EPA/AA/CTAB-89-01
                        Technical Report
           Resistively  Heated  Methanoi  Dissociator  for
                   Engine Cold Start  Assist  -
                        Inter im Report  I I
                               by
                      Gregory  K.  Piotrowski
                          February  1989
                             NOTICE

     Technical Reports  do not  necessarily  represent  final  EPA
decisions or positions.   They are  intended  to present technical
analysis  of  issues  using  data which  are  currently  available.
The purpose in the release of such reports  is to facilitate the
exchange  of  technical  information and  to  inform  the  public of
technical developments which may form the basis  for  a final  EPA
decision, position or regulatory action.

              U. S. Environmental  Protection Agency
                   Office of  Air and  Radiation
                    Office of Mobile Sources
              Emission Control Technology Division
           Control Technology and  Applications Branch
                       2565 Plymouth Road
                   Ann Arbor, Michigan  48105

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   \   UNITED STATES ENVIRONMENTAL PROTECTION AGENCY

   1°                ANN ARBOR. MICHIGAN 48105
                                                        OFFICE OF
                                                     AIR AND RADIATION
MEMORANDUM
SUBJECT:   Exemption  From  Peer  and  Administrative Review
FROM:      Karl H.  Hellman,  Chief
           Control  Technology  and  Applications  Branch

TO:        Charles  L.  Gray,  Jr., Director
           Emission  Control  Technology  Division
     The attached  report entitled, "Resistively  Heated  Methanol
Dissociator  for  Engine Cold  Start  Assist -  Interim  Report  II,"
(EPA/AA/CTAB/89-01)  describes   the   evaluation   of  a  methanol
dissociation  catalyst  that provides  a cold  start assist for  a
light-duty   methanol   engine.    Methanol   was   boiled  in   a
steam-heated  vessel,  superheated  and  passed  to a  dissociator
which  made  use  of  resistively  heated  porous  silicon  carbide
technology.   The  catalyst  used  for   the methanol  dissociation
reaction was  a noble  metal/rare  earth formulation developed  by
Nissan Motor Corporation.

     Since  this  report is concerned  only with the  presentation
of data and  its  analysis and  does not  involve matters  of policy
or   regulations,   your   concurrence    is   requested   to  waive
administrative review  according to the policy outlined  in  your
directive of April 22, 1982.
   Concurrence
. Xx>^ ~w
• /_--^_	  '	
               Charles L. Gra'y,Jr/. ,/Dir.,  ECTD
                                 / r
Nonconcur rence:	Date
               Charles L. Gray, Jr., Dir.,  ECTD

cc:  E. Burger, ECTD

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                        Table of Contents


                                                          Page
                                                         Number

 I .   Summary	   1

 II.  Introduction   	   2

 III. Program Design   	   3

 IV.  Dissociator Operation  	   3

V.   Supporting Equipment   	   4

VI.  Discussion                   	   5

     A.    Bench Test Experiments   	   5

     B.    Cold Start Experiments   	   8

     C.    Examination Of Substrate Following Testing   .  10

VII. Test Highlights	11

VII I.Acknowledgments	12

IX.  References	13


APPENDIX A - Dissociator Element Specifications  ....  A-1

APPENDIX B - Hydrogen Content Determination  	  B-1

APPENDIX C - Test Engine Specifications  	  C-1

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 I.    Summary

      A catalyst specifically formulated for the dissociation  of
 methanof   to   hydrogen  (H>)  and   carbon   monoxide  (CO)  was
 evaluated  for  the  application  of  a  cold  start   assist  for  a
 light-duty  methanol-fueled  engine.   The  dissociated  methanol
 generating  system consisted  of  a steam-heated methanol boiler,
 a  gas superheater,  and  a  catalyzed  dissociation  element.  The
 dissociation   element   substrate  was  resistively  heated  and
 constructed primarily  from  fibrous  silicon carbide.

      The objective of  this  experimentation  was to determine the
 ability  of   the  catalyst  to  facilitate   the dissociation   of
 methanol,  and  to  start and  idle  a 4-cylinder  engine  on the
 product gas from  the dissociator.

      Hz/CO  product  gas yield  varied between  13 and 15 percent
 for   a  feed  flowrate   of   2500  grams  of  methanol  per   hour.
 Dissociator  yield was  not  a  function of  superheater  feed gas
 temperature,  for  feed gas  temperatures  into the  dissociator
 between  400°   and 700°F.   Power  to the  dissociator  was kept
 constant at 345 watts during  this testing.

      H;,  CO,   non-dissociated   methanol,   and  possibly   other
 reactor products  from  the  dissociator were piped to the exhaust
 gas  recirculat ion port of  the  test  engine.   This  product gas
 mixture  served  as  the fuel  supply during  the  engine   start
 experiments;  the  stock  methanol injectors  on the  test   engine
 were  disabled prior  to this testing.

      At an  engine temperature of  73°F the  product  gas mixture
 easily started  and  idled the test  engine.  The  combination  of
 hot   methanol   vapor  and  H2/CO  may  be  too  rich  to   enable
 extended  idle,  however;  flowrates  between  1800-2500  grams per
 hour  of  feed  methanol  are  difficult to control  with  the test
 apparatus.

      It is difficult to quantify emission  control  benefits from
 the  use  of dissociated  methanol compared  to M100 liquid fuel
 using  the  dissociation system described  in this  report.   Only
 13 to 15 percent  of  the feed flowrate of 2500 grams of methanol
 per hour was  dissociated  to  H,,  and CO.  Any  emissions control
 benefit may  be minimized  by  the  presence  of  large amounts  of
 unconverted   liquid   methanol   in    the   H^/CO  fuel   stream.
Additional  testing should be  conducted  with a fuel  mixture much
 richer  in   dissociated product   than M100  in  order  to more
properly define  the difference  in  emission  levels  between the
 two fuels at cold start.

     No  coking  was  observed  on  the  walls  of   the  ceramic
substrate following  this evaluation.   Traces of coke were  found
at  the  interface   between  the   silicon   carbide  substrate,

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                               -2-
 stainless   steel   wool   gaskets,  and   the   stainless   steel
 electrical  contacts.   Hot spots caused by areas of high current
 density  along   this  interface  may  have  contributed   to   this
 localized  coking.

 I I.   Introduct ion

      Light-duty  M100  neat methanoI-fueled  engines are difficult
 to  start and  run  in  cold weather  because  of  the  high boiling
 point  of  methanoI,  methanol's  high  heat  of  vaporization  (5.5
 percent  of  the  heat  of  combustion  compared  to  less   than   1
 percent  for gasoline),   and  the  increased  fuel  flow  needed for
 methanol   (about  double  that   of  gasoline).   Gasoline-fueled
 engines  start with  less  difficulty  under  the  same  conditions
 partly because of  the easily  ignitable  light  ends  of  this  fuel
 such   as  butanes,   which   are  vaporized   at  relatively  low
 temperatures.

     Some   state-of-the-art   methanol   engines    require   the
 addition    of    gasoline  to   the   fuel    to   improve   their
 startabiIity.[1]  Other  methanol engines utilize  separate  cold
 start  systems relying   on  gasoline  or  propane for  cold  start
 assist.[2,3]   Finally,   some  researchers  have suggested   that
 stratified-charge combustion will produce reliable  cold starts
 of  a  neat methanol-fueled  engine at   relatively  low  ambient
 condi t ions.[4]

     Methanol  may  be  catalytically  decomposed  to  hydrogen and
 carbon monoxide  gases.   Hydrogens'  higher  flame speed and  lower
 boiling point may make it an ideal cold start  fuel.

     Methanol dissociators using resistively  heated ceramic and
 metal  technology  for  substrates have  been  evaluated  by  EPA for
 their  use   in  assisting  the  cold  start  of  methanol-fueled
 engines.[5,6,7]   The  noble  metal  catalysts  employed  in   these
 efforts were  platinum and a platinum/palladium mixture.   These
 catalysts,   however,  did  not provide substantial  yields  of H2
 and CO at  lower converter gas temperatures.

     A   significant   problem    noted  during  these   earlier
 evaluations was  the formation  of soot   in  the  superheater and
 dissociator sections.[6]   Coke  formation appeared  to  positively
 correlate  with  operating  temperature  in  the superheater  and
 dissociator.  Temperatures  in  excess  of  900°F  invariably led to
 sooting of the superheater.

     Other  researchers working with  methanol  dissociation  have
noted  this coking. [8,9]    One  solution   to  this problem is the
use of a  catalyst  that  promotes  the dissociation reaction at
 lower temperatures (less than or equal to 570°F).

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                               -3-
      Representatives  of  Nissan  Motor Company, Ltd., presented  a
 summary of  their  experience  with  the  "Methanol  Reformed  Gas
 Engine" to  EPA  on  March  13,  1987. [10]    One  part   of   this
 briefing concerned the  results  of screening candidate  methanol
 dissociation catalysts.   Some   of  these  catalyst   formulations
 and their  application processes  have been patented.[11,12,13]

      The catalysts referred to  above  utilize active components
 from the noble metal, rare earth  and  titanium families applied
 to granular  or monolithic alumina substrates.  A portion of  the
 March  13,   1987   briefing  to   EPA  concerned  a   confidential
 presentation  of   catalyst  activity   as  a  function  of   bed
 temperature  for specific formulations  of the catalyst materials
 above.   This  data  indicated  that several  Nissan   formulations
 could  provide  substantial  dissociative  activity  at  reactor
 temperatures below 600°F.

      EPA  sought  permission  from  Nissan   to  use  a   specific
 dissociation  catalyst  formula   [14]    on   a  silicon  carbide
 substrate  similar to  those  tested  in  references  5  and 6.  This
 permission   was   granted;[15]  Engelhard  Industries  agreed   to
 cooperate  in  this   joint  effort  by   catalyzing   the  silicon
 carbide substrate using  the Nissan formulation.   An agreement
 to provide  Engelhard  with access  to  the  pertinent   catalyst
 information  was   then  reached  between  Nissan and  Engelhard  to
 facilitate this work.

 III.  Program Design

      The testing was conducted in  two separate phases:

      1.    Bench  testing; and

      2.    Cold start  and emissions testing  at 73°F  conditions.

      The  bench  test   phase  consisted  of determining   catalyst
yield    at     control led     steady-state      feed     methanol
flowrate/temperature  conditions.  The  cold  start   testing  was
conducted  to determine whether  a  4-cyUnder,  1.8-liter engine
could  start  and  idle on  the  product  gas from  the dissociator
with  no  supplemental   liquid  methanol  fuel.   If  it  proved
possible to  start and  idle  the  test engine on the dissociator
product  alone,  the engine would then  be emission  tested  using
alternately  M100  liquid  methanol  from  a  conventional  fuel
injection system and product gas from the dissociator.

IV.  Dissociator Operation

     Methanol  may  be  dissociated   to  hydrogen   and  carbon
monoxide via  the reaction:

           i  >	  2H2 < g > +• C0( g >

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                               -4-
      The  dissociator described below accomplished this  reaction
 by  a  three-step  process.   First,  methanol was  vaporized in a
 boiler  and  the  vapor  stream  flowed  to  a  superheater.   The
 vaporized  methanol  was then superheated  and the hot gas  passed
 to  a  catalyzed and heated dissociator.   The hot  methanol vapor
 was  dissociated  in  this   final  stage and  passed  into  the test
 engine  intake  manifold.   A detailed  description of each part of
 the process  is given below.

      A.    Boiler Unit

      The  boiler  was a  5-gallon  capacity, type  316 stainless
 steel  pressure  vessel.    The  vessel  was  fitted  with  a steam
 heating   coil,  pressure  relief   valve,   liquid   temperature
 monitor,  and   pressure   gauge.   The  boiler   was   filled  with
 approximately  three  gallons of methanol  prior to each test and
 sealed;  no provision  was made  for adding fuel   to  the  vessel
 following the  commencement of a test.

      Liquid  temperature  and  pressure inside  the  boiler were
 maintained at  approximately  190-195°F and  30  psig  respectively
 during  testing.  Fuel  feed  rate  was determined  indirectly; the
 filled vessel  was carefully  weighed prior  to  and  at the end of
 testing, and the  test process timed.

      B.    Superheater

      The superheater was  constructed from  a 3-foot-long  section
 of 1-inch diameter 304 stainless  steel  pipe.  This pipe  section
 was   heated  by  wrapping  it  with  a  ceramic  bead  insulated
 nichrome   wire  heater   that   utilized   120-volt   alternating
 current.  Power to the heater was controlled by a  thyristor.

      C.    Catalytic Dissociator

      The  superheated  methanol  vapor  passed  through a  porous
 silicon  carbide  substrate  which   had   been   coated  with  the
 catalyst to be evaluated.  The substrate was  resistively  heated
 by  passing  direct current  through  it.   This  catalyzed  heater
 acted as the methanol dissociator.

     The  substrate   was   shaped   in   the   form  of  a   hollow
 cylinder.  Methanol  vapor  flowed radially  through  the  porous
 heater walls;   the dissociation  reaction  occurred  as the vapor
 contacted the  hot  catalyzed  walls.  Element specifications are
 given in Appendix A.

V.   Supporting Equipment

     H2  composition  in the  product  gas  mixture  was determined
by gas chromatography.   A GOW-MAC Model 69-550 gas chromatograph
was used, and  its operation  is detailed in Appendix B.

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                               -5-
          test engine used  for  this experimentation wa
          single-overhead   camshaft,   1.8-liter   di
          Details  and  engine   specifications  are  pr
          C.
     The test engine used for this experimentation was  a  Nissan
CA18E,   single-overhead   camshaft,    1.8-liter    displacement
engine.   Details  and  engine  specifications  are  provided  in
Append i x
      Emissions  characterized  as  hydrocarbons were measured with
 a  Beckman Model 400 flame  ionization detector.   A FID  response
 factor  of  76 percent was used.[16]

      Exhaust formaldehyde was measured using a dinitrophenyI-
 hydrazine  (DNPH)  technique.[17]    Exhaust   carbonyls   including
 formaldehyde  are drawn  through  DNPH-coated  cartridges forming
 hydrazone  derivatives.  These  derivatives  are  separated from
 the   remaining   unreacted   DNPH   by   high  performance   liquid
 chromatography    (HPLC).      A     spectrophotometer     in    the
 chromatograph   effluent   stream   drives   an  integrator  which
 determines formaldehyde derivative concentration.

 VI.   Discussion

      A.    Bench Test Experiments

      The  bench   test  experiments  were  conducted to  determine
 catalyst   yield    under    specific   inlet   gas   temperature
 conditions.  Catalyst  yield  is  defined  as  the  percentage  of
 feed  methanol converted to H2 and CO gases.

      The  methanol   flowrate  from  the boiler during  dissociator
 operation  varied between  2400-2500 grams  per  hour;   this  was
 calculated to be close to  the  flowrate  necessary to start and
 idle  an   engine  of   the   same   displacement    as   our   test
 engine.[18]  The temperature  of  the  methanol   vapor  into the
 dissociator was  an  important parameter because  it indicates the
 degree of superheating for a given methanol  flowrate.

     Methanol was heated  in the  boiler  to  195°F and passed to
 the   superheater.    Current  to    the  heating    coils   in  the
 superheater was controlled to superheat the methanol  vapor to
 various temperatures  over  the range 400°F to 700°F.   Power to
 the  dissociator  was  supplied   by  a  Power  Mate  alternating
 current   to  direct   current  converter;  this  device  allows  a
maximum power output  of  1000 watts.   The  maximum  power  level
attained with the dissociator was 345 watts;  15  amps current at
23 volts.  Electrical  resistance  across  the dissociator and its
electrical leads was measured at  2.5 ohms.

     Table 1  presents  a   summary  of  test  conditions  for  the
catalyst yield evaluation.

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                                -6-


                              Table 1

         Test  Conditions For Catalyst  Yield Determination
Test cell  temperature

Boiler  liquid  temperature

Boiler  pressure

Methanol  flowrate from boiler

Gas temperature out of superheater

Gas temperature out of dissociator

Power to  dissociator
73°F

195°F

35 psig

2400-2500 grams/hour

410-710°F

316-365°F

345 watts
     Tedlar  sample bags  were( used to  collect the  product  vapor
from  the dissociator;  the  collected  vapor  was  then  fed to  the
gas   chroma tograph   by   evacuating   the  sample   bag   to   the
chromatograph  column.   Unreacted  methanol  vapor  was  condensed
in  the   sample  bag  and  volumetrically  measured  to ensure  its
inclusion  in the  yield calculation.

     A  graph  of   superheated  vapor   temperature  versus  product
yield is given  below in Figure 1.
                                FIGURE 1
                     METHANOL DISSOCIATION CATALYST YIELD-
                   VERSUS GAS TEMPERATURE INTO DISSOCIATOR
                          — H2/CO PRODUCT YIELD
           16
             YIELD IN PERCENT
           14

           12

           10

           8

           6 -

           4 -

           2
             -i—i—i—i—i—i—i—i—i—i—\—i—i—i—i—i—i
           400
                  460
                        500     660    600    660

                       INLET GAS TEMPERATURE (DEG. F)

        •2500 G/HR METHANOL FEED FLOWRATE
    700

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                               -7-
     Product  yield   proved   to   be  only  slightly  dependent  on
dissociator  inlet  gas  temperature.   A  300  degree   increase  in
inlet  gas  temperature from 410°F  to  710°F,  increased the methanol
conversion rate only  2 percent,  from  13  to  15 percent.

     The data  in  Figure 1 suggests that  the yield may  be limited
by   factors  other  than  energy   supplied   by  the  superheater.
Effective  substrate  surface  area may   be  a  problem  here;  the
fibrous  silicon   carbide  may  not  provide  a  surface  area  as
effective  for  the catalytic  activity  required as  alumina-coated
monoliths  or  packed  bed ceramic  substrates,  for  example.   Vapor
flow  inside  the  dissociator  was  not  studied;  flow  through  the
catalyzed  fiber walls may occur  in such  a  manner  as  to make less
than  optimum use of  the  total  catalyzed  surface  area.   Flow
conditions  through the  walls may allow certain  sections  of  the
            exposed   to  higher  volumetric   flowrates  of   the  hot
            other  sections (uneven flow  distribution  through  the
             The  flow of vapor may also cause certain sections of
                        fibers  to  experience   greater  catalytic
                       sections   of  the  same   fibers  (geometry
                       conditions  on  parts  of  individual  fibers).
                      be   limited   by  an  insufficient  amount  of
catalyst material  coated  on  the  substrate  to carry  the  reaction
to a  greater  degree  of  completion  in  the   residence  time  of  the
gas in the dissociator.
wal I   to  be
vapor  than
substrate).
individual  substrate
activity  than  other
resulting in  stagnant
Activity  might
also
     Power  to  the  resistively  heated  dissociator  substrate  was
kept constant at 345 watts  during  the testing.  High power levels
for dissociator operation  were  considered  desirable  in  order to
provide  sufficient  energy  for  the  endothermic  dissociation  to
proceed to a high degree of  completion.
     Oissociator  outlet  gas
sampling.  A  graph  of gas
temperature at the outlet of
                             temperature  was also  measured during
                             temperature  at  the  inlet  versus  gas
                             the dissociator is  given in Figure 2.
                               FIGURE 2
                       GAS TEMPERATURE AT DISSOCIATOR
                    OUTLET VERSUS INLET GAS TEMPERATURE*
          400
          300
           200
           100
             OUTLET GAS TEMPERATURE (DEG. F)
            400    460    500    660     600     660    700    760
                       INLET GAS TEMPERATURE (DEG. F)

        •2500 G/HR METHANOL FEED FLOWRATE

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                               -8-
      Outlet  gas   temperature   from
 positively  correlate with  increases
 the   superheater.    Instead  outlet
 relatively constant  at approximately
                           the  dissociator  did  not
                           in  temperature  of gas from
                           gas  temperature  remained
                          350°F during testing.
      Energy  supplied  by the resistively heated substrate may be
 a   very   important   limiting  factor   for   the   dissociation
 reaction.   Karpuk  [19],  in  a  private  communication  to  EPA,
 calculated a power requirement of  2256  watts to dissociate 2000
 grams  per  hour  of  methanol .    Our   calculations   of  this
 requirement  show  it  to be  2230  watts,  essentially  the same.
 Significant  heat  transfer  from  the dissociator housing to the
 atmosphere  may  be  occurring  despite  our  efforts  to  insulate
 this  housing.   If  the endothermic reaction  is power limited,  it
 may  be necessary  to reduce  the  feed  flowrate of  methanol  to
 improve  percent product  yield at  lower temperatures  with the
 current dissociator system.
     B.
Cold Start Experiments
     A  cold  start  of  the  73°F  overnight-soaked  engine  was
attempted  using only  the product  gas from  the  dissociator  as
the  fuel  source.    (Prior  to   testing  the  engine  main   fuel
injectors  were  disconnected.)   Test  conditions  are  given  in
Table 2.

                             Table  2

           Test Conditions For Cold Start Experiments
Test cell temperature

Boiler liquid temperature

Boiler pressure

Methanol  flowrate from boiler

Gas temperature out of superheater

Gas temperature out of dissociator

Power to dissociator
                                 73°F

                                 190-195°F

                                 20 psig

                                 2400 grams/hour

                                 450 °F

                                 335°F

                                 345 watts
     Approximately  12  feet  of  plastic  tubing  connected   the
dissociator  to  the  EGR  port.   A  valve  to  allow  emissions
sampling and  a flame arrestor  were also  located  in this  line.
These  restrictions,  however,  did  not  combine  to  reduce  fuel
flow   to   the  point  that   engine   performance   at  idle   was
noticeably affected.  Although  the  fuel  entry  passageway  to  the
combustion chambers was not  standard (via EGR chamber to  intake
runners) it proved  sufficient to allow a  start and  idle at  the
cond it i ons i n Tab Ie 2.

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                               -9-
      Product  gas  from the dissociator  was fed  to  the EGR  port
 for  3 seconds prior to a crank attempt.   The engine  immediately
 started.   The  idle  was  rough,  however,   possibly  signifying  a
 fuel/air  imbalance;  spark from  the ignition system was present
 during crank  and  run periods.  Wetting  of  the plugs was noticed
 following  rough  idle periods  that ended with engine stalls.

      The  engine  may  be  operating  in  an   improperly  rich  mode
 during  an  extended idle.  Heating  of  the  boiler,  superheater,
 and  dissociator  cannot  be  regulated  in  a  manner  that  would
 provide  instantaneous  changes in  fuel  flowrate  to accommodate
 changes  in fuel  flow requirements.   Dumping part  of the  fuel
 flow to the  stack scrubber  with  a  three-way  bypass  valve by
 hand was tried;  the response was improved, yet this  improvement
 was  not sufficient to prevent engine  laboring.

      Two other factors combined to  change  the fuel  mixture  from
 those  mentioned   in  reference  6.    First,   substantially   more
 H2/CO  was   produced  at  lower  temperatures  with   the catalyst
 tested here than  from other  noble  metal  catalysts evaluated at
 similar feed  methanol  flowrates.    Second,   a  practical, onboard
 methanol dissociator  would  not  be  provided  with  a  blanket of
 nitrogen or  other inert  gas  in  the  dissociator  to prevent
 undesirable  combustion  reactions  from occurring.    Previously
 N2 was  added  over the  boiler  to  prevent these  reactions and
 to act  as  a  carrier  gas to  increase the  quantity of methanol
 flow from   the  boiler.   It  was   recently  noticed   that   feed
 methanol flowrates similar  to the  rates   in  references 5 and  6
 could  be   attained   through  changes   in  boiler    operating
 temperature  and  pressure,   rather   than  with  the  addition of
 Nj .   These engine  tests were  conducted  without   the addition
 of   N2  to   better  simulate  actual  onboard  conditions.   The
 elimination of  this additional diluent N2 caused  the fuel/air
 mixture to  be somewhat richer than  the mixture  in references  5
 and 6.

     Emission  results  are  presented  in   Table  3.    Levels of
 emissions  characterized  as  hydrocarbons  and  formaldehyde  were
measured in  order  to  determine  whether   the   choice of   fuel
 systems  influenced pollutant emission  levels.  The  test cycle
was  a cold start  followed   by  a 5-minute idle.   HC  and   HCHO
 emissions  are expressed  in  average  rates of grams  per minute
and  milligrams  per minute,  respectively.    Oxides  of nitrogen
 (NOx) and  CO  emissions were  not  measured with  the M100  liquid
 fuel  system due to problems  with the analyzers.

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                              -10-


                             Table 3

         Emission Levels Over Cold Start and Idle (73°F)


                             HC       HCHO       CO        NOx
 Fuel System Configuration  (g/min)  (mg/min)   (g/min)   (g/min)

 Methanol  injectors          3.68      1.0        N/A       N/A
 functioning

 Oissociator fuel system     2.38      0.8       1.45      0.02


     Emissions  of  HC were  slightly lower  with  the dissociator
 system  than  from  the  injector-fed liquid  fuel system.   This
 difference may be due  to improved starting  performance caused
 by  the  methanol and  H2/CO  fuels  admitted  to  the  engine  in a
 hot  gaseous   state   rather   than  as  atomized  liquid.   HCHO
 emissions with the dissociator  were  relatively  unchanged  from
 liquid  fuel  system levels.   NOx  emissions  with the dissociator
 were 0.02 grams per  minute;  engine coolant temperature however
 did  not  exceed  110°F  during  the  test  cycle.   NOx  and  CO
 emissions with  the  liquid fuel  system were not  measured  due to
 problems with the analyzers.

     A  trend  toward  lower  HC and HCHO  emissions  with partial
 dissociation   of   the  methanol    fuel   was   observed.    These
 decreases  in  emissions  may  not  be  definitive,   however;   the
 engine was tested only three times  using  the  dissociator as  the
 fuel  supply  system.   Additional  testing  would  have  to  be
 conducted in  order to  more  properly  define  the difference  in
 emission levels.

     C.     Examination of Substrate Following Testing

     Following  the  cold start   testing,   the   superheater   and
 dissociator  were disassembled to  check for  signs of  coking  and
 subsequent   catalyst   poisoning.    This   particular   catalyst
 formulation    was  evaluated    in  order   to   determine    its
 effectiveness  during  operation   at   lower  temperatures  less
 likely  to promote  the  undesirable coking  react ion.[20]   Signs
 of  coking would obviously be  given serious  consideration  with
 regard  to catalyst   durability   given  the  limited  amount  of
 testing conducted here.

     The  walls  of  the  substrate were  visibly   free  of   any
 carbonaceous  matter;  no coking was  observed on  either  the inner
or  outer  walls of  the  hollow  cylinder.    Traces  of  coke  were
noticed  at  the  interface between the  nichrome  flame-sprayed
ceramic, the  stainless  steel wool gaskets,  and the  stainless
steel  electrical contacts.

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                               -11-
      Current  density  may  be uneven  across  the  flame-sprayed
 ceramic surface.   Several rust/corrosion  spots  were noticed  on
 the  flame-sprayed   surface;  any  unevenness   in   the   physical
 characteristics  of  the   interface  could  have  caused  areas  of
 increased   current   density   across  the  interface.    Areas   of
 higher   current  density  would  also   be  areas   of   higher
 temperature.     Temperature   was    not   measured    at    the
 ceramic-to-metal  interface.   It  is possible  that the  interface
 temperature   significantly   exceeded     the    measured    gas
 temperatures.   The  fiber substrates  are  very  porous;  it   is
 possible  therefore  that  some of the  dissociated CO contacting
 the  interface  was   brought   to  a  high   enough  temperature   to
 undergo decomposition  to  coke.[21]

      Earlier  in  this  report  it  was  stated   that  electrical
 resistance  across  the  dissociator,  to  include  its electrical
 contact system,  was measured at  2.5  ohms.  Resistance  over  the
 substrate   alone   was  measured  at   various  points   on   the
 flame-sprayed  ends  of   the  hollow cylinder.    These   measured
 resistances varied  between 2.0 and 10.5  ohms.

      This  variation in resistance  may  be  caused by  an  uneven
 flame  spray  on  the  ends  of  the  hollow  cylindrical  ceramic
 substrate.    Flame-sprayed   metal   absorbs  into   the   porous
 ceramic.    The  flame-spray   process   also  must  be   carefully
 controlled  to  prevent cracking of  the  sprayed  ceramic  surface
 because of  differences  in  thermal   expansion  coefficients
 between the  ceramic  and   the   metal.    The  ceramic-to-metal
 interface  should  be  improved to  reduce  the  possibility of  hot
 spots   developing  at  the  bond  surface  that  could   promote
 undesirable side chemical reactions.

 VII.  Test Highliqhts

      1.     The  catalyst  evaluated  converted  15  percent  of a
 stream  of   2400 grams per  hour  of  methanol  to H2/CO  gaseous
 fuel.   Temperature  of   the  feedstream   into  the  dissociator
 reactor was 410-710°F during this testing.

     2.    The dissociation  catalyst  substrate  was resistively
 heated; power was  supplied  to the dissociator  at a rate of  345
watts during  testing.   Gas temperature  out of  the dissociator
 remained  relatively  constant,  at  approximately  350°F during
 testing.    This  temperature  did   not  change   as   inlet   gas
 temperature  for   a   constant   mass  flowrate   feedstream   of
2400-2500 grams  per hour varied between 410-710°F.

     3.     A 1.8-liter  test  engine was  cold started  and  idled
on  the  product gas  stream from  the dissociator alone.   Extended
 idle  periods  were  characterized  by  rough engine  performance;
plug  wetting  was  noted  after   several  stalls.   The  engine
appeared to be operating  in  a very  rich  mode at idle  with  the
dissociator.  Methanol  flowrates  between  1800-2500 grams  per
hour  are   difficult   to   control   with  the  tested  dissociator
apparatus,  however.

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                              -12-
     4.    Pol lutant   emissions   from  the   test   engine  were
 measured  over  a cycle consisting of a cold start and a 5-minute
 no-load   idle  with the  dissociator  as  the  sole  fuel  source.
 Pollutants  characterized  as hydrocarbons  and  formaldehyde were
 measured  at  2.38  grams   per  minute  and  0.8  milligrams  per
 minute,  respectively.  CO and  NOx emissions over the same cycle
 were measured at 1.45 and 0.02 grams per minute, respectively.

     5.    No  coking  was  observed  on  the  walls  of  the ceramic
 substrate  following this  evaluation.   Traces of coke were found
 at  the   interface  between  the   silicon  carbide  substrate,
 stainless   steel  wool   gaskets,   and    the   stainless   steel
 electrical contacts.  Hot spots caused by  areas of  high current
 density  along   this  interface  may  have   contributed  to  this
 I oca Ii zed cok i ng.

 VIII.AcknowIedgmen t s

     The silicon carbide  substrate  used  in this experimentation
 was provided  by Coloroll,  pic.,  a United Kingdom  corporation.
 The  dissociation   catalyst  formulation   evaluated   here  was
 developed  by  the Nissan  Motor  Company,  Ltd.   The  catalysis of
 the   silicon   carbide   substrate   was   done   by   Engelhard
 Industries.  The test engine was also provided by  Nissan Motor
 Company,  LTD.

     The  author   appreciates  the  efforts  of  James  Martin,
 technician, Standards  Development and Support  Branch,  Emission
Control  Technology Division, who greatly  assisted  the  author
with this project.   Jim  was also  largely  responsible  for the
 setup of  the engine used for this testing.

     In  addition,  the   author   appreciates   the   efforts  of
Jennifer  Criss  and Marilyn Alff  of the Control  Technology and
Applications Branch,  ECTD,  for  typing,  formating,   and  editing
 this report.

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                               -13-


 IX.   References

      1.     "Development  of Methanol  Lean Burn  System," Katoh,
 K. Y.  Imamura, and  T.  Inoue, SAE Paper 860247, February  1986.

      2.     "Interim Report  On Durability  Testing of  Low Cost
 Catalysts   for  Methanol-Fueled  Vehicles,"  Wagner,  R.  and  L.
 Landman, EPA/AA/CTAB/TA/84-4,  August 1984.

      3.     "Using   Methanol   Fuels   In   Light-Duty  Vehicles,"
 Brown,  D. ,   F.  Golden, E.  Gons,  R.  Potter, SAE  Paper 872071,
 November 1987.

      4.     "Unassisted  Cold Starts  to  -29°C and Steady-State
 Tests  of  a  Direct-Injection   Stratified-Charge  (DISC)  Engine
 Operated On Neat  Alcohols," Siewert,  R.  and E. Groff, SAE Paper
 872066, November 1987.

      5.     "Evaluation  of  Coloroll  Methanol  Dissociator  For
 Cold Start  Assist Application," Piotrowski, G., EPA/AA/CTAB/
 87-08, December 1987.

     6.     "Resistively Heated Methanol  Dissociator  For Engine
 Cold    Start    Assist-lnterim    Report,"   Piotrowski,    G.,
 EPA/AA/CTAB/88-02,  March, 1988.

     7.     "Resistively Heated Metal  Monolith As A  Cold  Start
 Assist For  A Methanol  Engine - Interim Report," Piotrowski, G.,
 EPA/AA/CTAB/88-11,  December, 1988.

     8.     "Study of the  Methanol  Reformed Gas Engine," Hi rota,
 T., Japan Society of Automotive Engineers Review, March  1981.

     9.     "Dissociated   Methanol   Citation:    Final    Report,"
 Finegold,   J.,  G.   Glinsky,  and  G.  Voecks,  SERI/TR-235-2083,
 DE85000505,  August  1984.

     10.    Briefing  to C. Gray, Jr.,  U.S. EPA  by Nissan  Motor
 Company,  March 1987.

     11.    "High  Activity  Catalyst  For  Reforming Of  Methanol
And  Process  Of  Preparing  Same,"  Masuda,  K.  to Nissan  Motor
Company,   Ltd.,   United   States  Patent   No.  4,499,205,  dated
 February 12, 1985.

     12.    "Catalyst For  Reforming Of  Methanol  And  Process Of
Preparing  Same,"  Masuda,  K.  to   Nissan   Motor  Company,  Ltd.,
United States Patent No. 4,501,823, dated February 26, 1985.

     13.    "Catalyst For  Reforming Of  Methanol  And  Process Of
Preparing  Same," Eto, Y.,  to Nissan Motor  Company, Ltd., United
States Patent No.  4,511,673, dated April  16, 1985.

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                              -14-
 X.    References  (cont'd)

      14.    Letter  from He 11 man, K.  H.,  U.S. EPA,  to Kawajiri,
 H.,  Nissan  Research and Development,  Inc., February 16, 1988.

      15.    Letter   from  Kawajiri,   H.,   Nissan   Research  and
 Development,  Inc., to  Hellman,  K.  H., U.S. EPA, April 4, 1988.

      16.    FID   Methanol   Response,  Memo,   Edward   A.   Barth,
 OAR/OMS/ECTD/TEB, Ann  Arbor, Ml, August 1987.

      17.    Formaldehyde Measurement  In  Vehicle Exhaust At MVEL,
 Memo, Gil key, R. L., OAR/OMS/EOD,  Ann Arbor, Ml, 1981.

      18.    Dissociated Methanol Fuel  Requirements  to Start  A
 Four-Cylinder   Engine,   Memo   from   Gregory  K.   Piotrowski,
 OAR/OMS/ECTD/CTAB, Ann Arbor, Ml,  1986.

      19.    Private Communication,  Karpuk, M.  E.,  to  U.S.  EPA,
 1987.

      20.    "Engine  Cold   Start   With   Dissociated  Methanol,"
 Greiner,   L.  and   E.   Likos,   Proceedings  of    the   Third
 International Symposium on  Alcohol Fuels Technology,  May 29-31,
 1979.

      21.    "Dissociated  Methanol   Test  Results,"  Finegold,  J.
G., and J. T. McKinnon, SERI/TP-235-1582, April 1982.

      22.   Fundamentals p_f  Gas Analysis  by  Gas Chromatography,
Thompson, B., Varian Associates, Inc., Palo Alto,  CA, 1977.

     23.   Basic Gas   Chromatography, McNair,  H. ,  Bonelli,  E.,
Consolidated Printers, Berkeley, CA, 1968.

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                           APPENDIX A
               DISSOCIATOR ELEMENT SPECIFICATIONS

     The  dissociator  substrate  consists  of   a  highly  porous
ceramic to which  electric  current is applied.  The  fluid  to be
heated  is passed  through  the void spaces in the material.  Heat
transfer  is  encouraged by the  very  large  surface  area  of  the
ceramic  (the material  contains  greater than  80  percent  void
space).
     Specification   ranges   for  certain  properties   of   the
material  used  in  the  dissociator are  given below.   The exact
specifications for the  dissociator  material are  proprietary to
the manufacturers  of  the  elements,  Coloroll,  pic.,  Havenside,
Boston,  Lincolnshire, U.K.
     	Property	   	Range of Values	
     Power density                       10-1600 W/cm3
     Normal  range                        10-300 W/cm3
     Power dissipation                   0.01-0.75 W/cm2
     Heatup/response  time                 Milliseconds
     Heat  transfer surface/volume        400-750 cm2/cm3
     Operating temperature                Up  to 1000°C
     Material  density                    0.1-0.5 gin/cm3

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                           APPENDIX B

                 HYDROGEN CONTENT DETERMINATION
Background

     The  basis   for   gas  chromatographic  separation  is  the
distribution  of   a  sample  between  two  phases.   One of  these
phases  is  a  stationary bed,  and  the  other  is  a  gas  which
percolates  through  the  stationary bed.    An  inert  carrier  gas
carries   the   components  to   be  separated  through  a  column
containing  the stationary phase.  The active component of  the
stationary  phase  selectively  retards  the  sample  components
according to  their  distribution  coefficients,  until  they  form
separate  bands in the  carrier gas.  These component bands leave
the column  in  the gas  stream and are recorded  as  a function of
time by a detector.

     If  the stationary  phase is  a  solid, this particular  gas
chromatographic   technique   is    referred   to   as   gas-solid
chromatography.  Common  packings  used are  silica  gel, molecular
sieve and charcoal.  Gas-solid chromatography was   used  in  this
experimentation,   and   the  details of  the  procedure  are  given
below.    More  complete   explanations  of   gas   chromatographic
technique are provided by Thompson and McNair.[22,23]

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                           APPENDIX B

             HYDROGEN CONTENT DETERMINATION (CONT'D)

 Specificat ions:
 Chromatograph model

 Detector:

   Operating principle
   Temperature control
   Carrier gas
   Detector elements
   Noise
   Drift

 Injection:

   Number of ports
   Control

   Operating temperature

 Column Oven:

   Temperature range
   Control

 Co Iumn:

 Gas flow system:
The rmaI  conduc t i v i t y
  bridge control:
Electrical :

  Power requirements
  Circuit breaker

Physical:
 GOW-MAC Model  69-550
 Thermal  conductivity type
 Ambient  to  300°C
 N2
 Four  (4)  rhenium tungsten elements
 10-micro  volts  maximum
 40-micro  volts/hour  maximum
Two
Solid-state,  variable-voltage
  phase control
Ambient to 300°C
Ambient to 300°C
Solid-state time apportioning

5' x 1/4" molecular sieve

Dual-column with dual-inject ion
ports and exits

Continuous current adjust 50-300
mA.  Bridge zero adjust.
Attenuator for bridge output, 10
posi t ions to 512.
105-125 volts, 50/60 H,
7 amps

Two-section construction.  Upper
section houses column oven,
detector and vaporizers.  Lower
section contains power supply,
bridge control circuit and
temperature controllers.

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                           APPENDIX B

             HYDROGEN CONTENT  DETERMINATION (CONT'D)


Compressed Gas Auxiliaries:

  Zero gas                    N2
  Span gas                    40 percent H2/60 percent N2

Output:

  Stripchart recorder         So I tech model 3318

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                           APPENDIX C
                   TEST ENGINE SPECIFICATIONS
Manufacturer
Basic engine designator
Displacement
Cylinder arrangement
VaI vet rain
Combustion chamber

Bore x stroke
Compress i on ratio
Compression pressure
Fuel control system

EGR
Valve clearance
Idle speed
Eng i ne oil

Fuel
Engine cranking speed
 Nissan  Motor  CO.,  LTD.
 CA18E
 1809 cc
 4-cyIinder,  in-Iine
 Single-overhead  camshaft
 Semi-spherical,  2  spark plugs
  per cyIinder
 83 mm x 83.6  mm
 11.0
 17.0 kg/square cm  (350 rpm,  80°C)
 EIectron i caI Iy controI Ied  fueI
  inject ion
 EGR not used
 0.30 mm HOT,  intake and exhaust
 700 rpm
 Special  formulation supplied by
  Nissan for methanol engine
  operat ion.
M100 neat methanol
240 rpm

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