfunction in the  electronic circuit of  the CO  analyzer
permitted the  actual gaseous  emission levels of CO  to be unintentionally
higher than  the  limits  specified for  the  LA-4 cycle of 47.0 g/mi CO.
All  data  taken while the CO analyzer was  malfunctioning have been corrected
in Table  1 to  give  the  real values  during the  tests.

-------
                                  TABLE 1.   SUMMARY^F  TEST RESULTS
Run
Date
4-4
4-6
4-7
4-9
4-10
4-11
4-12
4-13
4-16
4-17
4-18
4-19
4-24
4-20
4-25
4-26
5-9
5-10
5-11
5-14
5-15
5-16
5-17
5-18
5-19
5-21
5-22

Car
Fuel
Cycle
Test Conditions
Car Fuel
W
W
W
W
W
W
W
W
W
W
B
B
B
B
B
B
B
B
B
W
W
W
W
W
W
B
B

W -
NL -
LA-4
NL
NL
NL
NL
NL
NL
NL
NL
NL
NL
L
L
L
L
L
L
L
L
L
NL
NL
NL
NL
NL
NL
L
L

White
Cycle
LA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (M)
IA-4 (tf)
IA-4 (M)
IA-4
IA-4
IA-4 (M)
IA-4 (M)

B -
Nonleaded L -
(M)
Schedule
I
I
I
I
I
I
I
I
I
I-S
I
I
I
I
I
I
II
II
II
II
II
II
II
II-S
II-S
II
II

Blue
Leaded
General Comments
Checkout
Checkout
Checkout
Checkout
Checkout
High HC, CO
High HC, CO
High HC, CO
High HC, CO
Std. Cycle
Checkout only
Abort >d
Aborced
High HC, CO
High HC, CO
High HC, CO
Baseline
Baseline
Aborted
Aborted
Baseline
Basel-.ne
Basel-. ne
Std. C/cle
Std. Cycle
Basel .ne
Basel-Lie
KEY
Emissions, e/mi
Part.
--
—
0.192
0.173
0.195
0.189
0.041
__
--
--
0.319
0.349
0.340
0.135
0.153
__
—
0.040
0.046
0.044
0.075
0.071
0.211
0.203

HC
--
—
5.81
5.96
6.13
6.22
3.12
_..
—
—
6.07
5.94
5.76
3.91
5.35
.._
—
3.43
3.56
3.99
4.66
4.12
3.37
3.46

Particular +



Cycle with 55 -second initial idle
CO
--
—
68.8
73.9
72.5
77.7
58.6
__
--
—
71.9
68.2
75.8
34.1
47.4
__
—
35.5
33.2
38.5
52.4
46.8
38.2
44.1

Based on
weights
Sampling
f t%e+ ff»t* a T
NOV
—
--
2.46
2.53
2.88
2.91
2.72
__
—
—
1.99
2.06
1.90
2.60
2.21
_-
—
2.35
2.48
2.50
2.47
2.49
2.19
1.93

Metric'
only,
Ratio
wo t r» r>
Schedule
           LA-4
Cycle with 20-second  initial  idle
Choke plate opening schedules defined
  on Pages A-14 to A-17
         isokinetic velocity)"
         2.2
NO -H-  Not corrected  for humidity

-------
                                  14
          Rather than use only the data with relatively high gaseous emission
levels as baseline data for particulate emissions, new Choke Schedules II
and II-S described in the Appendix (pages A-16 to A-17) were developed to
lower gaseous emissions to acceptable levels.  The baseline runs were
repeated with modified LA-4(M) standard LA-4 cycles (Runs 5-9 through 5-22).
These included a consecutive pair of baseline runs with the modified IA-4 (M)
cycle on leaded fuel, a consecutive series with the modified cycle on un-
leaded fuel, and a consecutive pair using the standard IA-4 cycle with un-
leaded fuel.

           Reproducibility of Mass of Particulate Emissions

          Samples of diluted exhaust were taken from the downstream end of
the tunnel and from the residence chamber during each of the ten Runs 4-10
to 4-26.  Particles filtered from the samples were collected on two types
of membrane  filters.  All samples used two filters assembled together in
the same filter holder as a primary and a backup  disk, according  to the
procedure described previously, to distinguish adsorbable vapors in the same
stream.  Each type of filter was used in duplicate filter holders and fil-
ter assemblies, so that four sample streams were filtered altogether.
          Table 2 shows the mass of particles collected from the tunnel
for each of  the valid baseline Runs 4-11 to 4-26, and for each of  the filter
types to permit comparison with each other and with the gaseous emissions
in the exhaust.  Mean values and standard deviations are given for each
filter type  and each fuel.  These comparisons show good agreement between
filters and  good reproducibility of particle emissions in repeated runs with
the modified cycle,,  Emissions from the single run with the standard cycle
are significantly lower than the emissions from the modified cycle.
          Table 3 presents emissions data of Table 2 recalculated as mass
concentration of particles, and includes the mass concentrations of par-
ticles sampled from the residence chamber immediately after a tenfold
dilution and mixing of the tunnel sample, and after aging of the mixture
for about 3-1/2 hours.  The means and standard deviations, and coefficients
of variation (CV, 7<>) of each group of samples have been calculated for the
modified LA-4 cycle operated with unleaded and lead fuel, using the two

-------
                                    15
             TABLE  2.   MASS  EMISSIONS OF PARTICLES COLLECTED
                       FROM  TUNNEL BY FILTRATION
                       (Composite samples,  dilution ratio,  30,
                       one cycle, cold start)


Emissions, g/mi

Particles on
Filter Type
Run No. Fuel Cycle
4/11 RE-141B Modified
Unleaded IA-4
4/12 Ditto Ditto
4/13
4/16 " "
Mean
4/17 " Standard
LA-4
4/20 RE-141C Modified
Leaded IA-4
4/25
4/26
Mean
MET(a)
.192
.173
.195
.189
0.188 * .009
.041
.319
.349
.340
0.337 * .019
MIL(b^ CO HC
.204 68.8 5.81
.178 73.9 5.96
.214 72.5 6.13
.208 77.7 6.22
.201 * 0.014
.043 58.6 3.12
.285 71.9 6.07
.360 68.2 5.94
.386 75.8 5.76
.344 * 0.044
NO
2.46
2.53
2.88
2.91
2.72*
1.99
2.06
1.90
(a)  Metricel Filter DM450, Part No. 64519,  Batch  80557,  142-mm,  0.45//m pore
      Flow 4.29±  .10  cfm (Isokinetic flow rate 1.95 cfra).

(b)  Millipore Filter AAWP 047 00 Lot 66499  15, 47 mm,  0.8 X-'m pore.
      Flow 0.70 cfm (Isokinetic flow rate 0.11 cfm). '

-------
TABLE 3. MASS CONCENTRATIONS OF PARTICLES COLLECTED FROM
         TUNNEL AND RESIDENCE CHAMBER
Run
4/11
4/12
4/13
4/16
Mean
CV, pc
4/17
4/20
4/25
4/26
Mean
CV, pc
Variables
Fuel Cycle
Clear Modified
141B
Clear Modified
141B
Clear Modified
141B
Clear Modified
141B

Clear Standard
141B
Lead Modified
141C
Lead Modified
141X3
Lead Modified
141C


Net
Tunnel
Composite
MET
2458
2208
2500
2419
2389 ± 145
6.0
526 ± 11
4090
4460
4362
4304 ± 85
2.0
MIL
2600
2297
2753
2680
2582 ± 167
6.5
550 ± 28
3673
4638
4961
4432 ± 586
11.
^\
Particulate Mass, g/m
Residence Chamber
Initial
MET
215
409
302
227
255 ± 113
44.
98 ± 16
390
448
392
415 ± 34
8.
MIL
317
197
394
266
293 ± 71
28.
—
386
481
368
409 ± 66
16.
Aged 3
MET
356
182
248
224
247 ± 74
30.
79 ± 6
304
348
313
324 ± 24
8.
-1/2 hr
MIL
__
340
336
249
308 ± 64
21.
--
313
367
436
372 i 108
29.

-------
                                  17
types of filter paper.  All entries in Table 3 are the mean of the net
weight increase of duplicate simultaneous samples, each of which  used two
filters in a single holder.  The weight change of the backup  filter was
applied as a correction to the particle weight collected on the primary
filter, as described above (page 11).
          These experimental data demonstrate the following characteristics
of the specified method of filtration:
          9  The coefficient of variation (CV) of the mean
             particle mass from the tunnel was about 6 percent
             for both unleaded and leaded fuels,
          9  There is no significant difference between the
             two comparable means of the masses on  the  two  types  of
             filter paper  from both the tunnel and residence
             chamber, even though the filter composition,  area, face
             velocity, and total sample weight and volume for
             the two  filter systems differed markedly.
          •  The backup  filter provides a correction that
             eliminates uncontrolled variability related to face
             velocity at the primary filter, gaseous composition  of
             the exhaust,  and equilibration of the filter samples
             before weighings.
          •  The coefficients of variation of the residence
             chamber  samples were higher than those of
             samples  from  the tunnel, because of the much
             smaller  sample from the residence chamber.
          «  The mean values of the initial residence chamber
             samples  were  each  in the expected range of 10
             percent  of  the corresponding tunnel sample,
             agreeing with the  tenfold dilution of  the
             tunnel  sample determined by gas analyses for
             CO and  hydrocarbons.

-------
                                   18

               Correlation of Light Scattering with Mass

          Light scattered by the aerosol in the residence chamber was
measured with an integrating nephelometer initially and after aging of the
particles to determine the correlation of the light scattering coefficient
with the mass of the suspended particles.  Table 4 gives the light scattering
coefficients and the mean mass concentrations of samples weighed on  two
types of filters for each of Runs 4-11 to 5-22.  Figure 2 gives a plot of
                              3            4
the straight line MASS in u-g/m  = 65.5   (10  bt - 0.4) that was calculated
for minimum standard deviation  (a = 0.59) of residuals of all points.  The
intercept at b     = 0.4 is the measured background scattering of filtered
              scat
air in the chamber.  Correlation coefficient R of MASS with ^scat is 0.91.
There is no apparent systematic influence of particles from either fuel
type or aging -because points  in all categories  fall around  the  regressed line,
The correlation of auto exhaust light scatter measured in this study
                                                    (1)               4
differs substantially from the Charlson correlation    MASS = 38 x 10
b     for atmospheric dust, which is also shown in Figure 2.  Charlson has
 scat
found no deviations from his empirical experimental correlation, but he
points out that it "may or may not hold in all cases",  This is an instance
in which either the light scattering of auto exhaust is less  than for
atmospheric dust,  or the mass  measured by filtration of exhaust  according
to the methods described above is greater than would be found by filtra-
tion of atmospheric dust with the same scattering coefficient.   More
investigation is necessary, but the empirical relation for auto  exhaust
may be useful before an explanation is found.

                 Addition of Foreign Materials  to the
                           Residence Chamber
          Following the development of procedures and some shakedown runs,
Runs 12-6 to 1-15 were carried out as summarized in Table 5 to investi-
gate the effects of humidity in the chamber, lead in the fuel, dust and
(1)  Charlson, R. J., Ahlquist, N. C., Selvidge, H. and MacCready,  P.  B.,  Jr.,
     Journal Air Pollution Control Assoc.,  Vol. 19, pp 937-942 (1969).

-------
                                    19
            TABLE 4.   CORRELATION OF LIGHT SCATTERING WITH AEROSOL
                      MASS IN THE RESIDENCE CHAMBER
Run
4-11
4-12
4-13
4-16
4-17
4-20
4-25
4-26
5-15
5-16
5-17
5-18
5-19
5-9
5-10
5-21
5-22
Fuel
Clear
141-B
Ditto
M
ii
"
Lead
141-C
Ditto
11
Clear
141-B
Ditto
ii
it
it
Lead
141-C
Ditto
11
M
LA-4
Cycle
Modified
Ditto
ti
11
Standard
Modified
Ditto
11
Modified
Ditto
it
Standard
Ditto
Modified
Ditto
"
11
h -4 -1
scat (10 m )
Initial 3-1/2 hrs
5.0
4.6
5.5 1.8
5.5
1.5
6.0
7.2 6.9
6.4 6.2
1.4 1.1
1.3 1.4
1.2 1.2
1.9 2.1
2.1 1.7
1.8 2.0
2.8 3.2
2.4 2.2
2.6 2.7
Mass, y,
Initial
266
306
348
247
98
388
465
380
84
70
50
95
120
138
173
197
233
g/m
3-1/2 .hrs
--
--
292
--
--
--
358
375
--
49
19
56
98
133
--
145
135
Nominal  sample  flow  rate  from  tunnel  to  chamber  = 10.0  cfm,  isokinetic  flow
•rate  = 7.5  cfm.

-------
                                 20
 o
 o
c
0)
'o
o>
o
O
o>
t
o
o
CO
                 100
200
300
400
500
600
                        Mass  Concentration,  /xg/nrr
             FIGURE 2.  CORRELATION BETWEEN LIGHT  SCATTERING
                        AND AEROSOL MASS CONCENTRATION

-------
TABLE 5.  STUDIES OF ENVIRONMENTAL VARIABLES
Run
Tvst Conditions
D«-.{» Car
12-6
12-13
12-15
12-18
12-19
12-20
12-21
12-22
!-]7
1-19
!-23
12-27
12-28
12-29
J-3
1-5
1-10
1-11
1-12
1-15
W
W
W
W
W
W
W
W
W
W
W
B
B
B
0
B
B
B
U
B
Fuel Cycle Sc
XL
Nl.
VI.
Nl.
NL
NL
NL
Nl.
NL
Nl.
NL
1.
L
1.
L
!_
L
L
L
L
I.A-'UM)
I./1 -4 'M)
f.A--; (M)
LA-4 (\'l
I.A-4 (M)
LA--I IM)
LA-.J(M)
I.A-t (M)
I.A-'I(M)
l.A-4 (V.)
I.A--KM)
f.A-4(M)
LA-4(M)
LA-4 (M)
l,A-t(M)
I.A--1 (M)
LA-MM)
LA-! (M)
l.A-1 (M)
LA-4 (M)
Module c:on!ro!lct MAAS
UD DPC
uc :>if:
(JD Dfc:
L'D WC.
\ WO
! IJpiJ
i nn:
I DPC
t Rl
'. IU
1 Kl
t DfC
I I>PC
i DPC
I Rl
1 IU
t m
i m
1 Rl
I Rl
Yes
No
Yes
Ycv
No
No
No
Yes
Wo
No
Yes
Yes
Yes
Yes
No
No
No
No
Yes
Yes
C.enetal Comments Hum.
0
So.ik ;eoip low - Nllj erratic O
O
So.ik remp lew O
CS c'lnnxc.-! -• low CO lOle O
O
A
A
O
A
O
Various problems A
R'jn-ln mileage low O
O
Run length low. Idle CO low A
Soak time short A
Soak short, soak temp low A
Idle CO lilg'.i, soak temp low O
Soak temp low O
A
Variables Emissions. >;/mi
Lead
0
O
O
0
O
O
O
O
O
O
0
3
B
B
B
B
B
B
B
B
Dust NU3 Part* IIC
O O 0.011 1.08
O D 0.011 1.70
O O O.OM 2.06
O D 'O.OIR 1.63
O D O.OO'.l 1.73
C O Dust 1.70
O D 0.014 1.89
C O Dust 1.84
O D 0.038 7.69
C 1) Dust 1.0:i
C D Dus: 1.40
C O Uust
C O Dust 5. US
O D 0.255 6.05
C D PuM 4.?2
O O O.iMl 7.'J3
O D 0.2C» 6.33
C D Dust 3.34
O O 0. 1G2 4.04
O O 0. IC4 5.3U
CO
.1.!.
2r».
"2.
27.
2-1.
23.
36.
33.
32.
31.
2f.
--
58.
7).
3-1.
53.
•17.
33.
41.
3J.
3
8
I
ft
3
9
n
0
C
7
2

1
6
0
1
7
4
1
0
NO
C.H-
2.7S
2.4P
2.S2
3.23
3. 12
2.25
1.71
:.45
1 . ;i '.
1.30
2.13
2.17
--
C. 53
--
2. i:
l.'-'ii
1.19
1.3S
At this point the cars were leak checked and a small leak waj found In the white car and a very small

Car
Fuel
Cycle
Choke
leak




In




Schedule

NO



















the blue car.
W - White
NL - Nonleaded
LA-4(M)

UD
I
Nitrogen oxide






B - Blue
L - Leaded
Cycle with




55 -second


Controller

initial idle Humidity
Partlculate

DPC
Rl
(SI)
+
Under development
Defined In
- Values not





text
corrected





Variable*
for humidity





0
A
B
C

D


Magnetic tape
Paper tape
Steam injection
Based on Metricel weights
Sampling Ratio "2.2
Low or normal values
High humidity
High lead
High dust (solid impurity
In atmosphere)
High ammonia (gaseous
Impurity In atmosphere)




f



































-------
                                   22
ammonia in the atmosphere, on the nature and fate of particles from the
two matched cars.  Residence time in the chamber was an independent
parameter which was varied from about 1 to 24 hours.
          Because the weighing procedure in the early stages was not as
precise, and because of some operating malfunctions, the data are useful
and valid only for interpretations given in following sections; broader
interpretations should not be attempted.  Subsequent runs with more
definitive results have already been described in Table 1.

              Size Distribution of Auto Exhaust Particles
                       with the Cascade Impactor

          No significant data on cumulative mass as a function of particle
diameter were obtained when particles carried in the exhaust were separated
into aerodynamic equivalent diameter  fractions by  passing a  sample  stream
through six stages of the Battelle cascade  impactor backed  up  by an ab-
solute  filter.   The aerosol suspensions were  too dilute  and  the  time avail-
able for sampling was too short  to build  up weighable amounts  of each
fraction on individual  impact  stages.  All  stages  gained'weights in the
range of a few  to  tens  of micrograms,  presumably because there was  ad-
sorption of volatile material  as well  as  collection of  solids  by impact.
Electron micrographs of collections  on the  impactor surfaces  showed the
particles were  being classified  by size.  The morphology of particles  in
some of the size fractions  is  illustrated in  a  subsequent section.
         The  absolute filter,  which  retained  unfractionated  undersize  with
an equivalent diameter  less than  0.25  M-m, collected amounts  of material
weighing several hundred micrograms.   Thus  the  predominant  particles are
in the  size range  below 0.25 p,m.
                 Size Distribution  of  Particles with  the
                   Minnesota Aerosol  Analyzing System
          The Minnesota Aerosol-Analyzing System (MAAS) was used in ten
 tests, five with unleaded fuel and five with leaded fuel, as shown in
 Table 6.  Size distributions indicated by MAAS for one selected run with
 each fuel are plotted  in Figures 3 and 4.

-------
TABLE 6. COMPARISON OF AUTOMOBILE PARTICUIATE DATA



Filtration
Mass Concentration,

Test No.
11-29
12-1
12-4
12-6
12-15
12-13
12-18
12-19
1-17
12-21
12-22
1-23
12-20
1-19
1-5
1-15
12-29
1-12
1-10
12-28
1-3
12-27
1-11
Foreign
Material
(a)
(a)
(ae)
(o.)
(o)
(d)
(d)
(d)

(ad)
(ac)
(cd)
(ce)
(acde)
(ab)
(ab)
(bd)
(be)
(abde)
(be)
(abed)
(abce)
(bcde)

Tunnel*
480
230
172
290
176
137
169
121
492
183
3360
1869
1645
1608
3088
2100
3260
2070
3450
6194
4780
20,240
4818
Residence
Initial**
—
72.5
42
27
37
38
24
10
91
25
152
-
94
—
233
120
271
186
177
331
246
1066
221

U8/m
Chamber
4 Hours
—
50
-
18
40
33
6
37
40
14
81
-
85
—
236
145
213
135
145
222
267


Light Scattering
b -A W1
scat (10 m ),
Initial 4
fm
2.6
2.9
0.82
0.95
0.70
0.65
0.52
0.65
0.65
3.8
3.6
2.5
3.3
5.7
2.4
5.5
1.9
4.7
7.4
5.0
Hours
^
1.7
2.6
0.85
1.0
0.80
1.10
1.15
0.65
0.75
2.6
2.7
2.2
2.3
5.1
2.5
4.6
1.8
4.5
5.4
3.7
16.8 13.6
238
(a) High humidity.
(b) Leaded
(c) Arizona
(d) Ammonia
gasoline.
road dust



4.25
+ Sampling
++ Sampling
3.3
Ratio
Ratio

MASS Instruments

Particulate
Initial
—
61
386
-
36.4
-
19.7
-
-
-
1152
-
-
-
_
262
697
264
_
1228
-
2786
^
= 2.2
= 1.3
2
Vol. UJP /cc
4 Hours
•»
30
24i
-
35.9
-
68.5
-
-
-
356
-
-
-
_
163
422
202
_
476
-
1307
*™


contaminant.
gas contaminant.
(e) Long residence time.
(o) Represents all variables at
low level.





                                                                                  NJ
                                                                                  CO

-------
u
o
s
:*.
c
o
.Q

t_

to

<5
O
                Test 12/15/72
               i    i  i  i  i  : : i

                Unleaded Fuel
     10
      0

      0.001
0.01
10.0
                                           Particle Diameter, p.rr\
                      FIGURE 3.  VOLUME DISTRIBUTION)? UNLEADED PARTICLES

-------
 o
 o
 
-------
                                   26
          Figure 3 (Run 12-15) shows the results obtained with unleaded
automobile exhaust with no addition of any contaminant or humidity.  The
distribution changed little in 3-1/2 hours except for the removal of the
very large particles and some growth in the small particles.  Figure 4
(1-12) similarly shows some slight changes in 3-1/2 hours for the size
distribution of leaded exhaust particles.  The curves are similar in
shape but differ greatly in the total volume of the two aerosols, since
the ordinate scales differ tenfold.  These are two single runs made
with different choke schedules, so that the emissions found are not
comparable as a typical difference in emissions from unleaded and leaded
fuels. Multiple runs in each car under entirely similar controlled
conditions must be made to obtain a significant comparison.  The relative
measurements of particles from unleaded and leaded fuels found by filtra-
tion and by MAAS instruments are sufficiently similar to encourage the
use of both methods in detailed studies of the amounts and properties
of particles.

                 Correlation of Particulate Mass with
                         Hydrocarbon Emissions

          A correlation was found between the mass rate of particle
emissions and total hydrocarbon emissions, which is plotted as the curve
in Figure 5 for unleaded fuel.  The plot includes all of the data from
all experiments (except dust injection runs), and one datum from an API
study at Battelle with a so-called "warm start".  The correlation is
truly remarkable for unleaded fuel considering the many other parameters
being varied.  The leaded data do not correlate as well, particularly
the three high humidity runs marked B, but the trend appears similar to
that for the unleaded curve.  The particulate emissions from the leaded
fuel are from 0.05 to 0.15 g/mile above the nonleaded curve, or from
60 to 100 percent higher when compared at the same hydrocarbon emission
level.
          The reproducibility of the measurements of emissions in six
sets of consecutive replicate runs was ±6.4 percent for particulate
emissions and ±10.0 percent for gaseous emissions, expressed as the

-------
                        27
 o    Modified cycle, unleaded fuel
 A    Standard  cycle,   "
 a    API,
 •    Modified cycle, leaded fuel
I, IE  Choke schedules
                     345
                HC Emissions, g/mi
FIGURE 5. CORRELATION BETWEEN PARTICLE EMISSIONS
          AND HYDROCARBON EMISSIONS

-------
                                   28
unweighted mean of the percentage standard deviations of each set.  These
include all of the data on emissions in Table 1, page 13, except the
single run on 4-17.   Reproducibility after a longer period, such as
10 days between the duplicate pairs of Runs 5-9 and 5-10 and Runs 5-21
and 5-22, was not as good.  This is the only such set of two pairs
available for comparison, which precludes interpretation and definite
conclusions.

              Morphological Characteristics of Particles

          Exhaust particulates were collected by means of the cascade
impactor directly onto electron microscope carbon support films on
electron microscope grids.  Without further specimen preparation the
particles were examined in the transmission electron microscope.
          In general, the same types of particles are seen, independently
of the fuel used and the conditions of generation; agglomerates and
aggregates are comprised of carbon black type material, condensate,
and spherical fly-ash-like particulate matter.  Figure 6 shows typical
unleaded exhaust particles; there are several tar droplet particles
which have low enough vapor pressure to persist in the vacuum system of
tine electron microscope under bombardment by the electron beam.  Also,
there is usually present a carbon-black-type structure of a chain-like
aggregate, and fairly electron-dense particles which are cemented
together with less dense material, which appears to have condensed
around them.
          Figure  7  shows  an electron micrograph of leaded auto exhaust.
Carbon black and fly ash are cemented into aggregates by material which
appears  to have  condensed around them.   In some of the small aggregates,
highly electron-dense structures are in evidence and probably are lead-
rich.
          Figure  8  is a group of four electron micrographs of unleaded par-
ticles from the  residence chamber collected by the impactor in the two
smallest stages, initially and after four hours of aging.  The 0.25 um
stage  has brushy and chain-like aggregates and many very small individual
particles.   After  aging many more aggregates of a few particles each are
visible.  The initial sample at 0.5 M.m is mostly spherical structures,
several  aggregated from three or four units.

-------
                              29
J22216                                              10,OOOX

FIGURE 6.  AN ELECTRON  MICROGRAPH OF UNLEADED EXHAUST
           PARTICULATE  COI.LKCTED AT TUM 0.5-Um 1MPACTOR
           STACF, AFTKK  4  HOURS RFSIDMNCE (Run 4-17)
 J22219                                             10.000X
 FIGURE 7,  AN ELECTRON MICROGRAPH OF LEADED EXHAUST
            PARTICULATE COLLECTED AT THE 0.5-p.m 1MFACTOR
            STAGE AFTER 4  HOURS  RESIDENCE (Run 4-25)

-------
                                    30
O.Z5>UM COLLECTION
0-HOUK5
                    COLLECTION
                                                                0-HOURS
                                 \.0/U,M
                                .	1
  /£5>UM COLLECTION
  JZttT!

4-HOURS
                0.5MM COLLECTION
                                                                4-MOORS
            FIGURE  8.  ELECTRON MICROGRAPHS SHOWING NONLEADED
                        EXHAUST PARTICULATE FROM  RUN 12-15

-------
                                   31
         Figure 9 is another group of four views of particles from leaded
fuel, not significantly different in shape and degree of aggregation from
the unleaded particles of Figure 8.
         Figure 10 shows four individual views of particles from the
residence chamber with foreign materials also present.  The dust con-
taminant added in Run 12-20 with unleaded gasoline persists for 20 hours
of aging, and exhaust particles are not distinguishable from the dust.
The presence of alkaline ammonia in the diluted exhaust of Run 12-13 from
unleaded gasoline causes the growth of needles.  A condensate  layer appears
to enclose aggregates of aged particles in  the high humidity chamber at-
mosphere.


                              CONCLUSIONS

Emission Levels

          (1)  Particulate emission levels correlated very strongly
with HC  (and CO) emissions for the two fuels.  For unleaded fuels, the
level of hydrocarbon emissions appears to be the major significant
factor correlating positively'with particulate emissions.
          (2)  "The same choke schedule resulted in significantly different
HC (and CO) emission levels for the two fuels.
          (3)  The same choke schedule resulted in significantly
different weights of particulate emissions for the two fuels.
          (4)  For a given HC emission leaded fuel always gave higher
weights of particulate emissions.  For roughly equivalent gaseous
emissions, the particulates from the leaded fuel are about 50 to 100
percent heavier than from the unleaded fuel.
          (5)  The reproducibility of the emission data on consecutive
run days was a few percent.
          (6)  The determination of the particulate loading of the auto-
mobile exhaust is heavily dependent upon the characteristics of the
sampling system and, in order to correlate results from different labora-
tories,  there should not be any major differences in the filter media or
sampling procedure.

-------
                                      32
  0-HOURS
                           J2I834
COlLECnON
      ?  •.:*?
  tt-tWURS
     *,
               . *
               r ;
COLLECTION
0-HOOR5
         J21644
O.S^UM COLLECT10M
                        J27000
               05XIM COUeCTlON
                                  KEY
                        RUN
                       12-28
                RUN
                1-5
                        RUN
                       1-15
                RUN
                1-15
FIGURE 9,   ELECTRON MICROGRAPHS SHOWING  LEADED EXHAUST
            PARTICULATE FROM SELECTED  EXPERIMENTS

-------
LEADED GAGOUNt
tO>UM COLUCTKJM
NON-LEADED GASOUME     W HOURS
0.5,14 M COLLECTION           DUST
                                I 0/U.M
                                      NON-LEADED GASOLINE
                                             COLLECTION
                             .
  0-MOUR9
AMMONIA
                                           J21I99
                                         O-HOURS
                                        AMMONIA
                                                            AMOURS
                                                            HUMIDITY
                                  KEY
                       RUN
                      12-20
                         RUN
                        12-13
                       RUN
                      12-29
                         RUN
                         1-15
     FIGURE 10. ELECTRON MICROGRAPHS  SHOWING EFFECTS  OF  DUST,
                 AMMONIA,  AND HUMIDITY FROM SELECTED EXPERIMENTS

-------
                                   34
Particulate Characteristics

          (1)  Both the cascade impactor and MAAS (Minnesota Aerosol
Analyzing System) indicated little difference in the particle size of
the particulates from leaded or nonleaded gasoline.  For the most part,
the mass-median diameter of the dilute exhaust measured at the tunnel
(30:1) was less than one-quarter micron.  On the basis of the Minnesota
System, the particle size distribution appeared to be bimodal.
          (2)  High humidity in the chamber produced no apparent effect
on the size of the leaded particles; however, there was a considerable
increase in the size of the unleaded particles.
          (3)  Ammonia caused no apparent increase in the particle size
of the leaded particulates; however, there was a considerable increase
in size of the unleaded particulates.  Ammonia was the only additive to
cause an increase in the particulate mass in the chamber as a function
of time, and this effect occurred only for the unleaded particulates.
          (4)  The integrating nephelometer data for light scattering by-
the auto exhaust correlates directly with the mass data obtained by
filtration.  However, the slope of the correlation curve for auto exhaust
is greater than the slope of the correlation curve proposed by Charlaon
for atmospheric dust.

Morphological Analysis

          Four mechanisms of particle growth, listed in order of prevalence,
were identified based on morphological studies of electron micrographs of
the particles from both unleaded and leaded fuels.
          First.   Agglomeration
                   Almost every exhaust particle seen in the electron
                   microscope can be classified as an agglomerate.
          Second.  Condensation
                   Many of the particles are surrounded by low density
                   envelopes of what appears to be a condensate.

-------
                                   35
          Third.   Crystal Growth
                   Sometimes crystalline particles are detected, part
                   of which are associated with oil or tar droplets.
          Fourth.  Ablation of Deposits
                   Particles larger than one micron and irregular in
                   shape are likely to be chunks of material broken
                   off exhaust system deposits.
          The significant differences in particles from the two fuels
were that the leaded particles frequently had an electron-opaque core,
which undoubtedly represented a lead-rich nucleus;  that agglomerates
formed as a function of residence time; and that ammonia addition to the
suspension of unleaded particles drastically affected their structure.
The particles produced during runs in which ammonia was added to the
dilution tunnel were highly irregular acicular structures, while in
all other runs the particulates were generally spherical agglomerates.

-------
APPENDIX

-------
                                  A-l
                                 Fuels
                TABLE A-l.  CHARACTERISTICS OF FUELS
                                                     (a)
          Properties
                                                    Blend Designation

RE -14 IB
unleaded
RE-141C
Leaded
Research Octane No. (RON)
Motor Octane No. (MON)

Vapor Pressure, Reid, Micro (D-2551)
TEL as Lead, ppm (M-1059)
TEL as grams Pb/gal. (M-951)

Sulfur, % wt
Chlorine, ppm  (M-600)
Phosphorus, ppm (M-798)
Nitrogen, ppm  (M-1042, Col.)

API Gravity (D-287)
ASTM Distillation, °F
Initial Boiling Point
5% Distilled
10% Ditto
20%
30%
40%
50%
60%
70% "
80%
90%
95%
End Point
C, & Lighter, Gas Chroma tographic
D-2887(C)
-16
63
77
142
188
207
231
241
275
292
335
369
—
Analysis, wt - %
Propylene
Propane
Isobutane
Isobutylene +  Butene-1
n-Butane
trans-Butene-2
cis-Butene-2
3-Methylbutene-l
Isopentane
Pentene-1
2-Methylbutene-l
n-Pentane
trans-Pentene-2
cis-Pentene-2
Total Cs & Lighter
 93.6
 85.4

  9.0
  0.7
 (0.002)
  0.01
  0.08
  0.70
  0.07
  5.00
  0.07
  0.09
  0.06
 10.88
  0.16
  0.34
  2.56
  0.41
  0.22
(20.7)
100.0
 91.7

 10.6

  2.49

  (d)
Present
  1.
 21

 60.3
  0.01
  0.07
  0.69
  0.06
  5.02
  0.07
  0.09
  0.06
 10.99
  0.16
  0.34
  2.59
  0.42
  0.23
(20.8)

-------
          A-2
TABLE A-l.  (Continued)
Blend Designation^

Properties
C$ & Heavier, Mass Spec PONA, wt - %
Paraffins
Monoolefins
Cycloolefins & Diolefins
Monocycloparaffins
Dicycloparaffins
Alkylbenzenes
Alkylindanes & "tetralins
Alkylnaphthalenes
Total Cg & Heavier
Approximate Distribution of Alkylbenzenes by Mass
C6
c?
C8
C9
GIO
Cll
C12
Total Alkylbenzenes
Total Sample GC + MS PONA Summary . wt - %
Paraffins
Olefins
Naphthenes
Aromatics
Grand Total CG & MS
Distillation- Chromatoeraphic-UV Analysis
Benz (a )anthracene
Benso(a)pyrene
Re -14 IB
unleaded
/.O Q
*r .3 . O
3.9
0.6
1.6
0.2
27.5
•» l # *s
0.8
0.8
(79.3)
Spec, wt - %
1.8
6.9
9.0
6.8
2.2
0.8
0.1
(27.6)

63.1
5.9
1.8
29.2
100.0

3.3 ppm
r * ^^
1.0 ppm
RE -14 1C
Leaded
AO A
H J . w
4.0
0.6
1.8
0.2
27.2
0.9
0.9
(79.2)

1.7
6.5
9.1
6.8
2.2
0.8
0.1
(27.2)

63.0
6.0
2.0
29.0
100.0

(d)
(d)

-------
                                  A-3
Footnotes to Table A-l:
(a)  Data supplied by Mobil Research and Development Corporation.

(b)  Fuels RE-141B and RE-141C were prepared from a single 6000-gallon-
     lot which was composed of five blending components.  Those components
     which tend to be unstable in long-term storage had antioxidant and
     metal deactivator (grades approved for use in military gasoline)
     added at the refinery.

     Half of the 6000-gallon lot was put into clean drums and labeled
     RE-141B.  The other half had Tetraethyllead Motor Mix added and,
     after mixing, was drummed, then labeled RE-141C.  TEL Motor Mix con-
     tains ethylene dichlorlde (1.0 theory) and ethylene dibromide (0.5
     theory) according to the usual specifications.  No other additives
     were added during blending of either RE-141B or -C.

(c)  Simulated distillation by gas chromatography of RE-141B.

(d)  S, BaA, and BaP in RE-141C should be the same as that determined by
     analysis of RE-141B.

-------
                                  A-4
                         Air Flow Measurements

          Figure A-l shows measured engine air flow and road horsepower as
functions of vehicle speed from idle (at 0 speed) to 60 mph.
          Figure A-2 is a plot of air fuel ratio versus engine air flow
showing the carburetor flow curve supplied by Ford Motor Company (dashed
line) and the data calculated from tailpipe CO, CO , HC, and 0  measurements.
The two curves agree reasonably well up to 50 scfm (about 40 mph).   At
higher air flows the carburetor flow curve from Ford shows an air-fuel
ratio higher by almost 1 A/F number.  The reason for this is not known.

                            Car Maintenance

          In preparation for each run, performance of the cars was observed
and any necessary adjustment or maintenance was done.
          After checkout runs were completed the oil was changed, a new
oil filter and air filters were installed, points checked and cleaned,
timing and dwell checked on both cars, and a series of 17 experimental runs
(Runs 12-18 to 1-15) was completed.  Then, the exhaust systems of both
cars were pressure-tested at 1 psi for leaks.  On the unleaded-fuel car a
leak was noted at the joint between the Y-pipe and the muffler.  A much
smaller leak was noted at the same location on the leaded-fuel car.  Both
leaks were stopped by tightening the clamps.  The cars were then not used
for about 10 weeks while the data were examined in planning for the next
series.
          In preparation for the new series of runs the compression
pressures on each engine were checked under motoring conditions.  The
results were as follows in order of cylinder number:  unleaded-fuel car,
148, 158, 145, 146, 150, 155, 150, 150; leaded-fuel car, 155, 152, 150, 148,
133, 147, 150, 150.  The compression in cylinder No. 5 in the leaded-fuel
car is significantly lower than all other compression pressures.  However,
it is not low enough to indicate any major problem such as broken rings,
stuck or warped valve, or burned valve seats.
          Services on both project cars were:  oil change,  new oil and air
filters, new spark plugs, points checked and cleaned, timing and dwell

-------
                                   A-5
90
80
70
60
E
*4—

tf>

 f*


_g

u_
50
40
30
 10
 0
   0
                  10
                                         Air  flow
                                     	f
20         30         40

     Road Speed,  mph
                                                                    Hp
                                                                            20
                                                                            15
                                                                        10
                                                                                0)
                                                                                £
                                                                                o
                                                                                Q.
                                                                                
-------
o
or
o>



I
k-

<
                                                                                      Ford carburetor  flow  curve

                                                                                                8/6/70
                                                                                       BCL  carburetor  flow  curve

                                                                                                      4/14/73
                                                 40         50         60


                                                  Engine  Air  Flow,  scfm
                          FIGURE A-2.  AIR-FUEL RATIO VERSUS CARBURETOR AIR FLOW WITH UNLEADED FUEL

-------
                                  A-7
checked and set to specifications, and the ignition patterns were observed
with an Ignition Analyzer.  No problems or malfunctions were noted after
servicing.

                            Oil Consumption

          When the oil and oil filter in both cars were changed, the new oil
and new filters were weighed before use.  Following the test series the oil
was drained and weighed again along with the filter.
          Oil consumption by the unleaded-fuel car was 0.58 lb per 1000
miles over a total distance of 2,344 miles, and by the leaded-fuel car was
0.95 lb per 1,000 miles over a total distance of 1,212 miles.  The oil
density is 7.35 lb per gallon; thus, the oil consumption rate for the
white unleaded car as shown in Table A-2 was 0.32 quart per 1,000 miles and
for the blue leaded car was 0.52 quart per 1,000 miles.
          In appearance, both oils were considerably darker after use than
when fresh.  Oil drained from the unleaded-fuel white car was black but not
dirty in  looks or feel.  Oil from the leaded-fuel blue car was grey-black
and looked and felt dirty.
          Accumulated mileage at the beginning and at the end of the oil
economy measurement was 10,583 miles and 12,927 miles, respectively, for
the unleaded fuel car, and 9,217 miles and 10,429 miles, respectively, for
the leaded fuel car.
          After six test runs on the leaded-fuel car and ten test runs on
the unleaded-fuel car, a check was made on the oil consumption.  Oil
consumption of the unleaded fuel car was 0.31 quart per 1,000 miles, and
of  the leaded fuel car was 0.39 quart per 1,000 miles.

               Development of Acceptable Choke Operation

Apparatus

          A device to move the choke plate automatically according to a
preselected time schedule is illustrated in Figure A-3.  A synchronous-type
gearmotor driving a shaft with a tab on its end through an 0-ring belt-and-

-------
                      A-8
TABLE A-2.  OIL CONSUMPTION DURING TEST SERIES
            (QUART PER 1,000 MILES)
    Run           Unleaded-         Leaded-
    No,           fuel car          fuel car


 11-29 to 1-15      0.32              0.52

 4-4 to 4-26        0.31              0.39

-------
       Choke plate-
Choke plate
linkages
Vacuum -
break diaphragm'
Drive  shaft
  Drive rod
Choke lever
                                                                       Drive pulley-
                                                                          Idler pulleys'
                                                                                                              Driven pulley
                                   FIGURE A-3.   DEVICE FOR CONTROLLED CHOKE  OPENING ON A
                                                 REPRODUCIBLE TIME SCHEDULE

-------
                                  A-10
pulley system was mounted on the choke housing, with the axis of the driven
shaft coincident with the choke-plate shaft.  The tab pushed against the
choke lever in the choke housing to move the spring-loaded choke-plate shaft.
          The gearmotor shaft speed was 1 rpm and the drive ratio was
approximately 10 to 1.  The shaft rotation rate is thus about 34 degrees
per minute.  Space limitations prevented using a higher drive ratio.  To
accommodate the gearmotor, drive ratio, and mounting housing and plate,
the engine air cleaner housing was raised 1 inch from the carburetor body
by means of a round spacer tube.  Gaskets were used at each face of this
spacer tube.
          The choke is free to be opened wider than the control lever
requires if intake-air velocity pressure is great enough to overcome the
choke spring force.  There was a lack of repeatability of the gaseous mass
emissions during the series of Runs 12-19 to 1-15 inclusive, which may have
been caused in part by too light a choke-plate spring resulting in erratic
action due to the air velocity.  Prior to resumption of testing with Runs
4-4 through 5-22 the automatic choke drive system was made more slip-proof
by adding two idle pulleys which increased the 0-ring belt tension and in-
creased the contact length ("wrap") of the belt on both driver and driven
pulleys.  A stiffer spring was also installed on the choke-plate shaft to
improve the stability of the choke plate under the influence of engine
vibration and carburetor air flow.  The lighter-than-normal spring had
been used in the earlier series to minimize the chance of choke drive-belt
slippage.

Characteristic Stages in Choke Schedules

          There are three stages of choke motion.  The first stage is a
quick partial opening to about 30 degrees, as soon as sufficient manifold
vacuum  is present, v/hich may require only 2 seconds.  The second stage is a
hold at partial opening while the thermostatic coil is warmed up by exhaust
heat.   The  length  of  time at this stage depends on ambient temperature and
the speed of thermostatic coil warmup.  The third stage is under the control of
the thermostatic coil and air velocity pressure on the choke plate.  Time at
this stage will depend on the design of the coil and the heat it receives.

-------
                                 A-ll
          Figure A-4 illustrates idealized choke-opening schedules for
cold-start IA-4 cycles under various laboratory controlled conditions.
Information used for the three solid curves on this chart was supplied to
Battelle by Dr. W. R. Pierson of the Ford Motor Company and is derived from
special development work conducted on Ford 351 CID engines.  Real choke
action is similar to the idealized curves in Figure A-4 but is not as sharply
defined.
          The lean and rich curves indicate limits within which -a normal
choke should be operated, for the particular engine and conditions of Ford's
development program, to avoid stumble and stall at the lean end and to meet
emissions standards at the rich end.  These limits are only approximate and
may be subject to wide variations with other cars, carburetors, or ambient
conditions.  Choke schedules developed in the experimental study of the
"CAPE-19 cars did differ, as shown in the next section.

Experimental Studies of Choke Schedules

          Experiments with the choke opening schedule were conducted in con-
junction with development and checkout of other systems, procedures, and
instruments.  Proper idle jet setting was also evaluated in these experi-
ments.  Initially, during a series of five runs, the idle jets were adjusted
to give lean-side smooth idle at approximately 0.5 percent CO or less in
drive idle.  However, during later experiments, the drive-idle CO was
raised  to  1 percent.  In the test program, the CO in drive idle was
allowed to  range between 0.6 and 1.2 percent or was readjusted to
1 percent.
          Table A-3 summarizes the results of the test runs which were
conducted in the process of developing the choke opening schedule.  Three
runs were made with the initial vacuum break angle of 30 degrees and with
choke movement to full open at 70 degrees.  Several tests were run at the
30 degrees vacuum-break angle but at several different time spans to full
open.  The vacuum break angle was then changed to 25 degrees for three more
runs with a 3-minute time span to full open.  Next, the vacuum break angle
was reduced to 17 degrees.  The time span to full open was kept at 3 minutes

-------
                                  A-12
d)
o>
cn
c
    601—  Full open —
50
    40
    30
              Opened  by manifold  vacuum
                                       I
              15      30      45      60      75      90


                       Time From  Start  of  Engine, seconds
                                                           105
120
      FIGURE A-4.   IDEALIZED CHOKE OPENING SCHEDULES  FOR MODIFIED

                    COLD-START LA-4 CYCLE

-------
                            A-13
TABLE A-3.  TEST DATA RELATING TO CHOKE SCHEDULE DEVELOPMENT

           Unleaded RE-14IB Fuel
           Tunnel Flow Rate 905  scfm
           Sample Point Pressure 1 inch H90
Choke Schedule
Test No.
10-13
10-16
10-18
10-25
10-26
11-15
11-16
11-17
11-29
12-1
12-4
12-6
12-18
CO.
percent
Idle 50
0.3
0.2
0.2
0.2
0.4
1.0
0.7
-
0.6
0.6
0.7
1.1
0.8
0
0
0


0


0
0
0
0
0
mph
.3
.3
.3
-
-
.5
-
-
.4
.5
.4
.5
.4
Time Span
Vacuum to Full
Break(b) Open (c)
Degrees Minutes
30
30
30
25
25
25
17
17
17
17
17
17
17
1
2
2
3
3
3
3
3
3
3
3
3
5
.7
.7
.2
.0
.0
.0
.0
.0
.8
.8
.8
.8
.3
Mass Emissions
R/mile
HC
14.
11.
1.
1.
3.
2.
2.
1.
2.
2.
2.
1.
1.
1<6)
7(e)
34
38
96
09
18
95
02
30
06
90
63
CO
11.
10.
9.
13.
19.
11.
54.
25.
30.
34.
26.
38.
27.

1
1
9
3
6
9
3
6
4
0
3
6
2
(a) Measured at tail pipe.
(b) Full open choke is 70 degrees.
(c) Measured from start of engine.
(d) Computed from tunnel-bag gas composition.
(e) High HC emissions on Tests 10-13 and 10-16 indicated ignition
misfire problem, which was found to be partially shorted spark
(f) Ignition system problem co'rrected.
(d)
NO
3.31
1.36
1.56
2.97
1.55
2.82
2.93
2.89
2.88
2.93
2.63
2.81
2.82
system
plugs.

-------
                                 A-14
then increased to 3.8 minutes0  Finally, a further modification was made
in the choke schedule beginning with Run 12/18 to provide a slightly longer
and also more realistic opening characteristic.  The rate of opening was
halved from about 32 degrees per minute to 16 degrees per minute.  Also, the
beginning of further opening from the vacuum-break position was advanced to
about 2 minutes after zero time in the starting sequence and the full-open
position was reached at about 5.3 minutes.  This sequence was selected for
use in the first tests and designated Schedule I, which completed choke-
schedule experiments.  Other schedules designated I-S, II, and II-S were
selected later, to accommodate cycle changes and to maintain emissions with-
in specified limits, as described in the next section.

                Choke Schedules and Starting Sequences

Choke  Schedule  I  (Modified  IA-4 Cycle)

           Figure A-5  shows  Choke  Schedule  I.   The sequence-time  clock,
exhaust-gas  diverter  valve,  and tunnel  bag and dilution air bag  sampling
are  started  simultaneously  at  time 0.   Fifteen seconds later the engine is
started.   At 30 seconds  the accelerator is "kicked down"  and at  40  seconds
the  car  is put  in  gear.   The choke motor  is  started  at 60 seconds  (although
the  choke  was  opened  17  degrees by manifold  vacuum when the engine  started).
The  choke  opening  rate  is 16 degrees/minute  so the choke  is full open  (70
degrees) at  322  seconds  (about 5.38 minutes).  The first  acceleration mode
of the cycle begins at  55 seconds.

Choke  Schedule  I-S  (Standard LA-4 Cycle^

           Figure A-6  shows  Choke  Schedule  I-S.  The  sequence-time clock,
exhaust-gas  diverter,  valve,  tunnel bag and  dilution-air  bag sampling, choke
motor, and engine  are  started  simultaneously.  Ten seconds later the
accelerator  is  "kicked  down", and the car  is put in  gear  at 15 seconds.
The  first  acceleration mode  begins at 20 seconds.  The choke opening rate
is 16 degrees per minute  so  the choke is full open at 262 seconds (4.38
minutes).

-------
                                             A-15
-
0.
e
-o
QJ O>
o> c
Q. <
CO
   0)
.
O)
>
   o
   _c
   o
    o>
 Q.

 E
 -o"  «
 0}  O>
 (U  C
 o. <
 CO

    o
    _c
    o
                                               Choke  plate angle
                Start  engine  (15 sec)
            Kick  down  (30 sec)

           (— In gear  (40 sec)


                —  Start choke  motor (60 sec)
                              Elapsed  Time From  Sequence  Start, minutes
                                  FIGURE A-5.   CHOKE SCHEDULE  I
       70
       60
        50
                                            Choke plate angle
   Tr
40
 -S?  n   30
        20
        10
 Start engine and  choke motor  (0 sec)

  Kick  down  (10 sec)

— In gear  (15 sec)
                               Elapsed  Time From Sequence Start,  minutes
                                   FIGURE A-6.   CHOKE SCHEDULE  I-S

-------
                                 A-16
Choke Schedule II (Modified IA-4 Cycle)

          Figure A-7 shows Choke Schedule II.  The sequence-time clock,
exhaust-gas diverter valve, tunnel bag and dilution-air bag sampling, and
choke motor are started simultaneously.  Fifteen seconds later the engine
is started.  At 30 seconds the accelerator is "kicked down" and at 40
seconds the car is put in gear.  The first acceleration mode begins at 55
seconds.  The choke opening rate has been modified to 30 degrees per minute
so the choke is full open in 140 seconds (2-1/3 minutes).

Choke Schedule II-S (Standard IA-4 Cycle)

          Figure A-8 shows Choke Schedule II-S.  The sequence-time clock,
exhaust-gas diverter valve, tunnel bag and dilution-air bag sampling,
choke motor, and engine are started simultaneously.  Ten seconds later the
accelerator is "kicked down", and the car is put in gear at 15 seconds.
The  first acceleration mode begins at 20 seconds, and the choke is full
open at 140 seconds (2-1/3 minutes)'.
          The dashed lines on Figures A-5, -6, -7, -8 represent the  first
and  second modes of the driving cycle.  Key events such as engine start,
acceleration "kick down", and in-gear are identified.

Periods of Choke Schedule Use

          Each of these schedules was developed to meet the requirements of
stable car operation.  Choke Schedule I and the corresponding starting
sequence were used in Runs 12-18 to 1-23, 4-4 to 4-16, 4-18 to 4-26.
Choke Schedule I-S was used for the standard IA-4 cycle of Run 4-17.
Choke Schedule II was preferred for Runs 5-9 to 5-17, 5-21 -and 5-22 to
control gaseous emissions closer to the maximum allowable concentrations.
Choke schedule II-S was adapted from II for two standard LA-4 cycle
Runs 5-18 and 5-19.  Other operational' and apparatus information on these
runs is summarized in the following section.

-------
               A-17
ru
60
Q)
0)
-c CT 50
QL 
o 20
0
10
ci
°
~7C\
t(j
60
w
QJ
0)
,c & 50
QL 0)
C7 "U
"g "I. 40
o> c
Q. <
« * *o
•o °
£ c1-
> ^
•g 20
O
10

7
r,
/
>
/[
!,
0
X^"" — Choke plate angle
- Start choke motor (0 sec)
r- Start engine (15 sec) /A/\ / V«\ ^ mph
p Kick down (30 sec) / ^
r~ In aear (40 sec) / v \
// \
1 ^
^*^ %/ V » f \
^^/ * f 1
X/ ' I ' \
i' l ' \
"III 1 \ 1 / 1 1 1 I ,
1 23456
Elapsed Time From Sequence Start, minutes
FIGURE A.-7. CHOKE SCHEDULE II
/*~~ Choke plate angle
- Start engine and choke motor (0 sec) /^
/ A / \
— Kick down (10 sec) 'v ^^ / v^ .mph
/ / V \_^^
— In gear (15 sec) ^ / v\
/ /" 
i/ , \ /, , , \ ,
1 23456
Elapsed Time From  Sequence  Start,  minutes
   FIGURE A-8.  CHOKE  SCHEDULE II-S

-------
                                A-18
                    Summary of Test Conditions in
                           Experimental Runs
          Table A-4 summarizes emissions of total particulates,  HC,
CO, and NO for the 58 experimental runs completed during tfhe course of
this study.

                            Dilution Tunnel

          The dilution tunnel (Figure 1, page 3) is a steel tube 36 feet
long and 23 inches in diameter constructed from six flanged sections bolted
together.  Dilution air is supplied by a blower to a filter section at the
upstream end, and the filtered stream enters the tunnel near the tailpipe
of the car.  Exhaust and air both pass through a mixing orifice and thence
through the tunnel to the sampling and outlet sections.
          The tunnel outlet system consists of a 3-foot tapered section, a
damper, and the discharge duct.  The damper is used to control the pressure
at the sampling point.  The tapered transition section ahead of the damper
assures that the tunnel flow patterns at the sample probes will not be
affected by the flow restriction of the damper.

Sample Probes

          The sample probes are located 30 feet 8 inches downstream from
the mixing orifice.  Figure A-9 is a cross-sectional sketch of the tunnel at
the sampling point showing the location of the various sample probes and
their function.  Sampling ratios for the Sinclair-Phoenix smokemeter and
single particle counter were 0.25 and   8.8,  respectively, and the cas-
cade impactor was operated at a sampling ratio of 9.2.
          Figure A-10 is a detailed sketch of the residence chamber sample
probe.  This sample probe is a 2-inch  (inside diameter) PVC plastic pipe
enlarged to 2.1 inches at the inlet.   The total length of the sample line
is 8 feet with two large-radius bends,  one in the tunnel as shown  in the
sketch, and one prior to entry into the residence chamber.  The sliding-
plate valve permits flow into the residence chamber when open and  is used
for precise control of the sampling time.

-------
              TABLE A-4.   SUMMARY OF  EXPERIMENTAL STUDIES OF  EXHAUST  EMISSION
Test Conditions
Date
10-13
10-16
10-18
10-25
10-26
11-15
11-16
11-17
11-29
12-1
12-4
12-6
12-13
12-15
12-18
12- 17
12-20
12-21
12-22
1-17
1-19
1-23
12-27
12-28
12-29
1-3
1-5
1-10
1-11
1-12
1-15
Car
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
W
0
0
B
B
li
B
8
B
B
Fuel
NL
.ML
NL
NL
NL
NL
NL
NL
NL
NL
NL
NL
Nl.
NL
NL
NL
NL
NL
NL
NL
Nl.
NL
1.
L
L
L
L
L
L
L
L
Cycle
LA-4(M)
LA-4(V.)
LA-4 (M)
I.A-4 (M)
I.A-4 (M)
LA--l(M)
LA-4(V!)
I.A-4 (M)
LA-4 (M)
I.A-4(M)
LA-4 (M)
LA-4 (M)
l.A-4 (M)
I.A-4 (M)
LA-4IM)
I.A-4(M)
LA-4 fM)
LA-4(M)
I.A-4 (M)
LA-4 (M)
I.A-4(M)
LA--I(M)
I.A-4 (M)
LA-4 (M)
LA-4(M)
I.A-4 (M)
LA-4(M)
I.A-4(M)
LA-4 (M)
LA-4 (M)
LA-4(M)
Schedule
UD-
DO
UD
UD
UD
UD
UD
UD
UD
UD
UD
UD
UD
UD
L'D
1
1
I
1
1
1
I
1
1
I
1
1
I
!
1
1
Controller
RI
RI
RI
RI
DT
Ki
RI
RI
RI
m

DPC:
DPC
DPC
DPC
DPC
DPC
DPC
DPC
RPC
DPC
RI
R!
RI
DPC
DPC
DPC
RI
!U
RI
RI
RI
RI
MAAS
No
No
No
No
No
No
No
No
No
Yes
Yes
Yes
No
Yes
Yes
No
No
No
Yes
No
No
Yes
Yes
Yes
Yes
No
No
No
No
Yes
Yes
General Comments
Ignition problems
Ignition problems

Choke development
Choke development
Choke development
Choke development
Manual drive
Choke development
Low idle CO


Soak temp low - Nllj erratic

Soak temp low - CS changed
CS changed - low CO idle






Various problems
Run-in mileage low

Run length low, idle CO low
Soak time: short
Soak short, soak temp low
Idle CO high, soak temp low
Soak temp low

Hum.
O
A (SI)
.A (SI)
--
A (SI)
--
--
--
A (SI)
A (SI)
A (SI)
0
O
0
O
O
O
A
A
0
A
O
A
O
O
A
A
A
O
O
A
Variables
Lead
O
O
0
O
O
-•
--
--
O
O
0
O
O
0
O
O
O
O
0
O
O
O
B
8
B
B
B
B
B
B
B
Dust
O
O
0
O
O
--
--
--
O
O
O
O
O
O
O
0
c
0
c
0
c
c
c
c
O
c
O
O
c
0
O
Nil,
0
O
0
O
O
--
--
--
O
O
O
O
D
O
D
D
O
D
0
D
1)
D
O
O
D
D
O
D
D
O
O
Part*
--
--
--
--
--
--
--
--
0.062'
0.031'
0.015'
o. on
0. nil
0.014
0.018
O.O'.'fl
Dust
0.014
Dust
0.03S
Dust
Dust
Dust
Oust
0.255
Dust
O.C41
0.269
Dust
0. 162
0.164
Emissions. s/nii
HC
14. 1
11.7
1.34
1.33'
3.0C
2.09
2.18
•1.95
2.02
2.32
2.05
1.08
1.70
2.06
1.6.1
1.73
1.70
1.89
1.84
1.60
1..V.I
1.40
--
5.95
6.55
4.82
7. '23
6.33
3.34
4.04
5.39
CO
11. 1
10. 1
7.9
13.3
14. C
11.9
54.3
25.6
30.5
34.2
26.2
33.3
25. P
22. 1
27.2
2:1.3
23.9
36.2
33.0
32. C
31.7
2S.2
--
58.1
71.6
3-1.0
53. 1
47.7
33.4
44.1
39.0
NO
3.3!
1.36
1.5C
2.97
1.55
2.82
•2.93
2.S9
2.88
2.93
2.63
2.81
2. 78
2.49
2.S2
3.23
3. 12
2.25
1.71
1.46
!.!>!
1.3C
2. i3
2.17
--
1.53
--
2.11
1.98
1.19
1.38
                                                                                                                        I
                                                                                                                        t-'
                                                                                                                        VO
At this point (lie cars were leak checked and a small leak was found in the white car and a very small

 leak in the blue car.

-------
TABLE A-4.  (CONTINUED)
Kuit
Da le
4-4
4-6
4-7
4-9
4-10
•j-n
4-12
4-)3
4-16
4-17
4-18
4-10
4-2-1
4-20
4-25
4-26

5-0
5-10
5-1!
S-!4
5-15
5-1C
5-17
5-13
5-19
5-21
5-22



Test Conditions
Car
W
W
W
W
W
W
W
W
W
V.'
B
&
B
B
3
a

B
B
B
W
W
W
W
W
W
3
B
Car
Fuel
Cycle
Fuel
NL
.NL
NL
NL
NL
NL
NL
NL
NL
NL
L
L
L
L
'L
L

t^
L
L
NL
NL
NL
NL
NL
NL
L
t



Schedule






Instruments












Cycle Schedule
LA -4 (M)
LA-1 CM)
LA-1 (M)
LA -i { M)
U-) (W)
LA -I (M)
LA-» (M)
LA-J(M)
LA -4 (M)
LA~!
LA-1 (M)
LA -4 (M)
LA -4 (M)
LA-» (M)
LA -4 (M)
LA-i (M)

LA -I ( K!)
LA-» (M)
LA-1 (M)
1/.-1 (M)
LA-»(M)
LA-4(M)
U-»(M)
LA-t
LA-»
LA-4(M)
1A-4 (M)
W - White
ML - Nonleaded
LA-4 (M)
LA-4
UD
I and I-S
II and II-S
HAAS




I
I
i
1
1
I
I
I
I
I-t
I
I
I
I
i
I

;t
i;
ii
u
ii
u
u
II-4
II-S
u
ii



Cor,tro!!cr
DPC
DPC
DPC
DPC
i)?C
DPC
DPC
DPC
DPC
DPC
CPC
DPC
DPC
DPC
DPC
DPC

DPC
DPC
npc
DPC
DPC
DPC
DPC
DPC
DPC
DPC
DPC
B - Blue
L- Leaded
Cycle with
Cycle with
MA AS
Mo
No
No
No
No
No
No
No
No
No
No
No
No
No
No
No

No
No
No
No
No
No
No
No
No
No
NO


55-second
20-second
Gcr.cr-i Comments
Checkout
C!ie.;kout
C!ie.:kc'jt
Checkout
Chc-.-kc-ut
Hivli KC. CO
High !!C. CO
High JiC. CO
High HC, CO
it.:. Cycle
Checkout only
Atoned
Aborted
High '.1C. CO
High !IC. CO
Kign :iC. CO

Ba'.ciine
llasclinc
Aborted
Aborted
Dateline
Caroline
batcline
Std. Cycle
SfJ. Cycle
Uas.-linc
B«selln«
KEY

Initial idle
Initial idle
Variable.
Hum. Lead
O
O
O
O
O
O
O
O
O
0
O
O
O
0
O
O

O
O
O
O
O
0
O
O
0
0
0



O
O
O
O
O
0
O
O
0
O
B
3
B
E
B
B

B
B
B
O
O
0
O
O
O
B
S
Controller

Humidity
Particulate
Dust
O
O
0
O
O
O
0
0
0
0
O
O
0
O
O
O

O
0
0
O
0
0
O
O
O
O
0
DPC
RI
(SI)
Under development *


Defined In
Defined In
text
text




Variables

Minnesota Aerosol Analysis 'System
























0
A
B
C

D

Emissions. R/rriU
Nil., Pan.* HC CO NO
O -- 	
O -- 	
O -- 	
O -- 	
O -- 	
0 0.192 5.81 68.d 2.46
O 0.173 5.96 73.9 2.53
O 0.195 6.13 72.5 2.33
O 0.139 C.22 77.7 2.91
O 0.041 3.12 5S.G 2.72
O -- 	
O — 	
O -- 	
O 0.319 C.07 71.9 1.99
O 0.340 5.04 0:3.2 2.0C
O 0.340 5.70 75.8 1.90
1
O 0.135 3.01 :«.! 2.CO £>
O 0.153 5.35 47.4 2.21
0 -- 	
O -- 	
O 0.040 3.43 3S. 5 2. :IS
O 0.046 3.50 3.-I.2 2.48
<' O.W4 .VJJ W..1" •-'. f.O
« 0.07S 4.CC •'•'-•. 4 ;.*7
" 0.071 4. 12 •)l'.'< 2.«9
O 0.211 3.37 38.2 2.19
0 0.20J 3.96 «"1 l.»3
Magnetic tape
Paper tape
Steam Injection
Based on Metricel weights, Sampling Ratio " 2.2
Without backup filter
Low or normal values
High humidity
High lead
High dust (solid tnpurlty
in atmosphere)
High ammonia (gaseous
Impurity In atmosphere^

-------
                              A-21
1/4-in. ID
{CO, C02, NO
 analyzers)
                 l/16-in. ID
                 (single  particle
                  counter)
1/4-in.  ID
(HC analyzer)
                                                             1/4-in. ID
                                                             (cascade
                                                              impactor)
                                                     l/4-in. ID
                                                     (47mm  filters)
l/2-in. ID
 (142 mm filters)
                                                   l/2-in. ID
                                                   (Sinclair -
                                                    Phoenix)
     2.1 -in.  ID
     (residence
      chamber)
       FIGURE  A-9.   PATTERN OF PROBE  INLETS  IN CROSS SECTION
                    OF DILUTION TUNNEL AT  SAMPLING POINT

-------
                        A-22
                          To
                      residence
                       chamber

     Tunnel-bag
     sampling probe.
                                       Sliding plate valve
                                       Tunnel.
                               \\\\\\V\\\\\\\\\\\\\\\V\\\\\\\\'
FIGURE A-10.
CONNECTION AT TUNNEL  OF  PIPE TO CARRY DILUTED
EXHAUST TO RESIDENCE  CHAMBER

-------
                                 A-23
Tunnel Sample-Point Pressure

          Operation of the tunnel at a positive pressure is necessary to
provide a means for transferring sample from the tunnel to the residence
chamber, which is always at ambient pressure because of its flexible walls.
A further requirement of this sample-transfer operation is that the sample
should always be proportional to the exhaust gases produced throughout the
driving cycle.  Since the tunnel flow rate is nearly constant, the sample
flow rate should also be constant to achieve proportional sampling.  The
sample flow rate will be constant if there is a constant differential
pressure between tunnel and residence chamber.
          The differential pressure between tunnel and residence chamber
was measured during a number of tests using a strain-gage pressure trans-
ducer with a range of 0 to 0.1 psi (2.77 inches H_0).  Tunnel sample-
point pressures from about 1/2 inch HO up to about 2 inches H~0 were used.
It was concluded from these tests that a tunnel sample-point pressure of
about 1 inch H20 results in an acceptably constant pressure differential.
          Figure A-ll shows a reproduction of the chart record of tunnel-
to-chamber differential pressure during a run in which the sample-point
average pressure was 0.91 inch H.O.  The chart shows that AP remains
acceptably constant throughout the cycle.  Deviations from a steady pressure
appear to be about ± 2 percent during most of the cycle.  In the second
high-speed mode of the cycle the tunnel pressure increased to about 10
percent over the average for a period of about 1 minute.

Tunnel-Bag Sample

          A composite sample of the diluted exhaust gas is collected from
the flow going into the residence chamber during the test run.  This com-
posite bag sample was analyzed for gaseous components to measure the final
dilution from tunnel to chamber, as well as to monitor gaseous emissions
for assurance of normal engine operation.
          Figure A-12 is a sketch of the tunnel-bag sampling system.  A
diaphragm pump in conjunction with a rotameter and regulating valve supplies

-------
    1.2
    1.0
   0.8
O
 CM
X
en
   0.6
 o
a.
<3 0.4
                                                                                                             I-O
                                                                                                             -O
   0.2
      0
 8               12
      Elapsed Time, minutes
16
20
24
                       FIGURE A-11.
RECORDED DIFFERENTIAL  PRESSURE BETWEEN TUNNEL AND
RESIDENCE CHAMBER DURING A MODIFIED LA-4 CYCLE

-------
                                     A-25
Tunnel bag
   Regulating valve
       Diaphragm pump
                              Bag shut-off valve
                                 Rotameter
                                      I   I
                                     Yr_
                                               •Filter
Residence chamber
sample pipe
                                                            Bag-sample probe
                       FIGURE A-12.  TUNNEL-BAG SAMPLING SYSTEM

-------
                                 A-26
a constant sample flow rate to the bag.  Particles are filtered out before
the pump.  At the end of the cycle the bag is disconnected from the rota-
meter and connected to the gas analyzers to measure the average gaseous
emissions.
Calculation of Exhaust Mass Emissions
from Tunnel-Bag Sample
          A 23-1/2-minute bag sample of diluted exhaust gases from the
tunnel is collected during each test run.  This composite sample is
equivalent to a CVS-type bag sample.  Mass emissions per mile are computed
as the product of contaminant density (g/cu ft at 68 F and 1 atm pressure)
x contaminant concentration (vol/vol) x V  . .  The equation in the Federal
         (1)                              mix
Register    for calculating V . . the standard volume of the diluted exhaust
—°	                 &  mix'
gases emitted per mile, is as follows:

          V .  = total tunnel flow rate  (cfm) x run  length (minutes)
           mix
                                           tunnel absolute pressure (in. Hg)
                                         x
             x
                                                         29.92
                            528                     1
                 tunnel temperature (°R)         7.5 miles

Lead Deposits in Pipe to Residence Chamber

          Lead deposits were measured in the sample-transfer pipe between
tunnel and residence chamber (Figure A-10, page A-22) after the pipe had
been exposed to diluted exhaust from nine cold-start IA-4 cycles using
leaded fuel.  The operating parameters were as follows:
          Fuel:  2.5 g Pb/gal; density, 6.25 Ib/gal; rate, 4.25
                 Ib/cycle Lead in fuel residues from nine cycles:
                 9 x 2.5 x 4.25/6.25 = 15.3 g
          Sample Flow:  Tunnel flow, 905 cfm; sample flow through pipe;
                        10 cfm (average values for all test runs)
          Sampling Ratio:  1.3.
 (1)   Federal  Register,  Vol. 37, No. 10, January 15, 1972.

-------
                                 A-27
          Assuming all lead is discharged in exhaust, then total sample
flow in nine cycles contained 15.3 x 10/905 = 0.17 g Pb.
          Found in sample pipe:   0.006 g Pb, or (.006/.17) x 100 =
                                 3.5 percent of Pb in samples.
          A particulate sample was collected on filters from the tunnel gas
in Test 1-12 amounting to 0.006 g weight.  Sample gas flows were 4.5 cfm
through filters, and 10 cfm through pipe to residence chamber.  Gas sample
to chamber contained 0.006 x 10/4.5 = 0.013 g particles.  Assuming the
exhaust particles contained a .mean value of 25 percent Pb, and that this
test was typical of nine leaded fuel tests, total lead carried through the
pipe was 0.013 x 9 x .25 = 0.029 g.  Sample collected from wall was
(.006/.029) x 100 = 21 percent of Pb exposure, based on the assumptions
made.
          It is concluded from these results that lead loss in the transfer
of sample gas to the residence chamber is a significant part of the total
particulate sample, and would affect a quantitative material balance.  Never-
theless, losses are not so severe as to preclude study of aging of particles
in the residence chamber.

Test for Uniformity of Mixing in the Tunnel

          Simultaneous samples of auto exhaust particles were collected at
the standard sampling location (Page A-18) from a 13-probe assembly to measure
the uniformity of particle distribution across two perpendicular diameters
of the tunnel.  The coefficient of variation was 4.5 percent, which is an
acceptably uniform distribution.

Gaseous Contaminant Injection System

          Figure A-13 is a sketch of the gaseous contaminant injection
system, which was installed for the study of the effect of a gaseous con-
taminant, ammonia, on aging of auto exhaust particles in the residence
chamber.  The gaseous contaminant is introduced into the tunnel for mixing

-------
                                         A-28

                                Tunnel inlet air flow
    Filter-
                        I U U U
                                                          Top Section View
Filter box
                                                         Direction of gas injection
                                                         "H-Pipe" diffuser
                                                         l/32-in. holes on
                                                         l-in. centers in
                                                         l/4-in. SS tubing

                                                         Supply pipe
                                                             Rotameter
                                                                         Regulator
                                                                              Gas
                                                                              cylinder
                                                      Regulating
                                                      valve
                     FIGURE A-13.  GASEOUS CONTAMINANT  INJECTION SYSTEM

-------
                                 A-29
with exhaust and dilution air.  The H-shaped distributor manifold is in-
stalled immediately downstream of the filters in the dilution tunnel filter
box, and has 1/32-inch-diameter holes drilled in the downstream side.
These holes provide a fairly uniform initial distribution of the contaminant
gas in the dilution air stream before it passes through the tunnel orifice,
where it is mixed with exhaust.
          The injection rate of ammonia was measured by bubbling the gas
through a glass tube containing ammonium hydroxide.  The flow rate was
determined by counting the bubble rate and estimating the bubble diameter
when operating with ammonia.  The same conditions were duplicated with
air, using a calibrated rotameter in the supply line to measure the
quantitative gas flow.  Becasue of the corrosive properties of ammonia, a
rotameter could not be used in direct contact with ammonia for the flow
measurement.

Solid Contaminant Injection System

          Figure A-14 is a sketch of the dust entrainment apparatus which
was used in some tests to add dust as a solid contaminant to the tunnel
air.  The apparatus consists of a motor driven disc containing four V-
shaped grooves.  Scraper vanes fill the grooves and level them.  The filled
grooves then pass under an aspirator which picks up the dust and dispenses
it.  The feed rate was controlled by the disc speed.  The resulting aerosol
is  fed into the exhaust pipe immediately downstream of the exhaust-gas
diverter valve.  Dust injected at this point is quickly entrained and mixed
with the exhaust gas and the mixture is diluted at the tunnel orifice plate.

Dust Contaminant

          The dust contaminant was Fine Arizona Road Dust which was screened
before use to remove all particles larger than 3.3 micrometers Stokes
diameter.  Figure A-15 is a Rosin-Rammler plot of the particle size dis-
tribution of the sample of dust as received before the larger sizes were
removed and discarded.

-------
                                     A-30
Filtered
  air
                                                                       Vibrator
                         FIGURE A-14.   SCHEMATIC OF DUST FEEDER

-------
                                          A-31
   99


   98




   95



   90




   80



   70


| 60


M 50


& 40
£  30
u
    20
 3

<->   5
   0.5


   0.2

    O.I

  0.05
   0.01
      0.2
0.3  0.4    0.6  0.8   I           2      34      6

                Equivalent Particle Diameter, microns


          FIGURE A-15.  PARTICLE SIZE  DISTRIBUTION OF

                        CLASSIFIED ARIZONA ROAD DUST
8   10
20

-------
                                 A-32

          Chemical composition of the classified dust was determined by
optical emission spectrometry, as shown in Table A-5.

         TABLE A-5.  CHEMICAL COMPOSITION OF FINE ARIZONA DUST
Element
Silicon
Aluminum
Magnesium
Iron
Manganese
Barium
Percent
15-30
5-10
0.7
3.0
0.05
0.05
Element
Chromium
Calcium
Vanadium
Copper
Sodium
Titanium
Percent
0.01
2-4
0.01
0.1
1-2
0.3
                           Residence Chamber
Chamber Configuration

          The residence chamber  (Figure 1, page 3) is a rectangular 6-Mnil
black polyethylene bag approximately 9 ft x 12 ft x 20 ft with a filled
volume of about 2160 cu ft.
          Figure A-16 is a layout of the residence chamber showing sample
probes, the  sample pipe, and the purge circulation system.  Diluted exhaust
gases from the dilution tunnel enter the residence chamber through a 2-inch
ID PVC plastic pipe which is located approximately 6 ft from one end of the
chamber and  4 ft down from the top.  The sample pipe projects horizontally
into  the chamber for a total length inside the chamber of about 5 ft and is
curved slightly so that the sample flow is towards one upper corner of the
chamber.  In the final design, the sample pipe has a tapered discharge
nozzle to promote mixing.with dimensions as shown in Figure A-17.  This
design was selected after three  series of exploratory measurements with other
configurations and locations, described in following sections.

-------
Bleed valve
-!>=
\
             Control valve
                                     Chamber  walls
Steam supply line
 Removable
 end cap
v
        Removable
        end cap
                     Inlet damper
                              Particulate filter
                              Drier bed
                              Charcoal filter









z




/
Pure




ie duct






i

I
9_in Tn
                                   Humidifier
                                    D
                          sample probes
                             (2)
                                                    3/8-in. ID
                                                    sample probes
                                                       (4)
                                                                                                          2-in. ID
                                                                                                         .sample  probe
    Outlet damper
                                                                                       Wet/dry bulb-
                                                                                       system
Sample pipe
from tunnel
                                                                                                          Purge
                                                                                                          blower
                                                                                                OJ
                        FIGURE A-16.   LAYOUT  OF RESIDENCE CHAMBER AND PURGE-CIRCULATION SYSTEM

-------
               A-34
                    2-inch ID PVC
                    sample pipe
                  \\\\X\\N>
FIGURE A-17.  TUNNEL-TO-CHAMBER SAMPLE-PIPE
           DISCHARGE NOZZLE

-------
                                 A-35
          Chamber samples for gas analysis are withdrawn from the center
of the chamber through 3/8-inch-ID stainless steel probes..  Samples for
particulate and light scattering analysis are withdrawn through two 2-inch-
ID PVC sample probes with intakes near the center of the chamber.

Dilution Ratio Experiments

          The dilution tunnel when operated at a total flow rate of 905 cfm
dilutes the auto exhaust by an average ratio of 30 to 1 at 72 F and 1 atm.
To achieve an overall dilution ratio of 300 to 1 in the residence chamber,
a tunnel-to-chamber dilution of 10 to 1 is required.  Thus, the tunnel
sample-point pressure, and the sample-pipe and residence chamber design
were selected to achieve this 10 to 1 dilution and to achieve fast and
complete mixing in the chamber.
          The 2-inch  diameter of the tunnel-to-chamber sample pipe was
selected  to achieve approximately isokinetic sampling from the tunnel.
However,  the flow through this pipe at 1-inch H^O differential pressure was
considerably greater  than required for the 10 to 1 dilution.  Consequently,
flow was  restricted to the desired rate of about 9 cfm with a discharge
nozzle at the outlet  end.
          In the actual  test runs, the sampling rate averaged approximately
10  cfm.  With an average tunnel flow rate of 905 cfm for the test runs,
the isokinetic sample flow rate would be 7.5 cfm for the 2.1-inch-diameter
probe opening, thus,  the actual sample flow was about 33 percent greater
than true isokinetic  flow.
           Table  A-6 summarizes the  results of the first  series  of nine
 preliminary dilution-ratio experiments,  Runs  9-5  to 9-20,  at a  tunnel flow
 of about 1100  cfm.   Two  locations  for flow restrictions  were compared,  one
at  the discharge end  of  the pipe inside the chamber and  the other in  the
pipe immediately downstream from the sample-flow control valve.  This
configuration was a simple semi-venturi shape with a straight bore between
straight-sided conical converging and diverging sections.
          These  tests were performed before all of the instrumentation was
available and operational; hence, only HC and CO measurements were made in
the tunnel and chamber to determine dilution  ratio.  The dilution ratios

-------
                                      A-36
                 TABLE A-6.   SUMMARY  OF  INITIAL  TUNNEL-TO-CHAMBER
                             DILUTION RATIO EXPERIMENTS

                             White  Unleaded Car
                             RE-141B  Fuel
                             Sample Point  Pressure  1  inch H^O
                             Tunnel Air  Flow,  1100  scfm
Tunnel- to-Chamber
(a\
Dilution Ratio^ '
Run From HC
9-5 4.8
9-6 6.5
9-7 6.2
9-8 12.0
9-12 15.3
9-13 11.0

9-15 11.0
9-18 15.2
9-20 10.0
From CO
11.9
70.0
5.8
14.8
13.4
11.0

14.0
7.4
17.2
Average
4.8
6.5
6.0
13.9
14.4
11.0

12.5
15.2
10.0
Description of
Sample-Pipe Restriction
Open pipe
Open pipe
Open pipe
3/8-inch nozzle
3/8-inch venturi
1/2- inch venturi
with 1" nozzle
it
it
ii



at pipe end
above valve
above valve
at pipe end



(a)  Computed from HC and CO measurements  in tunnel bag and in residence  chamber
     before and after run.

(b)  Average value taken as value computed from HC data only when HC  and  CO data
     were not in + 10 percent agreement,  because of intermittent malfunctions  of
     CO meter.

-------
                                A-37
computed from both HC and CO measurements are presented.  However, the HC
data are considered more reliable wherever the two numbers do not agree
well, because of intermittent malfunctions of the CO meter.
          One configuration, which gave adequate control of flow, had the
1/2-inch primary restriction located downstream of the sliding plate valve
used to cut-off sample flow  (Figure A-10, page A-22), plus another 1-inch-
diameter nozzle at the tube end in the chamber.  The last four tests, 9-13
through 9-20, were reproducibility tests run with this restriction con-
figuration.  It was concluded that flow control was acceptable, but mixing
in  the chamber was too slow.

Chamber Mixing Experiments

          Beginning with Test 9-15, Table A-6, dilution ratios and mixing
in  the chamber were investigated at the same time.  It was found initially
that mixing was completed 15 to 30 minutes after the end of the auto-
exhaust-generation run.  Particle concentrations were then similar in
various regions in the chamber.
          In a second series of tests a more detailed evaluation of chamber
mixing was made with propane tracer, using short sample probes temporarily
installed in four corners of the chamber.  These probes projected 1 inch
into the chamber and were each located within about 6 inches of the corner
so  that they would be sampling from extreme regions of the chamber.  The
regular sample probes in the center of the chamber were also used.  The
mixing-study probe locations (listed in the sampling sequence generally used
in  the tests) were:  side center near chamber middle, side center near
chamber wall, top southeast corner near wall, bottom southwest corner near
wall, top northwest corner near wall, bottom northeast corner near wall.
A full sampling sequence required approximately 12 minutes.  This allowed
about 2 minutes at each position to stabilize the reading and to note short-
term changes if they occurred.
          A total of 11 experimental runs were conducted in the propane-
mixing study.  Propane (LPG from a trailer-type tank) was introduced into
the tunnel filter box with the tunnel air flow at approximately 900 scfra
and with a sample-point pressure of 1 inch H?0.  The rate of propane in-
jection was adjusted to yield a constant value around 800 to 1000 ppmC in

-------
                                A-38
the tunnel-.  When stabilized conditions were obtained in the tunnel, the
residence-chamber sample valve was opened for a period of 23 minutes, the
standard LA-4 cycle running time.  Immediately following the end of this
sampling period the concentrations of HC in the residence chamber at the
various sample-probe positions wera measured in the predetermined sequence.
The sequence was repeated several times over periods up to almost an hour
a-fter the end of the sampling period.
          With the 1-inch-diameter nozzle opening at the end of the sample
pipe in the chamber used in the first series, the velocity of the gas
leaving the pipe was about 28 ft per second.  This was insufficient to
promote rapid mixing into corners of the chamber.
          Experiments, in the third series were then conducted with one sample-
pipe flow restriction located only at the pipe end.  Mixing was substantially
improved, and nozzle dimensions of 7/16-inch diameter by 1 inch long were
found to yield the desired final dilution ratio.  With this nozzle (Figure
A-17, page A-34) the velocity of the gas entering the chamber at 9 cfm flow
rate was about 145 ft per second..  A uniform mixture in the residence
chamber was obtained 12 minutes after injection was completed at the end
of the test run, at which time all HC concentrations agreed within 10 per-
cent.  Figure A-18 shows the time variation of the HC concentrations in
the residence chamber from the various sampling probes after the simulated
auto-exhaust run with propane, with the final modification of the mixing
nozzle in place.

Chamber Humidification

          High residence chamber humidity was initially achieved in Runs 10-
13 to 12-4  (Table A-4, page A-19) by injecting steam directly into the
chamber with the purge-circulation system in operation.
           This method worked quite well for bringing the chamber up to 70
percent relative humidity in a short time, but it produced an unacceptable
increase of the background particle level in the chamber.
          Other methods were tried and the final technique selected combined
the use of  steam to raise the humidity in the whole laboratory, the in-
jection of  some steam directly into the purge system makeup-air inlet
(Figure A-16, page A-33) and the use of a wick-type humidifier in the purge
system line as shown in Figure A-19  (also Figure A-16, page A-33).  The

-------
                                 A-39
     80
o
.a
t»
o
o
o
     70
     60
     50
O


Q.
Q.
0>

"I
o
.c
o

c
o
^    40
c
CD
O


O
     30
     20
      10
Propane Mixing  Study

 Test  10-9              	=	

 Tunnel flow  rate 960 scfm

 Tunnel propane  concentration  865 ppmC
                    10           20           30           40


                Elapsed  Time From  End of Fill  Period, minutes
                                                                       50
       FIGURE A-18.
                     TIME TO MIX PROPANE  IN RESIDENCE CHAMBER

                     WITH SAMPLE INLET  NOZZLE SHOWN IN FIGURE 18

-------
                            A-40
Motor
                                                              Clean  air
                    Water
                    line
    FIGURE A-19.  SCHEMATIC OF WICK-TYPE  HUMIDIFIER
                  IN RESIDENCE CHAMBER PURGE DUCT

-------
                                 A-41
humidified air passes through the filters before entering the chamber.  This
technique requires a longer period of time but does not affect the back-
ground particle concentration in the chamber.
Dilution Ratio Definition and
Method of Calculation
          The dilution tunnel dilution ratio is the total tunnel flow divided
by the exhaust flow.  The residence chamber dilution ratio is the total
residence-chamber volume (after sample addition) divided by the volume of
diluted exhaust gas added to the residence chamber.
          Dilution tunnel dilution ratio is computed directly from measured
tunnel flow and exhaust flow.  Residence chamber dilution ratio is computed
indirectly from measurements of CO and HC concentrations in the chamber,
before and after sample addition, and in the tunnel bag sample.
          The development of residence-chamber dilution-ratio equations
follows.
          Symbol Definitions
          Let:  Q  = residence chamber volume before sample addition
                 3
                Q  = volume of diluted exhaust gas added to residence
                 s
                     chamber during driving cycle
                Q  = final volume of residence chamber after sample
                     addition
                C  = HC or CO concentration in residence chamber before
                 a
                     sample addition
                C  = HC or CO concentration in diluted exhaust gas
                 s
                C  = HC or CO concentration in residence chamber after
                     sample addition.
          Equations
                                  Qt
          D.R.  (dilution ratio) = r~	(1)
                                  ^s
          Q  + Q  = Q   (summation of volumes)	  (2)
           Si    S    C
          QC  +QC  = Q C   (summation of emission mass)	(3)
           a a    s s    t t

-------
                                 A-42
Solve equations (1), (2), and (3) simultaneously:
                          Q C    Q C    Q C
                           a a ,   s s _  t t
                          QC    Q C  ~ Q C
                           s a    s a    s a
                                             C
                                             _t
                                             C
                                              a
                                         C      C
                     (D.R.) - 1 - (D.R.)  T = ~  T
                 C   C
                  s -  e
                  1   P
                  *   *->
                  t   a
D.R. = CS"    	. . .	 . . . (4)
                            Instrumentation

Gas Analysis

          Direct reading and recording instruments were used for analyses of
gases from the tailpipe, the dilution tunnel, the residence chamber, the
filtered dilution air, and composite bag samples from the dilution tunnel.
In general, each instrument zero was set with a zero gas and the span with
one or more span gases covering the range of expected concentrations.  The
span and zero were checked and adjusted before and after each run.
Manufacturers' guaranteed values for gas composition were accepted for
standard gases to set zero and span at the reported concentration of the
span gas, and the instrument manufacturers' calibration curves were relied
on for interpolation and extrapolation.  There was no absolute standardiza-
tion by analysis of the standard gases.  On some occasions, zero gas and
two standard gases were used to construct a revised curve through the origin
and these two additional points.  Table A-7 shows the record of instruments
used during the year while developing the capability to obtain reliable
analyses of exhaust gas composition.  Some instrumental difficulties were
identified and corrected as soon as they were recognized.  Specific details
on calibrations and substitutions are described in tabulated comments dis-
cussing the individual gases.

-------
                                   TABLE A-7.   GAS ANALYSIS  INSTRUMENTS



Gas





CO
















HC


Samples


Location
Tailpipe




Tunne 1




Chamber



Background

Tailpipe



Tunnel

Chamber^ ^
Dilution
air


Time
Continu-
ous record
incl.
A/F ratio
modes
Cycle
record




Continuous
11/29-1/23
and 0, 30'
4/11 — >
Bag
sample
A/F ratio
modes


Cycle
record
0, 30'
Bag
sample

Approx.
Conc.n
1-5%




2-400
ppm




Low



Low

1000 -
2000 ppm


50 -
100 ppm
Low
Low

Instruments


Description
Olson-Horiba IR




Beckman NDIR




Same



Same

Beckman FID



Same

Same
Same

Standard Gases
Concentra-
tions
0, 4.99%




0, 152 ppm
0, 152, 220
0, 152,1075









0, 76.3 ppm









Use Period
12/6-5/22




12/6-4/25
4/26
5/9-5/22









12/6-5/22










Comments on Techniques and Instruments
Range 0-10%




Instrument malfunction 4/11-4/20;
corrected 4/25. Emissions above 1972
limit 4/11-4/26; adjusted to below
limit, 5/9 " X Bag samples from
tunnel 4/25, 4/26 , instead of con-
tinuous recorded analysis.

>
w



Tailpipe sampled for HC following
cycle during idle, 35 mph, 50 mph
modes. Span calibration before and
after cycle and after 50 mph mode.
Measurement used to detect abnormal
conditions .
Ditto
»

Chamber sample at zero time gives background concentration in chamber;  at 30 minutes  gives  concentration after.
dilution and mixing in the chamber.

-------
£ABLE A.-7.. (CONTINUED)




Gas




°2











Nn
w \j

Samples



Location
Tailpipe









Tunnel


Chamber

Dilution
air


j


Time
A/F ratio
measure-
ment







Bag
sample

0, 30'

Bag
sample



Approx.
Conc.n










1-20
ppm







Instruments



Description
Beckman 715


Beckman 715
Beckman 715



Beckman OM-11

Beckman NDIR
0-250 ppm
range







Standard Gases
Concentra-
tions
Air, 21%


Ditto
0.54,2.2%



Ditto

140 ppm


140,19 ppm




Ditto

Use Period
11/29-1/23


Ditto
4/11-4/26



5/9-5/22

11/29-1/12


1/12-1/23




4/11-5/22



Comments on Techniques and Instruments
First and second instruments gave
unsatisfactory and unreliable
measurements. Identical models.

Third instrument gave acceptable
results with improved techniques,
using long sampling time for slow
response.
Excellent results: Stable reading
with fast response.
>
Doubtful results JL.
-P-

Revised calibration curve to fit two
gases. Improved technique with
drastic dehydration in better cold
trap. Overhauled instrument. Good
results obtained with changes.
Reliable results.

-------
TABLE A-7. (CONTINUED)

Gas


co2




Samples
Location
Tailpipe

Tailpipe
Turme 1

Chamber
Dilution
air
Time
Bag
samples

Direct
reading
0,35,50
mph for
A/F ratio
Cycle
record

0, 30'
Bag
sample
Approx.
Conc.n







Instruments
Description
Beckman NDIR


LIRA IR
0-1%

Ditto
n
Standard Gases
Concentra-
tions
9.94%
12.4%


1100 ppm
7240

Ditto
ii
Use Period
11/29-4/20
4/25-5/22


11/29-1/23
4/11-5/22

Ditto
it
Comments on Techniques and Instruments
Instrument recorded sample from tail-
pipe 11/29-4/20 and 5/18-5/21. Bag
samples carried to instrument 4/25-
5/17.
Two span gases disagreed. Difference
represents 3% of measurement.

1100 ppra gas used routinely; 7240 ppm i
occasionally to check calibration 01
curve. Curve corrected to conform
to two concentrations of span gases.



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                                 A-46

Speed Controller

          A speed controller was used to drive the test? car automatically
through the LA-4 driving schedule after it was manually started and shifted
into gear.  During exploratory tests and choke schedule development* cars
were driven by a Research Incorporated (RI) controller, programmed by a
punched-paper tape (Table A-4, page A-19).  Problems were encountered with
faulty control by this instrument in a few tests and it was taken out of
service for repair.  While the system was being serviced, a second speed
controller, manufactured by Dynamic Precision Controls (DPC) and using a
magnetic  tape program input, was used for Runs 12-1 to 12-22.  The RI
punched-tape system was put back in service and used for Runs 1-3 to 1-15.
          The DPC magnetic tape speed controller system drives the car
through a more precise cycle than the RI punched tape speed controller,
because the punched tape tends to smooth out the minor speed fluctuations.
Therefore, a new DPC magnetic tape controller was obtained for all sub-
sequent tests.

Minnesota Aerosol Analyzing System

          A group of instruments known as The Minnesota Aerosol Analyzing
System  (MAAS) was available on loan* for some of the runs (Table A-4, page
A-19) and was used whenever available to characterize the size distribution
of automotive exhaust particles in suspension in samples removed from the
residence chamber.
           The MAAS consists of three aerosol particle counters in parallel
operation, which  in combination measure the aerosol size distribution
from 0.0032 to 10.0-u.m diameter.  The instruments consist of a modified Royco
Model 220  optical counter, a condensation nuclei counter (CNC), and a
Whitby Aerosol Analyzer  (WAA).  The output of the optical counter is fed
into a Nuclear Data (ND 812) computer, and the outputs of CNC and WAA are
fed into  a Hewlett Packard Data Acquisition System (DAS).
*  Courtesy  of Professor Whitby of  the University of Minnesota and Dr.
   William Wilson, Jr., of National Environmental Research Center, EPA.
(1) K. T.  Whitby, B.  Y. H.  Liu, R. B.  Husar, and N.  J.  Barsic, J. Colloid
    and Interface Science,  Vol. 39 No. 1, pp 136-164 (April,  1972)

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                                 A-47
          The size range of the modified Royco Model 220 sensor is from
0.562 to 10.0 M-m, and this range is classified into 512 channels under
control of the ND 812 computer.
          The condensation nuclei counter is a standard Environment-One
counter operated at an under-pressure expansion of 8 inches of Hg vacuum.
          The Whitby Aerosol Analyzer is an improved ion mobility analyzer
manufactured by Thermo Systems, Inc.  The instrument has feedback-controlled
high-voltage power supplies which permit automatic operation in conjunction
with the DAS.  It covers the size range between 0.0032 and 0.562 u.m and  the
minimum scan time is 2.0 minutes.

             Studies of Filtration  and Weighing Procedures

          The mass concentration of exhaust particles was determined by
measuring the net weight gain  of an absolute  filter  for filtration of a
measured volume  of diluted auto exhaust.  A procedure was developed to
 check the validity of  the weight gains measured.  Operations made a part
 of this  procedure are  described  in  following  sections.
Microbalance  in  Controlled Atmosphere
Balance  Room
          A  new Mettler Model M-5 microbalance xvith a claimed  sensitivity  of
 1  t-tg was  set up and  used  exclusively  on  this  project in an  isolated  room
 with controlled constant  humidity and temperature.  The microbalance was
 also used temporarily in  a  controlled humidity glove box, and  in  two other
 controlled-atmosphere rooms, with some results that were erratic,  before the
 satisfactory location was found.

 Repeatability of  Weighings  with  the Microbalance

          Table A-8  presents  typical  data  on  weighings of two  types 'of
 filters,  a stainless steel  disk, and  a Class  M platinum 500 mg weight.
 They were weighed every txvo hours one day  to  check on the operation  of  the
 balance and  on the technique  of  the  person performing the weighings. In

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TABLE A-8.  REPETITIVE WEIGHINGS  OF  BLANK FILTERS  AND  OTHER MATERIALS
Weights, g

Oct. 23 1972
Time
8:00
10:00
12:00
2:00
4:00
47-mm Glass
Filter
MSA J7864
0.105173
0.105181
0.105170
0.105165
0.105173

Stainless Steel
Disk
0.213274
0.213274
0.213265
0.213263
0.213272

142-mm Metricel
Filter DM450
0.574450
0.574545
0.574478
0.574509
0.574413

Type M 500 mg
Platinum Wt.
0.499996
0.499996
0.499995
0.499994
0.499995

Temperature,
F
72.3
73.5
74.0
75.0
73.0

Relative
Humidity, %
41.0
46.0
48.8 >
oo
46.5
28.5

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                                 A-49
 this  room  the maximum humidity was controlled below 50 percent RH,
but there was no control of minimum relative humidity.  The temperature
was controlled between 72.3 and 75.0 F in the weighing area.
          The apparent weight gains and losses of the filters in Table
A-8 did not correlate consistently with increases and decreases in humidity.
Therefore, the variations in these weights x^ere suspected to be attributable
to other causes, such as changes in electrostatic charge.  A small polonium
source had been used routinely in the balance during these weighings to
dissipate  static charges, but the observed variations, if caused by elec-
trostatic  charge, meant that the dissipator x^as undersized.
           Two new and larger polonium sources were then used to initiate
another series of experimental weighings  (data not given)„  Prior to each
weighing,  both sides of each filter were  exposed at a distance of one inch
from  these polonium sources.  After this  pretreatment, uniform weights of
± 4 (ig were obtained until there was a change in humidity.  When the
humidity remained within ±1.0 percent RH, the weight of a 47-mm Metricel
filter is  repeatable within about ± 15 M-g and that of a 142-mm Metricel
filter is  repeatable within about ± 150 u.g.  The larger size has approxi-
mately ten times the surface area subject to adsorption and desorption of
water vapor.

 Filter Media
           Two  types  of  polymeric membrane  filters were  selected for use
 in  the  determination of particulate mass by weighing.   Metricel DM 450
 membrane  filter  (Gelman Instrument Company, Ann Arbor,  MI, Part No. 64519)
 is  a  copolymer of  polyvinyl chloride and acrylonitrile, 0.45-nm pore
 size.   The filter  diameter was  142 mm.  The filter was  used in a filter
                                               2
 holder  with an active filtration area  of 125 cm  .  Flow rate, calibrated
 for each  batch,  was  about 7 cfm for one filter in the holder and about
 4.3 cfm for two  in series, with a pressure drop of about  10 cm Hg across
 the filter(s).   Face velocity at 4.3 cfm was  16,3 cm/s,
           Millipore  MF  AAWP 047 00 membrane filter (Millipore Filter
 Corporation, Bedford, MA) is a  mixed cellulose ester, reportedly pro-
 pionate-butyrate,  0.8 nm pore size.  Filter diameter was  47 mm, and active

-------
                               A-50
                          2
filtration area was 9.6 cm .   Flow rate calibrated for each batch was
about 1.0 cfm for one filter and 0.7 cfm for two in series in the holder,
with a pressure drop of about 10 cm Hg across the filter(s).  Face
velocity at 0.7 cfm was 34.4 cm/s.
          The membrane filters were chosen because they were expected
to be low in reactivity toward acidic constituents (e.g.,  802) i-n tne ex-
haust, and resistant to abrasive losses during insertion in and removal
from the filter holders.  Agreement in results from simultaneous parallel
samples taken with both types indicated probably negligible effects
on weight gains because of filter holder configuration, face velocity of
the filtered stream, and chemical composition of the filter medium.
          Filter-holder flow rate was controlled by an orifice downstream
of  the filter.  Orifices for each filter holder were calibrated with the
proper filters  in place, using a dry gas meter, and at the same manifold
vacuum as was used during  the actual sampling runs.  The calibrations were
repeated several times during the program to determine that no substantial
changes in flow rate were  taking place.
           The  SO  content  of the  automobile exhaust was  determined,  in
 order to  estimate  whether  the potential weight  change of a reactive filter
would be  significant if the  sulfur in the  fuel  (0.036 wt   %)  were con-
 verted  to SO-  followed by  reaction with the filter.   It  was found that the
 S02 in  the exhaust diluted in the tunnel (^30:1)  contained approximately
 0.2 ppm S0?.   A 22-liter  sample contained  by analysis 10.5 micrograms  of
 S0_.   In  tests that use a  4.0 cubic meter  sample volume,  SO could
 account  for  2,000  micrograms weight increase of the  filter if  all the  S0«
 reacted with the filter.   This  is about the same as  the  weight of particles
 collected  from unleaded fuel during one LA-4 cycle so that the effects of
 reactions  between  filter  and any  substantial part of  the SO,, would invali-
 date the  particle  weight  data.
           On the other hand,  these neutral filter media  change weight  with
 humidity  changes and by adsorption of exhaust constituents. This disad-
vantage was  compensated by using  a  second  filter disc  as backup  in each  fil-
 ter holder,  and by applying  the change in  weight of  the  backup filter  as a
 correction to  the  measured weight change of the primary  filter.

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                                 A-51
Pattern of Sampling for Particulate Matter

          Four simultaneous samples were filtered for determination of par-
ticulate mass in almost all experimental tests:   two were 142-mm Metrical
 filters in stainless steel holders with conical approach sections, and two
 were 47-mm Millipore filters in holders of similar configuration.
           Two filter discs were placed in each  holder,  with the primary
 filter for particle collection, and the backup  filter as a weight-change
 control.  The weight change in each filter following exposure was  determined
 by separate weighings.
           The efficiency of these filter media  is so high that no  solid
 particulute matter can penetrate to a  backup  filter in the same holder.
 Therefore, the algebraic difference between the weight changes of  the primary
 and the backup  filter after both have been exposed in series to the same
 sample stream is a measure of the weight of solid particulate collected on
 the primary filter;  It is assumed that the gas stream is not significantly
 changed in composition by passage through the first filter and that weight
 changes from adsorption or desorption of its constituents on the filter
 structure are the same in each of the two filters.

                Experimental Results — Supplementary Data

 Test Conditions

           Table A-9 summarizes pertinent laboratory conditions and Table A-10
 gives calculated air-fuel ratios for the modified and standard LA-4 cycle
 test runs.  All the runs are included where essentially complete data
 were acquired.  Problems were encountered on Runs 4-10 and 4-18, which are
 noted on the tables.  Any significant deviations in the test conditions
 from target or normal values are described in footnotes of the tables.
           The A/F ratios of Table A-10 were determined from CO, CO , 0
 and HC measurements made in the tailpipe at steady-state conditions of 0,
 35, and 50 mph immediately following each test  run.  Each entry is the mean
 of three values determined from CO-0 , CO-CO ,  and 0 -CO , using the•
 .Eltinge. charts.  C0_ and 0_ were corrected for  HC.  A fuel H/C ratio of
 1.90 was assumed.

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                                          A-52
       TABLE A-9.  LABORATORY AND OPERATING DATA  FOR  MODIFIED AND STANDARD LA-4 CYCLE RUNS
Run No.
           Run-in,
                  Soak      Avg.  Soak	Laboratory	  Chamber   .     Run
                  Tir.c,     Temperature, Tfiiporature,    Humidity,    Humidity   ,   Length
                                Y
                                             K
                                                         Kr/lh dry
                                    Unleaded Fuel Tests
                                                                         percent:
4-10
4-11
4-12
4-13
4-16,
4-17^
4-18v
4-20
4-25
4-26
5-15
5-16
5-17
5-18
5-19
(f)
              42
             101
             120
             139
             109
             117
              60
             126
             122
             111
116
122
120
124
121
                  19
                  16
                  17
                  16
                  17
                  14.2
13.6
18.1
14.7
17.0
             (h)



             (h)

             (h)
69
68
72
70
70
70
            71
            70
            69
            68
            74
            70
                      17.1
                      16.7
                      17.1
                      16.8
                      15.7
                      (h)
  Leaded Fuel Tests

70          73
70          77.5
70          71
70          73

 Unleaded Fuel Tests

70          70
70          70
70          69
70          71
70          71.5

  Leaded Fuel Tests
37
29
35
31
48
48
                                                          75
                                                          68
                                                          37
                                                          44
                           37
                           40
                           35
                           39
                           46
28, .
33<8)
30,
37
41
                                                                            (g)
                                                                            (8)
                                       50
                                       35
                                       30
                                       26
              (8)
              (8)
            30
            30
            29
            27
            27
                                                               23.41
                                                               23.25
                                                               23.37
                                                               23.28
                                                               23.26
                                                               22.75
           25.13
           23.53
           23.37
           23.35
           23.37
           23.40
           23.40
           22.83.
           22.78
5-9
5-10
5-21
5-22
121
114
108
118
16.7
17.2. .
15.9
16.7
70
70
70
70
77
72
71
7S
59
67
51
62
31,,,.
42(f)
29
34
23.40
23.42
23.40
23.40
(a)  Generally includes about 100 miles on the MV1-1A Durability Driving Schedule and two
     consecutive LA-4 cycles.

(b)  As measured by wet and dry bulb thermometers just before start of the test run.

(c)  Time-sequence clock on to clock off 5 seconds after vehicle stops on last mode, unless
     otherwise noted, this time period also represents the interval the exhaust-gas diverter
     valve opens the tailpipe to the tunnel and the interval of tunnel-bag sampling.

(d)  The tunnel-bag sampling was inadvertently continued for about 40 seconds after the
     clock was stopped, sampling dilution air only.  The mass gaseous emissions have been
     corrected for a 3 percent dilution; the run-in mileage for this test was also low.

(e)  The engine killed when put in gear, was restarted and test continued to completion with
     about 104 seconds additional time before first mode started.  The run-in mileage for
     this test was also low.

(f)  Tests 4-17, 5-18, and 5-19 arc standard FTP-cycle tests.

(g)  The chamber humidity on Tests 4-10, 4-12, 4-16, 4-17, 4-18, 4-20, and 5-10 was above
     target of 30 percent.
(h)  The soak time on Tests 4-17, 4-18, 4-25, 5-19, and 5-21 was less than the target of
     16 hours, but all were greater than the FIT requirement of 12 hours.

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                               A-53
      TABLE A-10.   AIR-FUEL RATIOS DETERMINED FROM STEADY-STATE
                   EXHAUST-GAS ANALYSES AFTER EACH RUN
Run No.

4-10
4-11
4-12
4-13
4"16(c)

4-18
5-16 / \
5-17)8(
5"18( )
5-19*1

5_9(g)
5-21
5-22

Idle
Unleaded
14.90
14.29
14.23
14'22(e)
15-01(e
14. 85^
Leaded
15.33
14.49
14.21
13.96
Unleaded
15.10$
14.97
14.66
14.64) ?
14.61(d)
Leaded
S:SS>
14.32
15.24
Air-Fuel Ratio
35 mph
Fuel Tests
15.23
15.46
15.39
15.43
15.26
15.38
FueJL Testa,
15.22
14.91
15.07$
15.02U;
Fuel Tests
15.60
15.57
15.59
15.59
15.48
Fuel Tests
15 31(h)
AJ * J J-/u \
14.79(h)
14.85
14.60

50 mph

tfm
15.15
15.02
15.10
15.03
15,16

14.90
l4'90fM
14.82(h)

15.20
-------
                                 A-54
          Table A-11 gives the overall dilution ratio in the residence
chamber of the samples taken for measurement of mass concentrations.  The
target for overall dilution ratio was 300.  Experimental variations are
caused by differences in the amount of filtered air held in the residence
chamber by partially collapsing the flexible walls.  The tunnel sample was
then injected for the final dilution.  The variations in ratio shown in
Table A-ll are acceptable..

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                                A-55
TABLE A-11.  DILUTION  RATIOS OF DILUTED EXHAUST  IN  RESIDENCE CHAMBER
             FOR MODIFIED AND  STANDARD LA-4 CYCLE RUNS
Run No.
4-10
4-11
4-12
4-13
4-16
4-17(b)
4-18
4-20
4-25
4-26
Overall
Dilution
Ratio(a)
__
223
284
278
268
293
278
262
271
252
Run No.
5-15
5-16
5-17
5-18

5-9
5-10
5-21
5-22
Overall
Dilution
Ratio
265
275
325
325
325

268
297
332

(a)   Calculated using average dilution ratio in tunnel of 31.9 and
     measured dilution ratio from tunnel to chamber using HC values.

(b)   Tests 4-17,  5-18, and 5-19 are standard LA-4 cycle tests.

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