EPA/AA/TSS/83-6
                      Technical Report
                  Determination of a Range
                    of Concern for  Mobile
                Source Emissions of Methanol
                             by
                       Craig A.  Harvey
                         July,  1983
                           NOTICE
Technical  reports  do  not  necessarily  represent  final  EPA
decisions  or  positions.    They  are  intended   to   present
technical analyses  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, Noise and Radiation
                  Office  of Mobile Sources
             Emission Control  Technology Division
                   Technical Support  Staff
                      2565 Plymouth Road
                  Ann Arbor, Michigan  48105

-------
Summary



This  paper  describes  an  effort  by  the  Emission  Control

Technology Division of the EPA  to  suggest  a  range of concern*

for  methanol  (CH^OH)  emissions  from  mobile  sources.   In

light  of  the action  called  for  in  section  202(a) (4)  of  the

Clean  Air  Act  (CAA)   (1)**  and  due  to  a  concern  within

industry as  to what emission  levels  will  be  used as the basis

for  the  evaluation   of  current  and  future  technologies,  a

methodology  was   developed  in  order  to  bracket  a  range  of

concern  for  various  unregulated  pollutants  (2).   This paper

uses   the  results  from  two  EPA  contracts  to  apply  this

methodology  specifically for an evaluation of methanol.



Mathematical  models  previously designed  for  various exposure

scenarios  (such  as enclosed  spaces, expressways,  and  street

canyons)   were    used    to    calculate   the    ambient   air

concentrations  resulting  from  a  range  of  potential  mobile

source methanol emissions.  It was assumed that methanol
*Range   of   concern  is   defined   as  a   range   of  ambient
concentrations   (or  corresponding  vehicle  emissions)  of  a
given pollutant,  the  upper limit of which  is  the  value above
which the  studies show that  the pollutant causes  so  great a
health  risk  as to strongly  suggest  it be  avoided;  the lower
value of the  range  will be the lowest level at which there is
some suggestion of adverse physiological effects.

**Numbers  in  parentheses  denote  references listed at  end of
report.

-------
                             -2-




fueled vehicles would  have to meet  the  same  HC,  CO,  and  NOx



emission  standards  as  gasoline  fueled  vehicles  currently



meet.   In  order  to  get a  worst  case  estimate  it was  also



assumed  that  the entire  vehicle   fleet  would  be  methanol



fueled with up to 25% having severe malfunctions.







In  conjunction with  this  work,  a  health effects  literature



search  for   methanol   was  conducted  by  Midwest  Research



Institute  under  contract to  EPA  to aid  in the determination



of  the  suggested  range  of concern  (3) .   The  health  effects



associated  with   exposure  to methanol  ranged  from weakness,



shallow  breathing  and  rapid  pulse,  to  headaches,  nausea,



vertigo, vision defects, convulsions, and death,  depending on



exposure and  individual susceptibility.








The  results  of  the  Midwest  analysis   suggest  a  range  of



concern  for ambient methanol concentrations  of from  4.5  mg/m



to  260  mg/m  .*   This corresponds  to motor  vehicle emission



levels   of   from   1.58-91   g/mile   to   107.1-6190.5   g/mile



depending  on  the  type of scenario  chosen to  represent public



exposure.   If  the  entire  vehicle  fleet  were  to  run  on



methanol fuel, the estimated  fleet  emission  factors are below



the  ranges of concern for all  expressway and street canyon



scenarios,  as well  as the typical  tunnel scenario.   In  the
*1 mg/nH = 0.764 ppm.

-------
                             -3-




severe roadway  tunnel scenario,  if  25% of  the vehicles  are



assumed  to  be malfunctioning  severely  (e.g.,  non-functional



catalyst),   the  resulting  methanol  concentration  could  be



somewhat higher than the lower limit of the range of concern.







Parking  garages are  also  estimated to  remain  below the range



of  concern,   but  personal   garages  could   have  methanol



concentrations within  the range of concern  for brief periods



of time  due  to  vehicle warm-up exhaust emissions  or  hot soak



evaporative  emissions.   Exposure  resulting   from  potential



self  service methanol  refueling  (50  mg/m )  is  expected  to



be within the range but not above  it.







It must  be  mentioned that  the range of concern for  methanol



suggested  in  this  report  is  based  on  its  "toxicological



properties  and  not  its  photochemical  reactivity  nor  any



possible carcinogenic  effects.   The  consideration  of  the



photochemical   reactivity  and   oxidant   formation   due  to



methanol is  an  important one  but beyond  the  scope  of this



report.  Furthermore,  potential combined  effects  of  exposure



to  other  pollutants   along   with  methanol  have  not  been



considered here.

-------
                             -4-




I.  Introduction







Changing technology  (including  different  vehicle powerplants,



fuels, and emission  control  systems)  can  significantly change



the  emissions  from  automobiles.   This  report  deals  with



methanol emissions because of the possible  use  of methanol as



an  automotive  fuel.   The   Clean  Air  Act  requires  EPA  to



evaluate the health  risks of new vehicle technologies.







Methanol   in   vehicle   exhaust   results   from   incomplete



combustion  of methanol  fuel in  the engine,  in  the  exhaust



system,  or  in the  catalytic  converter.   Other sources  of



methanol from  vehicles  are  evaporative  methanol emissions and



refueling emissions.







Due  to  its toxic  properties and  the potential  increased use



of methanol as an automotive fuel,  tests have  been  conducted



to characterize methanol emissions  as  a function of driving



cycle,  engine  type,  and emission control system.   These test



results along  with health effects  test  data determine whether



methanol  emissions  from  mobile sources  could  be of  concern



with respect to health and welfare.







To establish  a range of concern for  exposure to methanol via



inhalation,   Midwest   Research  Institute   (MRI)   compiled

-------
                             -5-




information  on  its  health  effects  in  different  exposure



situations  (3) .   That work  forms  the basis  for  the  vehicle



emissions range of concern suggested in this report.

-------
                             -6-




II. General Information on Methanol







Methanol is a colorless flammable  liquid with  a  lower heating



value  (heat  content)   half   that  of  gasoline  and  a  vapor



pressure  (volatility)  about  one  third  to one  half  that  of



gasoline.   It burns  in  air with  a  transparent  blue  flame



producing mostly H20 and C02.







Methanol is  used  in industry as  a solvent, a  denaturant for



ethanol, a  dehydrator  for  natural gas, and as a  raw material



in    the   production    of    formaldehyde,    methacrylates,



methylamines, methyl halides, ethylene glycol,  and plastics.







Methanol  is  a  well-known  poison,  discussed   today  in  most



standard  reference works  on toxic  chemicals,  "in  the  past,



methanol's  toxicity was debated,  and,  as  late  as  1936, doubts



existed as  to the  toxicity  of pure methanol.   The  toxicity of



wood  alcohol  was  attributed  to   its   impurities   by  some



authorities  (4).   A 1904  report by Wood  and Buller documented



the  earliest  recorded  cases of methanol poisoning;  it stated



that  275 cases  of blindness  or   death  attributable  to  wood



alcohol were  reported between 1856  (when  the  first scientific



report  of   toxicity  was made)  and  1904   (5).   Nevertheless,



methanol  was  a   frequent   component   of   liniments,  toilet



articles, perfumes, and some patent medicines well  into  this



century.

-------
                             -7-




Even today, exposure to small amounts  of  methanol occurs from



a  wide  variety  of sources.   For  instance,  cigarettes  have



been found  to contain  100 - 200  ug  methanoI/cigarette  (6) ,



and  certain  vegetables  such  as  Brussels  sprouts,  celery,



onions, parsnips,  potatoes, and  rutabaga have  been reported



to  contain  "large" or  "very  large" levels  (unquantified)  of



methanol  after  boiling  for  30  minutes   (7).   Occupational



exposures   to  methanol  are  certainly  possible   in   those



industrial  uses  mentioned  above,  but  the  data  available  on



this are very limited.








Alcoholic  beverages which  contain  ethanol  and which  may  be



contaminated   with  methanol  may   also  contribute   to   an



individual's   exposure   to   methanol   and   accumulation   of



methanol  in the  blood.   Levels  of  3.9 to  105.5'mg methanol/



liter  have been  reported  in  commercial alcoholic beverages




 (8,9,10).








Alcoholics  with  high  blood  ethanol   levels  (100  mg/100  ml)



tend to accumulate methanol  in their  blood  at  levels  up  to




2.7 mg/100  ml after an eleven day  intoxication (9).  Some  of



the  methanol  accumulated  by  alcoholics  is  believed  to  be



derived from  endogenous  (originating  within the body)  sources




and  accumulated   due  to  ethanol's   disruption  of  methanol



oxidation   and    elimination.    That   some   methanol   is



endogenously   produced   is   supported  by   studies  finding

-------
                             -8-




raethanol  levels  of  0.06  to  0.49  mg/m  and  0.40  to  4.52



rag/m    (0.3  to   3.4  ppm)   in   normal  human  breath(11,12) .



Another study of  54 healthy  nonsmoking  adults  found only 3.6%



of   387   breath  samples  to   contain  methanol;   the   mean



concentration when found was 0.549 mg/m  (13).
In   the   section   of   this   report   concerning   ambient



concentrations,  potential  exposures  from motor  vehicles  are



given which can be compared to the exposures mentioned above.

-------
                             -9-




III.  Legislative Background








The Clean Air Act amendments of  August  1977 included sections



202 (a) (4)  and   206 (a) (3)   which  deal  with   mobile  source



emissions of  hazardous pollutants  from  vehicles manufactured



after 1978.   These sections are as stated below:







    202  (a) (4)







    11 (A)  Effective  with  respect  to  vehicles  and  engines



    manufactured  after model  year  1978, no  emission control



    device,  system  or element  of design shall be  used  in a



    new  motor   vehicle   or  new  motor   vehicle  engine   for



    purposes  of  complying  with  standards prescribed  under



    this  subsection  if  such  device,  system,  6"r  element  of



    design will cause or  contribute  to an unreasonable risk



    to public health,  welfare, or safety in  its operation or



    function.








     (B)  In   determining  whether  an  unreasonable  risk  exists



    under subparagraph (A),  the Administrator shall consider,



    among other factors,  (i)  whether  and  to  what  extent  the



    use  of  any  device,  system,  or element  of design causes,



    increases,   reduces,   or  eliminates   emissions  of   any



    unregulated   pollutants;     (ii)  available   methods   for



    reducing  or  eliminating   any  risk  to  public  health,

-------
                         -10-




welfare, or  safety which may  be associated with  the use



of such devices, systems, or elements  of  design which may



be  used to  conform  to  standards  prescribed   under  this



subsection   without   causing   or   contributing  to  such



unreasonable  risk.   The Administrator  shall   include  in



the consideration  required  by  this  paragraph all relevant



information  developed pursuant to section 214."







206 (a)(3)







" (3)  (A) A certificate of  conformity  may be issued  under



this  section only if  the  Administrator  determines  that



the manufacturer   (or in the case of  a  vehicle or engine



for   import,   any   person)   has   established   to   the



satisfaction of   the  Administrator  that  "any  emission



control device  system,  or  element of design installed on,



or  incorporated in,  such   vehicle  or engine  conforms  to



applicable requirements  of  section  202(a)(4).








 (B)  The  Administrator  may conduct   such  tests  and may



require the manufacturer (or  any such person)  to  conduct



such  tests  and provide  such   information  as is necessary



to  carry  out  subparagraph  (A)  of   this  paragraph.  Such



requirements shall   include   a  requirement   for  prompt



reporting  of the  emission of  any  unregulated pollutant



from  a  system,  device  or  element  of   design   if  such

-------
                             -11-




    pollutant   was   not   emitted,   or   was   emitted   in



    significantly lesser amounts,  from the vehicle  or  engine



    without  the  use  of  the system,  device,  or  element  of



    design."








Prior   to   these   amendments,   EPA's   guidance   to   the



manufacturers regarding  hazardous unregulated  pollutants was



contained  in  the   Code  of  Federal  Regulations,  Title  40,



section 86.078-5b.   This subsection is stated as follows:








     (1)  "Any  system  installed  on or  incorporated  in  a new



         motor  vehicle  (or  new  motor  vehicle  engine)  to



         enable  such  vehicle   (or   engine)   to  conform  to



         standards  imposed by this subpart:








              (i)  Shall  not  in  its  operation  or  function



              cause the  emissions  into  the  ambient  air  of any




              noxious  or toxic  substance  that  would  not  be



              emitted  in the  operation  of  such vehicle (or



              engine)     without    such    system,   except   as
                                                ... •• >»•*»


              specifically permitted by regulation; and








              (ii)   Shall not in  its operation,  function,  or



              malfunction  result   in   any   unsafe   condition



              endangering  the  motor  vehicle,  its  occupants,



              or persons,  or property  in close  proximity  to




              the vehicle.

-------
                            -12-




    (2)   Every manufacturer  of  new  motor  vehicles  (or  new



         motor  vehicle  engines)   subject   to  any  of   the



         standards imposed  by  this subpart  shall,  prior  to



         taking any  of the  action specified  in section  203



         (a) (1) of the Act,  test  or cause to  be  tested  motor



         vehicles   (or  motor  vehicle  engines)  in  accordance



         with  good  engineering  practice  to  ascertain  that



         such  test vehicles  (or  test  engines)  will meet  the



         requirements of this  section for the useful  life of



         the vehicle  (or engine)."








Before certification can  be granted  for new  motor  vehicles,



manufacturers  are  required to  submit  a  statement, as  well as



data   (if   requested  by   the  Administrator) ,   which   will



ascertain  that the  technology  for  which  certification  is



requested  complies with the  standards  set  forth in  section



86.078-5b.  This statement is made  in section 86.078-23(d).







The EPA  issued an Advisory  Circular  (AC 76)   in June  1978,  to



aid the  manufacturers  in complying with section 202  (a) (4) .



Manufacturers  were asked  to  continue  providing   statements



showing  that  their technologies  did  comply  with the  vehicle



emission  standards  and  also  will   not  contribute   to   an



unreasonable risk  to  public health and safety.

-------
                             -13-




Another Advisory Circular  (AC 76-1) was  issued  in  November of



1978  continuing  these  procedures for  1980  and   later  model



years.  At that time, EPA  began work  to  develop and implement



a methodology which would  provide  a preliminary assessment of



potential  mobile  source  unregulated  pollutant  hazards  in



order to  assist  the  manufacturers in deciding  which,  if any,



unregulated pollutants are of particular concern.







Up  to this  time,  several  preliminary  assessments  have been



made  covering  sulfuric  acid,  hydrogen  cyanide and ammonia.



In  each  of these  cases,  the preliminary assessment found no



reason  for  suspecting  a  public  health  problem  from  the



current fleet  emissions of these  pollutants,  and  recommended



that  further  monitoring may  be appropriate  to be  sure that



new  vehicle/emission control  system  configurations did  not



result in greatly  increased emissions.

-------
                             -14-




IV. Methodology Overview







Along with the previously mentioned  activities,  EPA,  with the



input  from  several   interested   parties,   has   developed  a



methodology for  implementing section  202  (a) (4)  of  the  CAA.



This  approach  is  explained  in  detail in  EPA  report  number



EPA/AA/CTAB/PA/81-2,  "An   Approach for Determining  Levels of



Concern for Unregulated Toxic Compounds  from  Mobile Sources"



(2) .   Only  a   brief   summary  of  this  methodology  will  be



presented in this report.








Under  contract to  EPA,  Southwest Research  Institute  (SwRI),



and  Midwest  Research  Institute  (MRI), have  provided valuable



information  for  this  effort.    SwRI  developed  or  modified



mathematical models for predicting  ambient  concentrations of



mobile  source   pollutants  for  exposure  situations   including



enclosed  spaces,   street   canyons,   and  expressways.    Once



vehicle  emissions  for   various  vehicle categories  have  been



determined for a particular pollutant,  these  models are used



to   calculate  ambient  concentrations  for  both  severe  and



typical exposure  situations  for each scenario.







Health effects literature  searches have  been conducted  by MRI



to  aid  EPA  in  suggesting  a  range  of  concern for  various



selected  pollutants.   The upper  level of  the range  is  that



value  above which the studies show  that  the pollutant  causes

-------
                            -15-




so great a health  risk  as  to  strongly suggest it  be  avoided.



The  lower  value of  the range  will  be  the  lowest level  at



which  there  is  some  suggestion  of  adverse  physiological



effects.  The region  between  these  limits will be  termed  the



"ambient  air  range  of  concern",  indicating the  bounds  of



uncertainty  regarding   evidence   of  adverse   physiological



effects caused  by  exposure to  various concentrations of  the



pollutant.  Any  technology  whose  emissions result  in  ambient



air  concentrations within  the  range  of concern  should  be



subject  to  closer   scrutiny.    Technologies  with  emission



levels  above  the  highest  value  of  the  range  should  be



considered "high risk" with respect to human health.








For  the  purpose of this  report,  this particular  methodology



has  been  used  to  develop  a  suggested  range  of  concern



specifically for motor vehicle emissions of methanol.

-------
                             -16-




V.  Vehicle Emissions of Methanol







This  report  considers  only  vehicles  using  100%  methanol



fuel.  Nationwide  methanol  emissions from motor  vehicles  are



currently  negligible  due  to  the  small  number  of  methanol



fueled vehicles,  but  the  technology  does exist to  increase



this  use of  methanol.  Therefore,  the  following  discussion



examines  the  hypothetical  scenario in which  all  vehicles  are



methanol  fueled,  as well as  an  intermediate  scenario  having



25% of the fleet methanol fueled.








The data  in Table  1 are based on the assumption that methanol



fueled vehicles will have to  meet the same emission standards



that  gasoline  fueled  vehicles  now  meet,   in  order  to  be



certified  for  sale.   It   is  further   assumed "that  on  the



average,  in-use  vehicles will  exactly meet  the  HC standard,



except   those  with   malfunctions.    The   hydrocarbon    (HC)



standard  (e.g.  0.41 g/mi for light duty  vehicles on  the FTP)



would presumably apply only  to  the HC portion of  any unburned



alcohol  in the  exhaust or  evaporative  emissions.    Since HC



comprises  only  50% of  the mass of methanol,  the  standard to



be  met  for   actual methanol  emissions  would in  effect  be



double  that  for   gasoline   (e.g.  0.82  g/mi   for   light  duty



vehicles  on the FTP).

-------
                            -17-




In  order  to  better  characterize   methanol   emissions  and



exposures   under   certain   potential   high    concentration



conditions,  a  few  scenarios  are  considered  which  differ



considerably from standard FTP conditions.   For instance,  the



Hot Start  FTP column  in  Table  1  was derived  by  taking  the



ratio  of  Hot  FTP  emissions  to  regular  FTP   emissions  from



actual methanol  vehicle tests  (23,25),  and then  multiplying



that  ratio by the  emission  standard  for  the  FTP.   This  was



also  done  for the  highway (HFET)  column.   This was  done  to



provide  a  more  realistic  emissions  estimate   for  scenarios



such  as  tunnels  or  highways  where cold  start  emissions would



not normally be encountered.

-------
                            -18-

                                Table 1

                          Vehicle Emissions3
                      100% Methanol-Fueled Fleet
                                g/mile
                  Light Duty         Heavy Dutyb      Weighted Average0
   Scenario
(Driving Cycle         With 25%           With 25%           With 25%
    Used)       Normal Malfunction Normal Malfunction Normal Malfunction
Street
Canyon ^
(FTP)
Roadway Tunnel
(Hot FTP)
Expressway
1.17
0.08
0.02
2.60
1.22
0.19
5.47
4.05
2.88
11.03
8.94
3.81
1.44
0.33
0.20
3.12
1.70
0.41
(HFET)
(7-Mode S.S.)

Personal &
Parking
Garages (Idle)
0.007e   0.24e
0.007e   0.24e
aBased  on   expected  compliance   with   light-duty   FTP   hydrocarbon
standard  of  0.41  g/mile  (0.82  g  methanol/mi)   and  heavy-duty  HC
standard of 1.3 g HC/BHP-hr.

bg/KW-hr  engine   data   converted  to  g/mile   assuming   3  miles/gal
methanol,  0.708 kg fuel/kw-hr.

C93.8% light-duty, 6.2% heavy-duty vehicle miles traveled.

dlncludes   evap emissions  @  0.35  g/mi for  light-duty  and 0.54  g/mi
for heavy-duty,  based  on  1985  evap standards  (2.0  LD,  3.0/4.0  HD  HC
g/test) .

eg/minute  results  from  one vehicle; 0.007  is  with  a  warmed up engine
and catalyst; 0.24 is with a warmed up engine and no catalyst.

     applicable to scenarios studied.

-------
                             -19-




Light Duty Vehicles - Urban Emissions (FTP)







For  the  street  canyon  scenario,  the  FTP  was  chosen  as  the



most  representative  driving  cycle of  those available.   The



first column  of Table  1  shows the expected  methanol exhaust



emissions  (0.82  g/mi) based  on an  HC  standard of 0.41 g/mile,



multiplied  by   2  to   account  for   the  oxygen  content  of



methanol.   Recent tests  on  properly  functioning  4-cylinder



vehicles   with   oxidation  and/or   3-way   catalysts  yielded



methanol  emissions  less than  this value.   For  instance, Ford



Pintos with different degrees of engine modifications emitted



between  0.3  and  0.6   g/mile   (22),  and  a  recent   EPA test



program  using  a methanol-fueled  VW  Rabbit  and  Ford  Escort



yielded emissions of 0.1-0.5  g/mile  (15).








Hot  Start  "FTP"







For  the  severe  case  tunnel scenario, the  average  speed is 25



mph,  so  of the  data available, the  FTP was again  chosen as



the  most  representative driving cycle.   However, in a tunnel,



vehicles  are  assumed to be warmed  up already so the hot start



portion  of the  FTP  data  were used (Bags 2  and 3) .   The data



collected  for this  show  the hot  start  methanol emissions to



be  approximately 10% of  the  corresponding  FTP emissions, not



including  the evaporative emissions, since  they would not be



a  factor  in  emissions  while  actually  driving.  Using this



proportion  together  with  the  effective FTP  standard of 0.82

-------
                             -20-




g/mile, the  expected  methanol exhaust emissions  from  the hot



start portion of the FTP would be 0.08 g/mile.







Highway Emissions  (HFET)







The  EPA  driving  cycle  chosen  to  represent the  expressway



scenario  is  the  Highway  Fuel  Economy Test  (HFET)  with its



average  speed  of  48.2  mph.   Recent  data  (23,  25)  from



methanol  fueled vehicles with  3-way catalysts  and  oxidation



catalysts  (VW,  3-way  catalyst  prototypes)  show  the  HFET



methanol  exhaust  emissions  to  be  about  98% lower than the



methanol  emissions  from  the  FTP.   Applying   this  percent



reduction  to the  FTP standard  yields expected  emissions  of



0.02 g/mile  for highway driving conditions.  As  with  the hot



start   FTP  calculations   for    the  tunnel  s'cenario,   the



expressway scenario does not  include evaporative  emissions.







Two  contributing  reasons  for  this  large  difference  between



FTP  and HFET emissions could be differences  in  engine  speed



and  differences  in  the  thermal  condition  of  the  catalyst.



The  FTP includes  a cold  start  with  a large fraction  of the



overall emissions  being emitted  in  the first part of the test



before  the  catalyst  is  warmed  up,  but  in  the  highway  test,



the  catalyst is already warmed up.   Some  supporting evidence



for  the engine speed effect  is  found in  two studies   (17,25)



using  steady  state  tests.   The first  of  these showed 95%



lower methanol  emissions  at  3000  rpm than  at 1000 rpm and the

-------
                             -21-




second one showed a  25%  - 65% decrease  in  methanol emissions



at 50 mph relative to 30  mph.   The  actual  engine speed in the



HFET is a function  of  the vehicle  transmission  and axle gear



ratios which may vary.








Heavy Duty Engines







As with light  duty  vehicles, heavy duty engines  need to meet



certain EPA criteria.   The  regulations call for  no more than



1.3  g  hydrocarbons  per BHP-hr  beginning with  the  1985 model



year.   This,   again,  would  probably  apply only  to  the  HC



portion  of  any  unburned  fuel,  so the  effective  limit  for



methanol exhaust emissions would be 2.6 g/BHP-hr.







For  comparison,   testing  of  a  M.A.N.   methanol-fueled heavy



duty  engine   with  an  oxidation  catalyst  yielded  methanol



exhaust emissions of  0.4  g/BHP-hr  (0.5g/kW-hr)  on  the 7 mode



test  and  0.7  g/BHP-hr   (0.9  g/kW-hr)  on  the  transient test



procedure.  Another  engine,  made by Volvo,  used injection of



a pilot charge of diesel fuel to  ignite  the methanol  charge.



When tested with  an  oxidation catalyst,  the unburned methanol



emissions  were  0.67  -  0.75  g/BHP-hr   (0.9  -  1.0  g/kW-hr)  .



Without a  catalyst  these emissions  increased  to  1.6  -  3.7



g/BHP-hr  (2.2  - 4.9 g/KW-hr)  on the  7  - mode  and  transient



tests, respectively.

-------
                            -22-




To put  these  power-specific emissions  into terms  of  g/mile,



they can  first  be converted to g/kg  fuel by dividing  by the



fuel consumption  (kg fuel/kW-hr).   Then,  using  fuel  economy



data from other heavy  duty diesel tests  (29) ranging  from 44



-  69  liters/100  km,  and adjusting  for  the different  energy



content of methanol vs.  diesel  fuel,  a  corresponding range of



methanol  emission   factors  on  a   per-mile   basis  can  be



calculated.   This  is  how the  heavy  duty  engine  emission



estimates shown in Table I were derived.







Evaporative Emissions








Emissions  of  evaporated   fuel   from  methanol  vehicles  can



contribute  significantly   to   the  overall  vehicle  methanol



emissions.   Therefore  these   emissions  are  included,  where



appropriate,  in  the  fleet average  emissions   in  Table  I.



These  numbers  include  both diurnal  heat  build and  hot  soak



evaporative  emissions  as  specified  in  the Federal Register



test procedure.








As was  done with  the FTP emissions above, we will assume that



the  evaporative  gasoline  standards  would  apply  to  the  HC



portion   of  evaporative   emissions   from  methanol  fueled



vehicles.   This  would result  in  maximum  methanol evaporative



emissions  of  4.0  g/test  for  light duty  vehicles and  6.0  or

-------
                            -23-




8.0 g/test  for  heavy  duty  engines  and  vehicles,  depending



upon their Gross Vehicle Weight Rating (GVWR).







These  values  can  be  converted   into   grams/mile  for  any



scenario  that  would  include  evaporative  emissions  -  namely



street canyons.  This is done by  taking  the total evaporative



emissions per  day  (diurnal plus  hot-soak)  and  then  dividing



by the miles driven  per  day.   According  to MOBILE2,  in urban



areas, the  average light  duty  vehicle makes  3.05 trips/day,



totalling 31.1  miles.   Therefore, to  estimate  the equivalent



g/mile  emissions  of  a  car  meeting  a   4.0  g/test  methanol



evaporative standard, it is necessary  to  know  how much of the



4.0 grams is hot soak vs. heat build.







The hot  soak test  emissions are  usually  greater "than  the heat



build   emissions.    For   example,   in-house    tests   of   a



fuel-injected  methanol  fueled VW  Rabbit  have   shown  hot soak



test  emissions  to  be approximately  1.3  times  greater than



heat   build  emissions   (25) .    In   similar    tests   at  the



University  of  Santa  Clara, the  ratio  was about  3.0  (28).   A



couple of carbureted cars  (1980  Ford Pintos modified  to run



on methanol)  have  also  been  tested.  For  these  vehicles the



ratio  of  hot   soak  to  heat  build  emissions  were  greater,



averaging 10.0.








From  this rather  limited  data  it  appears  that  a reasonable



rough  estimate  of  the ratio  of  hot soak  (HS)  to  heat build

-------
                            -24-

(HB)  emissions  for  methanol fueled  vehicles  would  be  5.O.*

From this,  the  grams methanol/mile  can be calculated,  based

on  a  vehicle  just  meeting  a  2.0  g/test  evaporative  HC

standard.



     (1)  HS + HB  =  4.0 grams methanol

     (2)       HS  =  5 x HB



              HB  = 0.67 grams methanol

              HS  = 3.33 grams methanol



With   one   heat   build/day,   3.05   hot  soaks/day,  and  31.1

miles/day,  this results in 0.35 g methanol/mile.



Of  the  cars  that  have  been  tested  so  far,  "only one  has

exceeded  these  estimates  -   a  carbureted   1980  Ford  Pinto

(designed to  meet the California  2  g/test  HC  standard)  with a

total  of 5.7 g/test.   The other test vehicles  (  VW Rabbit,

Ford  Pinto,  and  Ford  Escort) have  ranged  from  1.2   -  2.4

g/test by FID measurement uncorrected  for methanol response,
*The  corresponding ratio  for gasoline  fueled  vehicles,  per
MOBILE2,  is  0.59.   It  is  not  certain why there should be that
much  difference  between methanol  and gasoline, but  it could
possibly  be  related to the much greater  heat of vaporization
of  methanol  necessitating  greater  temperature  for  a  given
rate  of  evaporation.   The FTP before the hot  soak  may result
in  a  higher  temperature  or  rate of  vaporization  compared to
the heat  build.

-------
                             -25-




which would  be  about 1.6 -  3.2  g/test if a  typical methanol



response factor of 0.75 is assumed.







Heavy Duty Evaporative Emissions







As  mentioned  above,   the   heavy  duty  vehicle  evaporative



emission standards beginning  in model  year  1985 (depending on



GVWR) are 3.0 and  4.0  g  EC/test,  which corresponds to 6.0/8.0



g methanol/test.   Per  Mobile 2,  the  hot soak  portion  of the



test contributes 37% of  the  total test emissions for 1984 and



later model  years, which methanol fueled vehicles  would be.



This  fraction is  based on  gasoline  data  since  no methanol



fueled  heavy  duty  evaporative  data   are  available.   Going



through the  calculation  to  determine  g/mile,  as was done with



light  duty  vehicles,   but   using  6.88  trips/d'ay  and  36.70



miles/day  for heavy duty  vehicles yields  0.53 g/mile  up to



14,000 GVWR  and  0.70 g/mile  methanol over 14,000 GVWR.







For  purposes of computing  an average  heavy  duty evaporative



emission  rate,  the  above  two  numbers  need  to  be weighted



according  to their respective  fractions  of  urban VMT.  Using



data  from the  MVMA (33) ,  only  5%  of the  non-highway urban



truck VMT  is from  combination trucks.   This  should serve as a



good  approximation  of  the  truck VMT  fraction  over  14000



GVWR.   Therefore,  the  weighted  average  heavy  duty  vehicle

-------
                            -26-
evaporative  methanol  emissions  are  estimated  to  be  0.54
g/mile.

Malfunction Conditions

A certain  percentage of  in-use vehicles  have  been  found  to
operate in a  less-than-optimum  condition  (34).   For instance,
a disconnected  air  injection  system or  a catalyst  that  has
been  either  removed  or  poisoned  with  use  of  improper  fuel
will  all  increase  emissions.   The  resulting  emissions depend
on the  type  and degree of  malfunction,  but at  this  time  the
most  data are available for a  severe malfunction.   This would
be the  lack  of  a  catalyst as  compared  to the  presence  of a
working  catalyst,   including   particularly   the  case  of  a
catalyst equipped  vehicle  tested without  a catalyst.   Such a
comparison shows the  "malfunctioning"  (no catalyst)  vehicle
methanol emissions  to be  much  greater  than  catalyst equipped
vehicles (references:  no cat.  14  through 21,25; catalyst 15,
18 through  23,26,27,28).   Table  II  gives the  ratios  used  in
computing the malfunction values  in  Table I.   These are based
on test data from one or more vehicles/engines.

-------
                            -27-

                          Table II

             Ratios of Malfunction (no catalyst)
                 to Non-Malfunction Exhaust
                     Methanol Emissions
                                          HFET
                   FTP     Hot FTP     (HP 13-mode)    Idle
8.0
5.5
58.0
5.8
35.0
2.3
34.3
Not used
Light Duty

Heavy Duty
The  potential  effect  of these  malfunctions  on ambient  air

concentrations of  methanol  is  shown  in  columns 2  and  4  of

Table   III   with   25%   of   the  vehicles   assumed   to   be

malfunctioning.  The  25% malfunction fraction was  arrived  at

from   FOSD*   data   indicating   that   in   areas   without

Inspection/Maintenance,  after   50,000  miles,  26%   of  the

vehicles had at  least one of  the three malfunctions described

above.
*FOSD:  EPA  Office of  Mobile  Sources  Field  Operations  and
Support Division.

-------
                             -28-
VI. Methanol Ambient Air Concentrations

The methanol  emission  factor information provided  in  Table I
can  be  used,   in  conjunction  with  the  modeling  techniques
developed   by   Southwest   Research   Institute   (2,33),   to
calculate  the  ambient  air  concentrations  produced.   Future
work  may   identify  other   scenarios  which   would  also  be
appropriate  for the assessment  of  human exposure  to  exhaust
pollutants,  but,  for this task,  five exposure scenarios were
investigated:   roadway   tunnels,   street   canyons,  personal
garages,  parking  garages  and  urban  expressways.   Two  case
situations,  "typical"  and  "severe",  were developed  tor  each
of  the  first four scenarios, and  three cases were considered
for   the  expressway  scenario.    Each   situation   has  been
considered   separately;    no  cumulative  effects  have  been
determined  at  this point  for  these  or  other  exposures  to
methanol.   Reference (2)  discusses  the reasoning behind using
these  specific scenarios as  well as  the  information  used in
the determination  of the modeling techniques.

Table  III  presents ambient  air  concentrations of  methanol
calculated  from the vehicle  emissions listed  in Table  I  for
seven   ambient   situations.    Evaluations   of   the   garage
situations  are  based  on  idle  emission  data  from only   one
vehicle  and  evaporative emissions from five vehicles.

-------
                             -29-




Two specific  tunnel designs were  chosen  to estimate  the two



roadway  tunnel  cases.   A newly  designed,  two lane  roadway



tunnel,  with  moderate traffic flow,  is  used for  the  typical



condition,  while  an  old  design,  heavily-traveled  roadway



tunnel   is   used   for   the   severe  condition   (2) .    The



calculations  for  the  typical  tunnel exposure  situation  will



be  developed  to  show  how  the  other   concentrations  were



determined.







From Section V of  this report,  the average methanol emissions



from light  and heavy duty vehicles  in a  typical tunnel would



be  0.38  g/mile.    Per   the   model  developed  by  Southwest



Research  Institute   (2) ,  an  average  emission factor  of  1



g/mile  of  any  pollutant  for  traffic  in  a  typical  roadway



tunnel  would  result  in  a  concentration  of  I."l2  mg/m   for



that pollutant.  Multiplying  this  by the  average emissions of



0.38 g/mile gives  an  expected methanol concentration  of 0.43




mg/m .







The  street  canyon  situations  are  simulated by examining the



parameters  of two  street  canyons.   The  typical  condition is



calculated  for a  four lane street canyon  with  a traffic load



of 800  vehicles per hour and sidewalk  location of the exposed



population.   The  severe  condition  is based   on  a six  lane



street  canyon with  a 2400 vehicles per hour traffic load, and



sidewalk  location of  the  exposed population.

-------
                             -30-




Three different  cases  were  considered  in order to  cover  the



possible range of  exposures in an  expressway  situation.   The



typical on  road  exposure is based  on a  four  lane expressway



with a  traffic  load of  1400 vehicles per hour and  a  wind of



1.0  meter/second  at 315 degrees  to  the  direction  of  travel.



In  this  situation, the  exposed  population is  located inside



the  vehicle.    The  severe  case   represents   an  identical



situation except with  much  more  traffic  (3675 vehicles/hour),



on  a ten  lane  freeway.  The third  case  necessary  to consider



is  the  "off  road"  case which is  an exposure involving a close



proximity  to the  highway   (i.e.,  living  or working  close to



it) .   This case  is calculated  on a  short term  basis (rush



hour) for a distance of  100  meters  downwind of the roadway.







Garages







The typical personal garage situation  represents  a  30 second



vehicle  warm-up time,  and  the  severe situation  simulates  a



five minute vehicle warm-up time.   Both  of  these  cases, of



course,  take place within a residential  garage  with the  door



open,  and  are  intended to correspond  to summer  and winter



conditions,  respectively.   Evaporative emissions, as  well as



idle emissions will be  examined.

-------
                             -31-




Currently,  methanol  idle  emission  data  are  only  available



from one  vehicle  -  a  VW Rabbit tested with  various  catalysts



and  calibrations.  Methanol  emissions  at  idle  range  from



0.001 to  0.034  g/min.f  averaging  .007 g/min.   However,  these



tests are with  a  warmed  up engine  and  catalyst  rather  than



cold-starts as  would  occur  in  a garage scenario.  So,  a  more



accurate  assessment of cold-start  idle  emissions might  come



from  using idle  tests  of  this vehicle  without  a  catalyst.



These data  range  from 0.18  to  0.31 g/min.,  with  an average of



0.24  g/min.   In a  personal  garage under the  severe exposure



situation,  0.24 g/min would  yield  a  methanol concentration of



16.08 mg/m3.







Evaporative emissions in  a personal garage  are  potentially a



greater  problem than start-up emissions,  because  the  garage



door  would more  likely be  closed,  reducing  the ventilation



from  615  cfm  to 20 cfm.  Only  the hot soak  situation will be



examined,  since these emissions are usually  greater than the



diurnal heat build  emissions of methanol.








To    calculate    expected   methanol    concentrations    from



evaporative emissions,  it will first be  assumed that vehicles



will  meet  the  standard of  2.0 g  EC/test.   As  described  in



Section  V, this  would  result   in  one-hour  hot  soak methanol

-------
                             -32-


emissions of 3.33 grams  due  to inclusion of the  oxygen mass.


in  a  typical   residential   garage  of  2189  ft   (61.95  m )


the   resulting   concentration   of    methanol,    neglecting

                                 3
ventilation,  would  be  54  mg/m .    With  ventilation  taken


into account  (20  cfm),  the  lower  bound on  the concentration


would  be 30 mg/m  .   This  figure  corresponds  to an  initial


concentration  of   54  mg/m    reduced  over  a  one  hour  time


period  by  ventilation at  20  cfm,  with  no further  methanol


evaporated  during  that  hour.   Since  what  actually  occurs


(continuous  evaporation  and   continuous  ventilation)   is


somewhere   in   between    54  mg/m    and   30   mg/m  ,   the


concentration   corresponding  to  3.3  grams   of  evaporated


methanol is estimated to be  40 mg/m .
The  exposure  to  this  concentration of  40  mg/m   would  occur


only  if  a person  re-enters the  garage  within the  hour,  and


the  exposure  will  also usually  be short,  lasting  from  the


time   the  person   enters  the   garage  until   either   the


ventilation from  the opened garage door  reduces  the methanol


concentration  significantly or the person  drives out of  the


garage.   After  10  minutes with  the  garage  door  open  the


concentration in the garage would drop by 94%  (3,  Figure 21) .




The  typical  parking  garage  case  simulates  an  above  the


ground,  naturally ventilated  garage  in  which it  is  assumed


that  a  vehicle spends  an  equal  amount  of  time  on  both  the

-------
                             -33-




parking level  and ramp  level.   The emission factors  used in



this  scenario  are  idle  emissions,  since there  are  no  data



available  for  any parking garage  driving cycle.   The severe



case  represents  an  underground  garage  wherein  the  exposed



population is  assumed  to be  at the  lowest parking  level.   It



is also assumed that this exposure occurs 20 minutes  after a



major  event  in which  the  parking  structure  is  emptying  from



an essentially full condition.  The  initial  concentration of



methanol   is   assumed   to   be  low   (1  ug/m  ) ,   since    the



ventilation system in a  parking  garage  would  remove  most of



the evaporative emissions as they occur  (2).








Concerning  evaporative  emissions   in  a  parking  garage,   the



only   potentially  high  concentration   situation   would  be



following  the  arrival  of many  vehicles,  which th'en proceed to



give  off  hot  soak  emissions.   This  is  not  expected  to  be a



problem   for   two   reasons.    First,   there   is   plenty  of



ventilation  (30,000-40,000  cfm per  parking  level  compared to



20   cfm   for   a   closed-door   personal  garage).    Secondly,



immediately after parking, the drivers would  leave  the garage.

-------
                            -34-
                             Table III
                       Ambient Air Scenarios
                 Methanol Concentrations
Scenario
Entire Fleet
   CH30H
   Fueled
Entire Fleet
  CH30H
  Fueled
   25%
Malfunction
25% of Fleet
   CH30H
   Fueled
25% of Fleet
  CH30H
  Fueled
   25%
Malfunction
Roadway Tunnel
  Typical           0.43
  Severe            1.09

Expressway
  Typical           0.02
  Severe            0.10
  Close             0.02
   Proximity

Street Canyon
  Typical           0.06
  Severe            0.41

Parking Garage
  Typical           0.03
  Severe            0.39

Personal Garageb
  Typical           0.06
  Severe            0.47
  Hot Soak         40.00
                2.87
                7.31
                0.05
                0.21
                0.04
                0.13
                0.88
                0.94
                3.63
                1.90
               16.08
               40.00
                0.11
                0.27
                0.01
                0.03
                0.01
                0.02
                0.10
                0.01
                0.10,
                0.06
                0.47
               40.00
                0.72
                1.83
                0.01
                0.05
                0.01
                0.03
                0.22
                0.23
                0.91
                1.90
               16.08
               40.00
aBased on weighted average emission factors from Table I.

'•'Since  the  personal  garage  scenario  considers  only   one  vehicle,
the  25%  malfunction and/or methanol-fueled  fractions in  columns  2,
3, and 4 were not taken.

-------
                             -35-
Vehicle Refueling Exposures

With  the  use  of  methanol  as  a  fuel,  another  scenario  that
needs  to  be  investigated   is  the exposure  encountered  by  a
vehicle  owner filling  up  his  fuel  tank  at  a  self  service
station.   According  to  1982 information  from EPA's  FOSD  it
was  found  that 75% of  the  refueling  is done  on  a  self serve
basis  (42)  .

The  estimate of methanol  exposure presented  here  is  a  very
rough  estimate based on  the limited  exposure data  that was
collected  for  benzene   (43).   It  was  found  that a  person
refueling  a  car  with  gasoline  would  be exposed to about 0.785
mg/m3   of   benzene   from   gasoline  vapor   containing  0.8%
benzene.   This means  a  total gasoline vapor  exporsure of about
100    mg/m .     Since    methanol    has   a   vapor   pressure
approximately  half  that  of  gasoline,  a  typical  refueling
would   result  in   a   methanol   concentration  of   about  50
mg/m  .   The  average refueling   time  for  a   gasoline  fueled
automobile  is  1.7  minutes.   For  methanol,   with   its  lower
energy content,  average refueling  time  would  double,  to 3.4
minutes on  the average.

-------
                             -36-




VII. Methanol Health Effects








Ingestion Studies







A literature review concerning  the  health  effects of methanol



was performed by Midwest  Research  Institute (3).   In addition



to  inhalation  data,  this  review  also covered  exposures from



ingestion and skin  absorption,  which could occur  with  use of



methanol as a vehicle fuel.







Practically  all  the   methanol  toxicity   data  involve  its



ingestion  with,  or  as   a  substitute  for,  ethanol   (ethyl



alcohol).    The   immediate   symptom   is  an   inebriation,



indistinguishable from  that  from  ethanol ingestion.  After 12



to  18  hours,  the  characteristic  methanol  toxicity appears,



presumably caused by  its  metabolites, formaldehyde and  formic



acid.   Symptoms include  headache,  weakness,   leg  cramps,  and



vertigo; nausea  and  vomiting sometimes with violent abdominal



pain;   back  and  leg  pain;   vision  defects;  rapid,  shallow



breathing  from  metabolic  acidosis;  and weak,  rapid pulse with



hypotension;   progressing   to   apathy   and   coma,  or   to



excitement,  mania,  and convulsions.   Death,  if  it occurs, is



usually  from   respiratory   failure.   In   nonfatal   cases,



convalescence   is   often   protracted   and   complicated   by



debility,  blindness, and  kidney problems.

-------
                             -37-




Relatively few experimental  studies  on  methanol  toxicity have



been published,  and  most of  them involved very  large  doses,



mechanistic studies  of  the  retinal  toxicity,  or  both.   Most



human  reports  are case  studies,  with  little exposure  data.



Toxicity  has  occurred  from  ingestion,  inhalation,  contact,



and confounded exposure through two or all three routes.







Methanol's  toxicity   (especially  its   ocular   effects)   is



generally believed to be caused  by its  metabolities, although



its metabolism  is  not  fully understood.   In  humans  and other



primates, methanol  is  first  oxidized  to  formaldehyde  by the



enzyme  catalase,  but   in   lower   animals  this  oxidation  is



effected  by  alcohol   dehydrogenase.    The   highly  reactive



formaldehyde  quickly  disappears  from  the  tissue  and  was



formerly  believed  to  be the  cause of toxic effects.   More



recently,  the  further  metabolites,  formic   acid or  formate



esters, have been suggested  to be  the toxic products (38).







Animal Studies







The  bioassay  data  were  limited  in applicability  to  human



toxicity,  but did  demonstrate that  in  the  animal ini  vitro



systems   studied,   methanol   is   not   very   toxic  and  not



mutagenic.  In  the one  in vitro  respiratory  tissue study, the



exposure  to 0.4  to 1.4 mg methanol  in  aerosol at the  rate of



27  ml/sec for  2 seconds  inhibited ciliary  activity   in  the

-------
                             -38-




esophageal tract  of  the  leopard  frog.   Another  study  found



low  levels  of  methanol  (15 ug)  increased  release of  lung



prostaglandins;   higher  methanol  levels  decreased  rate  of




release (3).








In different  animal studies  the  results varied quite  a  bit.



Rats exposed  to  50 mg/m  methanol  for  12 hr/day  for  8 weeks



developed  respiratory  tract  irritation,  liver  degeneration,



and  cortical  neuropathy,  but no such  effects  were  found  at



1.77  mg/m   (39).   Similarly,  minor  toxicity  was  found  in



rats  exposed  continuously   to   5.32  mg/m   methanol.   Dogs



exposed  to about  600  mg/m   methanol  18 hr/day  for  over  a



year developed no noticeable  adverse effects.
Human Studies







Human   experimental   studies   have   not   been   conducted



specifically   to   identify   methanol   health   effects   by



inhalation,  but  several  studies  have  determined  an  odor



threshold  for  methanol.   The  highest   of  these  was  7,800


     3                              3
mg/m  , while the lowest  was 4.3 mg/m   (3).








Experiments   have   also   been   conducted   measuring   eye



sensitivity  to  light(39).  A  threshold  of  3.3  to  3.7 mg/m



was   found  for  degradation   of  light   sensitivity   (dark



adaptation),  and  1.8  to  2.4  mg/m   had  no  effect.   At  a

-------
                             -39-




concentration  of  approximately  4.5  rag/m   the  pattern  of



dark  adaptation  was  markedly  altered   from   that  of  the



controls.
One  documented  study  of occupational  exposures  to  methanol



found  that  a  group of office  workers  exposed to  about  22 to



500  mg/m    from  spirit   duplicating   machines  experienced



recurrent headaches.  Workers  who  were  actually operating the



machines had more severe symptoms  (3).








Skin Absorption








Various  animal  studies have shown  methanol  exposure  via  skin



absorption  to  have effects similar  to  inhalation (3).  Also,



recent work with  humans has  shown methanol  sk'in absorption



and  ingestion  to  result  in   similar  quantities  of  methanol



being  excreted  in  urine and  exhaled air  indicating similar



effects  on  the  body.

-------
                             -40-

VIII. Determination of the Range of Concern and Conclusions



The  definition  of  "range  of  concern"  is  that  range  of

exposure  concentrations   which  may  be  detrimental  to  human

health.   The  lower value  of this  range  would be  the  lowest

concentration  at which  there  is  some suggestion  of  adverse

physiological  effects.   The upper  value  of this  range would

be that  level  above which the  studies  show that the pollutant

causes  so great a health risk as  to  strongly suggest  it be

avoided.   The   Threshold  Limit  Value*   (TLV)  for  a  given

pollutant  is usually appropriate  to use  as the upper level of

the  suggested  range of concern.



Although  it would  be  more  appropriate  to  consider exposure

concentrations  relative  to their  corresponding exposure times

for  each resulting health  effect,  this  degree of  detail was

not  feasible  with the data  available.  The  determination of

the  range  of   concern   was  based  primarily  on  acute  human

experimental   studies,   since   these  were  thought  to  most

closely  simulate  the  exposure  situations  examined in  this

report.
 *The  Threshold Limit  Value,  set by  the American  Council  of
 Governmental   Industrial   Hygienists,   is   the   recommended
 maximum  time  weighted average concentration  to  which workers
 can be exposed for an  8-hour work day or 40-hour work week.

-------
                             -41-




The Threshold Limit Value for  methanol  inhalation exposure is



260  mg/m ,  which  is  suggested as  the  upper  limit  of  the



range of concern.  Although  a  direct  comparison of inhalation



vs.   ingestion   exposure    would   not   be   valid   due   to



uncertainties  in  absorption and  metabolism processes,  it is



interesting to  note  the  correlation that  seems to  exist in



the exposure range around the TLV.







One reference  (40)  indicates that  the lowest ingested dose at



which  some  toxic  effect  occurred  for  humans  was  100  mg/kg



body  weight.   For  a  70  kg  (154  Ib)  person  this translates



into  7  grams or  8.75 ml.   Another  study (4) cited one unusual



case  in which  ingestion of  only  3 teaspoons  of 40% methanol



 (6 ml methanol)  resulted  in death,  whereas a third study  (41)



reported no toxic reaction  from ingestion of about 2 ml.  For



comparison,  an inhalation  exposure  at  the TLV  of  260  mg/m



would yield an  8 hr.  cumulative  exposure  of  3.25  ml  if it



were  all absorbed (3).  However,  it  is  probably not valid to



compare absorption and ingestion in this fashion.








Documentation  of adverse  physiological  effects  of  low level



methanol exposure is  poor,  making  the  selection of  a  lower



limit to the range of concern difficult.   The  level suggested



as  the  lower  limit  is 4.5 mg/m ,  which  was the  level at



which the pattern  of  dark  adaptation  markedly  altered  from



that  of  the  unexposed control sample  (39).   These  changes

-------
                            -42-




resulted from  a  5-minute exposure,  but  they were  reversible



within a couple hours following exposure.







Below  this  level  certain  physiological  effects  have  been



found,  such  as changes  in  the alpha-rhythm amplitude  of  the



cerebral cortex  reflex activity  (1.17  -  1.46 mg/m ).   It  is



not   known   whether   these  alpha-rhythm   changes   represent



adverse  physiological  effects  or  just altered  physiological



parameters.   Since  the  limits of  the range  of concern  are



based  on evidence of  adverse  physiological  effects,  4.5  mg/m



is considered  to be  conservative  (i.e. on  the  low  side)  for



the lower limit of the range of concern.







The  next  step  in  making  use  of  this  suggested  range  of



concern  is  to  translate  it into terms  of automotive emission



factors  for  each  scenario.   Table  IV shows   fleet  average



emission  factors that would   result  in the  lower  and  upper



limits  of  the ambient  air  range of  concern.   Since  these



numbers   are  total   emission  factors,   they   include  the



evaporative  emissions   (for  the  street canyon   scenario)  as



well as  the  tailpipe emissions.

-------
                            -43-

                          Table IV

       Emission Factors  (g/mile) Corresponding to the
   Lower  and Upper Limits of the Methanol Range of Concern
                                 4.5 mg/m3
260 mg/m3
Roadway Tunnel
Street Canyon
Expressway
(typical)
(severe)
(typical)
(severe)
(typical)
(severe)
(off road)
4.01
1.58
107.14
15.96
36.88
9.09
42.86
231.5
91.0
6190.5
922.0
2131.1
525.3
2476.2
Comparing these figures with  the  emissions  listed  in Table I,

it appears that the  severe  tunnel scenario  is the  only one of

the  roadway  scenarios  having   the  potential  for  exposure

within  the  range of  concern.   Using  the  weighted  average

emission  factors  from  Table  I,  the average  em-ission factor

for each  scenario can  be compared  to  the corresponding lower

limit of  the range of concern.  This is done  in Table V.

-------
                            -44-

                               Table V

           Range of Concern Compared to Potential Emissions
                              grams/mile
                   A

             Limits of
          Range of Concern
            (Severe Case)3
          i.e. Fleet Average
           Emissions Needed
           to be of concern
                           B
                    What Fleet Average       Column B
                    Emissions Would Be       with 25%
                   Assuming 100% CH30H       of Fleet
                 Fueled, Catalyst-equipped Malfunctioning
                       Vehicles'3             Severely13
Roadway
Tunnel

Street
Canyon

Expressway
 1.58- 91.0


15.96-922.0

 9.09-525.3
0.38


1.44

0.20
2.56


3.12

0.41
aFrom Table IV
DFrom Table I
As shown in Table V,  even  if  it  is assumed that all light and

heavy  duty  vehicles  on  the  road are  methanol  fueled   (with

oxidation or 3-way catalysts) , the emissions  could be within,

but not  above,  the  suggested range of concern  for the severe

roadway  tunnel  scenario.   The  street  canyon  and expressway

scenarios appear to be below the suggested range of concern.
Garage  scenarios  were  discussed  in  Section  VI.   Parking

garage  exposures,  even  with  all  vehicles  using  methanol,

would be  below the suggested  range  of concern, based  on the

few  idle  and  evaporative tests that have  been  run.  However,

-------
                             -45-




personal garages  are estimated to  have as  much as  16  mg/m



during  a  cold  start,   and  as  much  as  40  mg  methanol/m



during periods  of hot soaks.  Exposure  to  this concentration



would  probably be  brief,  but  within the  range of  concern.



Therefore,   further  monitoring  of   idle   and  evaporative



emissions from methanol  fueled cars may  be  appropriate,  since



exposures  in this  scenario  are likely  to  occur much  sooner



than  any of  the roadway  or parking  garage  scenarios  which



call  for a  large  fraction  of the  vehicle fleet to be methanol



fueled.








Vehicle  refueling  exposures,   as   discussed   in Section  VI,



could  involve concentrations  of  approximately  50  mg/m   for



a  few minutes at a time, each time the  tank  is filled.   This



is   within,   but  not  above,   the   range   of  'concern,   and



therefore,  may  call  for  closer  examination  as to  possible



adverse  effects  and  methods  of  minimizing   this  type  of



exposure.   For  instance,  Stage  II  refueling  loss  controls



would  be one  way of reducing  these  emissions  and  resulting



exposures.   use  of Stage II control  may be  easier  here  than



for  gasoline-fueled  vehicles  since  both  the  vehicles  and



service  station pumps would  probably be newly designed.

-------
                             -46-

References

1.  "Clean  Air  Act  as  Amended  August  1977",  Public  Law
    88-206,  89-272,  89-675,  90-148,  91-604,  92-157,  93-319,
    95-95, 95-190.

2.  "Estimating   Mobile  Source   Pollutants   in   Microscale
    Exposure   Situations,"    M.   Ingalls,   EPA   Report   No.
    460/3-81-021, NTIS PB 82101114, July 1981.

3.  "Methanol  Health  Effects",   Midwest  Research  Institute,
    Draft  Task  7 Report  for  EPA  Contract  No.  68-03-2928,
    NTIS-PB 82160797, August  28,  1981.

4.  "Acute  Methyl  Alcohol   Poisoning  -  A   Review  Based  on
    Experiences  in an  Outbreak of Cases",  I.L. Bennett et al,
    Medicine 32:431-463, 1953.

5.  "Death   and  Blindness   from  Methyl   or   Wood   Alcohol
    Poisoning  with  Means of  Prevention",  C.A.  Wood,  Journal
    of  the  American  Medical  Association   59(22):1962-1966,
    1912.

6.  "Vapor  Phase Analysis  of Cigarette Smoke",  J.R.  Newsome
    et al, Tobacco 161(4):24-32,  1965.

7.  "The  Low-Boiling  Volatiles of  Cooked  Foods", R.  Self et
    al, Chem.  Ind. 21:863-864, 1963.

8.  "Methyl  Alcohol",  S.A.  Schneck,  Handbook   of  Clinical
    Neurology  36:351-360, 1979.

9.  "Blood   Methanol  Concentrations   During  Experimentally
    Induced    Ethanol    Intoxication   in   Alcoholics",   E.
    Majchrowicz   and   J.  Mendelson,   J.   Pharm.  Exp.  Ther.
    179:293-300,  1971.

10. "Analysis    of    Alcoholic   Beverages    by   Gas-Liquid
    Chromatography",  R.B.  Carroll,  Quart.   J.  Studies  Ale.
    Suppl. 5:6-19, 1970.

11. "Methanol  in  Normal Human   Breath",  S.  Eriksen  and  A.
    Kulkarni,  Science  141(3581):639-640, 1963.

12. "Analysis  of Organic  Compounds  in Human  Breath  by  Gas
    Chromatography  -  Mass  Spectrometry",  B.  Jansson and  B.
    Larson, J. Lab. Clin. Med. 74  (6):961-966, 1969.

13. "Measurement  of  Chemical  Inhalation  Exposure  in  Urban
    Population in the  Presence  of Endogenous  Effluents",  B.
    Krotoszynski  et al, J. Anal.  Toxicol. 3(6):225-234, 1979.

-------
                             -47-

14.  "Fuels and  Emissions  -- Update  and  Outlook,  1974",  R.
    Hum  and  T.  Chamberlain,  SAE Paper  740694,  September,
    1974.

15.  "Unregulated   Exhaust   Emissions   from   Methanol-Fueled
    Cars,"  L.   Smith,  C.  Urban,  and   T.  Baines,  SAE  Paper
    820967, August 1982.

16.  "Potential  for  Methanol  as   an   Automotive  Fuel",   R.
    Tillman,  0.   Spilman,   J.   Beach,  SAE   Paper   750118,
    February 1975.

17.  "Methanol as Automotive  Fuel Part  1 -  Straight Methanol",
    R.  Fleming,  T.  Chamberlain,   SAE  Paper  750121,  February
    1975.

18.  "Vehicle Evaluation  of  Neat Methanol  -  Compromises Among
    Exhaust Emissions,  Fuel  Economy  And  Driveability",  N.D.
    Brinkman,  Energy Research 3:243-274, 1979.

19.  "Driving  Cycle   Economy,  Emissions   and   Photochemical
    Reactivity Using Alcohol Fuels and Gasoline", R.  Bechtold
    and J.B. Pullman, SAE Paper 800260, February  1980.

20.  "Methanol   as   a  Motor  Fuel  or   a   Gasoline  Blending
    Component",  J.  Ingamells  and R.  Lindquist,  SAE  Paper
    750123, February 1975.

21.  "Driving  Cycle   Comparisons   of   Energy  Bconomics  and
    Emissions  from an Alcohol  and Gasoline  Fueled Vehicle",
    R.  Bechtold  and B.  Pullman,  Proceedings  of the  Third
    International  Symposiumon Alcohol  Fuels  Technology,  Vol.
    Ill, May 1979.

22.  "Emission and Wear  Characteristics of an  Alcohol Fueled
    Fleet   Using   Feedback   Carburetion    and   Three-Way
    Catalysts", W.H. Baisley and  C.F.  Edwards, Proceedings of
    the   Fourth   International   Symposium   on  Alcohol  Fuels
    Technology, Brazil, October 1980.

23.  "Characterization of Exhaust  Emissions  from  Methanol  and
    Gasoline  Fueled  Automobiles",  L.   Smith  and  C.  Urban,
    Southwest   Research    Institute,    EPA   Report  No.   EPA
    460/3-82-004, March  1982.

24.  "Characterization   of    Emissions   from   Methanol   and
    Methanol/Gasoline  Blended   Fuels",   D.   Schuetzle,   T.
    Prater, and R. Anderson,  SAE Paper  810430,  February 1981.

25.  "Methanol  VW  Catalyst   Weekly  Update   Report  #16,"  memo
    from  T.  Penninga to  C.  Gray,  U.S. EPA  Emission  Control
    Technology Division,  May 26, 1983.

-------
                             -48-

26.  "Alcohol  Fueled   Fleet   Test  Program,   Fleet  No.   1
    Vehicles",  Final   Report  (informal)  MS-82-10,  State  of
    California Air Resources Board, July 1982.

27.  "Alcohol  Fleet  Test   Program  Fourth   Interim  Report,"
    California Air Resources  Board,  Project 3T8001, MS-82-11,
    August 1982.

28.  "The  Effects of  Fuel  Additives  on  Alcohol Exhaust  and
    Evaporative  Emissions",  S.  Espinola et  al,  University of
    Santa Clara, Santa Clara, California 95053, 1982.

29.  "Emission Characterization  of a  Spark-Ignited  Heavy-Duty
    Direct-Injected Methanol  Engine",  T.L.  Oilman and  C.T.
    Hare,  Southwest  Research  Institute,  EPA  Report  No.  EPA
    460/3-82-003, April, 1982.

30.  "Results  of  M.A.N.   -   FM  Diesel  Engines  Operating  on
    Straight Alcohol Fuels",  A. Neitz,  F.  Chmela,  Proceedings
    of  the Fourth  International   Symposium on  Alcohol  Fuels
    Technology,  1980.

31. "Emission   Characterization   of   an  Alcohol/Diesel-Pilot
    Fueled  Compression-Ignition   Engine  and  Its  Heavy-Duty
    Diesel Counterpart," Terry L.  Ullman  and Charles T.  Hare,
    Southwest   Research   Institute,    EPA   Report  No.   EPA
    460/3-81-023, NTIS PB 82154113, August  1981.

32. "Study  of Emissions  from Heavy-Duty Vehicles", C.  Urban
    and  K. Springer,  Southwest Research Institute,  EPA Report
    No.  EPA 460/3-76-012, NTIS PB  275952, May  1976.

33. "MVMA  Motor  Vehicle   Facts   and  Figures  1982",  Motor
    Vehicle  Manufacturers   Association  of   the  United  States,
    inc.,  1982.

34. "Inspection  and Maintenance for  1981  and Later Model Year
    Passenger Cars",  David  Hughes SAE  Paper 810281, February
    1981.

35. "Mobile  Source  Emission Factors:   For  Low Altitude  Areas
    Only", EPA  Report No. EPA 400/9-78-006,  March 1978.

36. "Ambient  Pollutant  Concentrations  from  Mobile  Sources in
    Microscale  Situations,"  M.   Ingalls  and  R.   Garbe,  SAE
    Paper  820787, June 1982.

37. "Air  Quality  Assessment  of   Particulate  Emissions  from
    Diesel-Powered Vehicles",  PEDCo  Environmental,  Inc.,  for
    EPA  Contract No. 68-02-2515, March  1978.

-------
                            -49-

38.  "The Biochemical Toxicology  of  Methanol",  T.R.  Tephly  et
    al., Essays in Toxicology, 5:149-177, 1974.

39.  "Materials   on   the  Hygienic   Standardization  of   the
    Maximally Permissible Concentration  of  Methanol Vapors  in
    the Atmosphere", Chen-Tsi Chao, Gig.  Sanit.  24(10):7-12,
    1959.

40.  "Methanol:   Its  Synthesis,  Use  as a  Fuel,  Economics,  and
    Hazards",  David  L.  Hagen,  for  the  Energy Research  and
    Development Administration,  December 1976.

41.  "Skin Absorption and Per  Os  Administration  of  Methanol  in
    Men",    B.   Dutkiewicz   et   al,   Int.   Arch.   Occup.
    Environmental Health 47(l):81-88, 1980.

42.  Telephone  conversation  with Barry   Nussbaum,  EPA  Field
    Operations Support Division, 5 May 1983.

43.  "Assessment  of  Human Exposures to  Atmospheric Benzene,"
    S.J. Mara and S.S.  Less,  EPA  Report  No. EPA 450/3-78-031,
    NTIS PB-284  203/7BE, June 1978.

-------