EPA/600/8-88/016
                                                                       June, 1987
                                     HEALTH EFFECTS ASSESSMENT
                                           FOR ALUMINUM
                           ENVIRONMENTAL CRITERIA AND ASSESSMENT OFFICE
                          OFFICE OF HEALTH AND ENVIRONMENTAL ASSESSMENT
                                OFFICE  OF  RESEARCH AND DEVELOPMENT
                               U.S.  ENVIRONMENTAL PROTECTION  AGENCY
                                       CINCINNATI, OH 45268
B
T-
-o

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                                    PREFACE


    This  report summarizes and  evaluates  Information  relevant  to a prelimi-
nary  Interim assessment  of adverse health effects  associated  with aluminum
and compounds.   All  estimates of acceptable Intakes and carcinogenic potency
presented  In this document  should  be considered as preliminary  and reflect
limited  resources  allocated  to  this  project.   Pertinent  toxlcologlc  and
environmental  data were  located through on-line literature  searches  of the
Chemical  Abstracts,  TOXLINE and  the  CHENFATE/DATALOG  data  bases.  The basic
literature  searched  supporting  this  document  1s  current  up to  Hay,  1986.
Secondary  sources  of Information have also been relied  upon  In the prepara-
tion of  this report  and represent large-scale health assessment efforts that
entail extensive  peer  and Agency review.   The following Office of Health and
Environmental Assessment  (OHEA)  sources have been extensively utilized:

    U.S.  EPA.  1984.   Drinking  Water  Criteria Document  for Aluminum.
    Prepared  by  the  Office  of Health  and   Environmental  Assessment,
    Environmental  Criteria  and  Assessment Office,  Cincinnati,  OH  for
    the  Office  of  Drinking  Water,  Washington,  DC.    External  Review
    Draft.

    The  Intent  In  these assessments  1s  to suggest  acceptable  exposure levels
for  noncarclnogens  and  risk  cancer   potency  estimates   for  carcinogens
whenever  sufficient  data were available.  Values were not  derived or larger
uncertainty  factors  were  employed  when  the  variable data were  limited  In
scope  tending   to  generate  conservative   (I.e.,   protective)   estimates.
Nevertheless,  the Interim  values presented  reflect  the relative  degree  of
hazard or risk associated with exposure to the chemlcal(s) addressed.

    Whenever  possible,  two categories  of values  have  been estimated  for
systemic  toxicants  (toxicants  for  which  cancer   Is  not  the  endpolnt  of
concern).  The  first,  RfD$  (formerly AIS)  or subchronlc reference  dose,  1s
an estimate  of  an  exposure  level that would not be expected to cause adverse
effects  when exposure   occurs  during  a  limited  time Interval (I.e.,  for  an
Interval   that does  not  constitute  a significant  portion of  the Hfespan).
This type  of exposure  estimate  has not been  extensively used,  or rigorously
defined,   as  previous  risk  assessment efforts  have been primarily  directed
towards  exposures  from  toxicants  In  ambient  air  or water  where  lifetime
exposure   Is  assumed.    Animal   data  used   for   RFD$  estimates  generally
Include exposures  with durations of  30-90  days.   Subchronlc  human  data  are
rarely available.  Reported exposures are usually  from  chronic  occupational
exposure  situations  or  from  reports  of acute  accidental  exposure.   These
values   are   developed   for   both   Inhalation  (RfD$j)  and  oral   (RfD$o)
exposures.
                                      111

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    The  RfD  (formerly  AIC)  Is  similar  In  concept and  addresses  chronic
exposure.  It 1s an  estimate  of an exposure level  that  would not be expected
to cause  adverse effects when  exposure  occurs  for a significant  portion  of
the llfespan  [see  U.S.  EPA  (1980a)  for  a discussion of this  concept].   The
RfO  1s  route-specific  and  estimates acceptable  exposure  for  either  oral
(RfDg)  or  Inhalation  (RfDj)   with  the  Implicit  assumption  that  exposure
by other routes 1s Insignificant.

    Composite  scores  (CSs)   for   noncardnogens  have also  been  calculated
where  data permitted.   These  values are  used  for  Identifying  reportable
quantities and  the methodology  for  their development  1s  explained  1n  U.S.
EPA (1983).

    For compounds  for which there Is  sufficient evidence  of carclnogenlcHy
RfD$  and  RfD  values  are  not derived.  For  a discussion of  risk  assessment
methodology for  carcinogens refer  to U.S.  EPA  (1980a).   Since cancer  1s  a
process  that  Is  not  characterized  by a  threshold, any  exposure contributes
an Increment  of  risk.  For  carcinogens,  q-|*s have been computed,  If appro-
priate, based on oral and Inhalation data If available.
                                      1v

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                                   ABSTRACT
    In  order to  place  the  risk  assessment  evaluation  1n proper  context,
refer  to the preface of  this  document.   The  preface outlines  limitations
applicable  to  all   documents  of  this  series  as  well   as  the  appropriate
Interpretation and use of the quantitative estimates presented.

    In a  short-term  balance  study using healthy humans,  125 mg aluminum/day
added  to the diet  was  homeostatlcally  controlled with  no adverse  effects
being  noted  (Greger  and  Baler,  1983a).  Up  to 200 mg/day  In  the diets  of
humans may be associated  with reduced  phosphorus absorption  from  the  gastro-
intestinal  tract,  but  not with  Impaired  body function  (Campbell  et  al.,
1957; Greger and Baler, 1983b).

    No RfD values were calculated  for  aluminum.  A CS  of  10 for aluminum was
based on  pulmonary and  thoracic  effects leading to death  in a  chronic  study
1n rats exposed  by Inhalation to aluminum oxide  (Klosterkotter,  1960).

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                               ACKNOWLEDGEMENTS


    The  Initial  draft  of  this  report  was  prepared  by  Syracuse  Research
Corporation  under Contract No.  68-03-3112 for  EPA's  Environmental  Criteria
and  Assessment Office,  Cincinnati,  OH.   Or.  Christopher  DeRosa and  Karen
Blackburn  were the  Technical  Project  Monitors  and  John  Helms  (Office  of
Toxic  Substances) was  the Project Officer.   The final  documents   In  this
series  were prepared  for  the Office  of  Emergency  and Remedial  Response,
Washington, DC.

    Scientists  from  the following  U.S. EPA offices provided  review  comments
for this document series:

         Environmental Criteria and Assessment Office, Cincinnati, OH
         Carcinogen Assessment Group
         Office of A1r Quality Planning and Standards
         Office of Solid Waste
         Office of Toxic Substances
         Office of Drinking Water

Editorial review  for the document series was provided  by the following:

    Judith Olsen and Erma Durden
    Environmental Criteria and Assessment Office
    Cincinnati, OH

Technical  support services  for  the  document   series  was  provided by  the
following:

    Bette Zwayer, Jacky Bohanon and K1m Davidson
    Environmental Criteria and Assessment Office
    Cincinnati, OH
                                      v1

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TABLE OF CONTENTS

1.
2.


3.










4.








5.
6.




ENVIRONMENTAL CHEMISTRY AND FATE 	
ABSORPTION FACTORS IN HUMANS AND EXPERIMENTAL ANIMALS . . .
2.1. ORAL 	
2.2. INHALATION 	
TOXICITY IN HUMANS AND EXPERIMENTAL ANIMALS 	
3.1. SUBCHRONIC 	
3.1.1. Oral 	
3.1.2. Inhalation 	
3.2. CHRONIC 	
3.2.1. Oral 	
3.2.2. Inhalation 	 ,
3.3. TERATOGENICITY AND OTHER REPRODUCTIVE EFFECTS. . . .
3.3.1. Oral 	 ,
3.3.2. Inhalation 	 ,
3.4. TOXICANT INTERACTIONS 	 ,
CARCINOGENICITY 	 ,
4.1. HUMAN DATA 	
4.1.1. Oral 	
4.1.2. Inhalation 	
4.2. BIOASSAYS 	
4.2.1. Oral 	
4.2.2. Inhalation 	
4.3. OTHER RELEVANT DATA 	
4.4. HEIGHT OF EVIDENCE 	
REGULATORY STANDARDS AND CRITERIA 	
RISK ASSESSMENT 	
6.1. SUBCHRONIC REFERENCE DOSE (RfDS) 	 	
6.1.1. Oral (RfDso) 	
6.1.2. Inhalation (RfDcr) 	
Page
. . 1
... 7
. . . 7
. . . 8
. . . 9
. . . 9
. . . 9
n
. . . 12
. . . 12
. . . 13
. . . 14
. . . 14
. . . 15
. . . 15
, . . 16
, . . 16
. . . 16
. . . 16
, . . 16
, . . 16
, . . 17
. . 17
. . 18
. . 19
. . 20
. . 20
. . 20
. . 21
       vll

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                               TABLE  OF  CONTENTS
                                                                        Page
     6.2.   REFERENCE DOSE	   21
            6.2.1.   Oral (RfD0)	   21
            6.2.2.   Inhalation (RfOj)  	   22
 7.  REFERENCES	   25
APPENDIX: Summary Table for Aluminum 	   33

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                              LIST OF  ABBREVIATIONS
 AOP                     Adenoslne dlphosphate
 AMP                     Adenoslne monophosphate
 ATP                     Adenoslne trlphosphate
 CAS                     Chemical Abstract Service
 CS                      Composite score
 DMSO                    Dimethyl sulfoxlde
 FEL                     Frank effect  level
 HA                      Health advisory
 MED                     Minimum effective dose
 NOAEL                    No-observed-adverse-effect level
 ppm                     Parts per million
 RfD                     Reference dose
 RfDj                     Inhalation reference  dose
 RfDg                     Oral  reference  dose
 RfD$                     Subchronlc  reference  dose
 RfD$j                    Subchronlc  Inhalation  reference dose
 RfD$Q                    Subchronlc  oral reference  dose
 RVd                      Dose-rating value
 RVe                      Effect-rating value
TLV                      Threshold  limit value
TWA                      Time-weighted average
                                      1x

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                     1.  ENVIRONMENTAL CHEMISTRY AND FATE

     Selected  physical  and  chemical  properties of  aluminum  and some  of  Its
compounds  are  listed  In   Table  1-1.   Aluminum  (CAS  no.  7429-90-5)  Is  a
metallic  element  with an  oxidation  state of  *3  except  under  extreme condi-
tions  when  oxidation states of *-2 and  «•!  have been found (RolUnson, 1978).
Aluminum  does not exist naturally  In the elemental  form (U.S.  EPA,  1980b),
but  Is found  In -300 minerals  (e.g.,  silicates,  feldspars,  micas  and clays)
(U.S.  EPA, 1984a).
     Aluminum  Is soluble In adds and  bases,  particularly nitric  acid,  hot
acetic acid,  sulfurlc and  hydrochloric  acids  and alkalis.  In  the environ-
ment,  It  may  exist as stable aluminum  salts  or as organo-alumlnum compounds
(Oriscoll, 1985;  U.S. EPA,  1984a).   The half-lives of aluminum and compounds
In air, water and soil  could not  be located In the available literature.   In
the  atmosphere, aluminum  1s expected  to be  present  mainly  In  participate
form as a result  of Industrial  emissions,  fossil fuel  burning and  natural
emissions  Including  those  from  volcanic  sources.   The  ratio of  aluminum
emissions  from anthropogenic sources  to natural  sources  Is 0.15  (F1shbe1n,
1981).   Monitoring data  Indicate that  aluminum  1s  removed  from  the  atmo-
sphere by  partlculate settling and washout  In precipitation  (Landsberger  et
al., 1983; Davidson  et al., 1985; Ulersema et  al., 1984).  Particles  emitted
from anthropogenic sources  tend  to  be smaller  In  size and  transport  over
longer  distances  than those  emitted  from natural  sources  (Mshbeln,  1981).
The  level  of  Al  found  In  natural  waters varies  geographically.   In  waters
where  pH  Is  <5,  as  with  Industrial  wastes,  mine runoff,  acidic  spring
waters, mires and volcanic  areas,  the  aluminum  level  can exceed  100  mg/l.
At pH  levels >5.5, Al*3 Is  nearly Insoluble.
                                    -1-                              11/04/86

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-5-
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    Substances dissolved In the water also affect aluminum water solubility.
ComplexIng  llgands  such as  fluoride,  phosphate and  sulfate,  and chelatlng
agents  such as ethylenedlamlne  tetracetlc  add, nltrllotMacetlc  acid  and
sodium tMpolyphosphate will also Increase the water solubility of aluminum.
The aluminum Ion also complexes  with hydroxide  under aqueous conditions.
    Since aluminum  1s  more soluble  In water  at an addle pH,  It  Is likely
that  It  will  accumulate   1n  aquatic organisms  and  vegetation  under  these
conditions.   Evidence  of photodegradatlon or  oxidation  of aluminum In water
Is not available (U.S. EPA. 1984a).  Strong bonding with  humlc  substances In
sediments by aluminum Is expected (Raspor  et al., 1984).
    The  fate  of aluminum  In  soil  will vary  depending  upon  soil character-
istics,  such  as  soil  type,  pH and  Ion  species present (Drlscoll,  1985).
Aluminum can be Immobilized by  strong  binding with humlc substances (Raspor
et  al.,   1984;  Drlscoll,  1985) and can  be   mobilized  by complexIng  with
HCOl organic and other  acidic  counteranlons  (Drlscoll, 1985).
   o
0114h                               -6-                             11/04/86

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           2.  ABSORPTION FACTORS IN HUMANS AND EXPERIMENTAL ANIMALS
 2.1.    ORAL
     Greger and Baler  (1983a)  conducted a  balance study with  eight healthy
 men.   Four  of the  subjects were  given a  control  diet containing  4.6 mg
 aluminum/day for  20  days,  while the other four subjects received a test diet
 of  125 mg aluminum/day as  aluminum lactate.   The diets were exchanged for an
 additional 20  days  with  each   subject  acting as  his own  control.   Fecal,
 urine  and serum aluminum determinations  Indicated  that  some absorption with
 rapid  elimination  occurred at  125  mg/day.   Other  studies with  different
 aluminum   compounds  (e.g.,   aluminum  carbonate,   aluminum hydroxide)  showed
 that  doses  >1000  mg  aluminum/day  resulted  1n  significant  gastrointestinal
 absorption and retention of aluminum (Recker et  al., 1977; Gorsky  et  al.,
 1979;  Clarkson et al., 1972; Cam et  al.,  1976).   Although  the  data Indicate
 that  homeostatlc  regulation  of aluminum  1s  effective at  doses of  <125  mg
 aluminum/day,  studies  that Investigated  the absorption  of oral  doses  of
 aluminum  between  125  and  1000  mg/day are  not available (U.S.  EPA,  1984a).
 Gastrointestinal  absorption of  aluminum varies not only  with the concentra-
 tion of  aluminum  but  also  with  type  of  aluminum compound and  pH (Savory et
 al., 1983).
    Krlgman  et al. (1985) concluded that  aluminum  Is  absorbed  from the human
 gastrointestinal  tract regardless  of the  form  1n  which  H  occurs.   They
 Indicated  that the  proportion  of  Ingested  aluminum  absorbed  Is  small  and
 estimate  that  -35 mg/day  Is Ingested.   In a  review  of the pathogenesls  of
 the  nervous  disorder,  dialysis  encephalopathy,  AMeff  (1985)   stated  that
 "significant absorption of  oral  aluminum can  occur In patients  with  chronic
 renal  failure," Implying  that absorption may  be  enhanced 1n these patients
and that they may  be a group with Increased  risk  to the toxldty of  aluminum.


0114h                               -7-                               02/11/87

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2.2.   INHALATION
    Studies with  humans have  shown  that aluminum  accumulates  In the  lungs
with age  (Upton and  Shafer,  1964; Alfrey,  1980)  and that aluminum levels  In
the  lungs  were relatively  high compared with  other tissues.  Including  the
trachea,  gastrointestinal   tract   and  visceral   organs   (Teraoka,   1981).
Although  thts  Information  suggests   that  pulmonary  absorption of  aluminum
dusts may  have occurred, this  cannot  be concluded  definitely  because  serum
aluminum  levels  and  other  pertinent  endpolnts  were not  assessed.   Particle
size  and  solubility  of  aluminum partlculate  and  compounds  may  determine
their fate In the lungs (U.S. EPA, 1984a).
0114h                               -8-                              11/04/86

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                3.  TOXICITY IN HUMANS AND EXPERIMENTAL ANIMALS
 3.1.    SUBCHRONIC
 3.1.1.    Oral.   Aluminum  Interacts  with  phosphorus  In  the gastrointestinal
 tract  to form Insoluble aluminum phosphate, which  Is readily excreted (U.S.
 EPA,  1984a).  Prolonged  aluminum  Intake from  antacids  (aluminum hydroxide)
 can  lead  to phosphorus depletion  with  hypercaldurla,  bone  resorptlon  and
 osteomalada 1n humans.
    As  discussed  1n Section 2.1.,  humans treated with  aluminum added to  the
 diet  at  125 mg/day  (1.8 mg/kg/day)  homestatlcally eliminate  the  absorbed
 excess  without evidence of 111 effects.
    It  appears that  dietary  Intake  at  levels  up  to -200  mg aluminum/day,
 although  associated with decreased  gastrointestinal  uptake  of phosphate,  Is
 not  sufficient to  Interfere with  bodily  function  (Campbell  et al.,  1957;
 Greger  and  Baler,  1983b).   Intake  of  aluminum compounds  In  the   form  of
 antacids  1n amounts of  >1 g aluminum/day may  cause  significant Interaction
 with  phosphorus   1n healthy  Individuals  (Insogna  et al.,  1980;  U.S. EPA,
 1984a).
    Persons  with  severe  reduction   of  renal   function  are commonly  given
 aluminum  hydroxide  orally 1n  large  amounts (~3  g  aluminum/day) to  prevent
 hyperphosphatemla (U.S.  EPA, 1984a).  This  large aluminum load may  lead  to
 Increased  aluminum  levels  1n the  bone and  possibly the  brain,  which  can
 result  1n osteomalada and  dialysis  encephalopathy.   An Increased risk  for
 encephalopathy has  been determined  when  serum  levels of  aluminum are >100
 yg/mt  as  compared  with  normal  levels  of  -5  yg/l  (U.S.   EPA,   1984a).
 High brain  aluminum levels have  also been associated with  encephalopathy  1n
 the elderly  and  In  Alzheimer's patients,  but 1t has  not been  established  1f
aluminum acts as  a direct causative agent (U.S.  EPA, 1984a).


0114H                               -9-                             02/11/87

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    Aluminum  chloride  was  administered  orally  (apparently   by  gavage  in
water)  to  unspecified numbers of male rats  and  male  guinea pigs at  doses of
0,  6,  17 and 50 mg alumlnum/kg/day  and  to male rabbits at  doses  of  0,  3,  9
and 27  mg  aluminum/kg/day for 20-30 days  (Krasovsk11  et  al.,  1979).   Assays
apparently  conducted  3 hours  after  cessation of  treatment  showed decreased
activity  of  serum  alkaline  phosphatase at  >17 mg/kg/day  1n  the rats  and
guinea  pigs,  and  >9 mg/kg/day In the  rabbits.   Serum levels of ATP,  AOP and
AMP were significantly decreased  In the  rats and guinea pigs  at >17  mg/kg
and In  the  rabbits  at 27  mg/kg.   Rats  were also similarly exposed to 0.0025,
0.25  or  2.5 mg  aluminum/kg/day  (as  aluminum  chloride)   for  6-12  months
(Krasovskll et  al., 1979).  Effects Included decreased serum  alkaline  phos-
phatase  and depressed motor  reflexes at 2.5  mg/kg; alkaline phosphatase was
also decreased  at 0.25 mg/kg, but  only during  the first month of exposure.
Treatment-related effects on  blood  erythrocytes  B-l1poprote1ns or  unspeci-
fied  transamlnase  activity   were   not   observed.   Additional  Information
regarding the design  or results  of  the  Krasovskll  et al.  (1979) experiments
was not reported.
    Gross  and  hlstologlcal   examinations  of   the  liver,  lungs,   spleen,
kidneys, brain, heart  and testes  of  groups of seven male  Sprague-Dawley rats
exposed  to  0,  5,  50 or  500 mg aluminum/1 (as  aluminum  chloride)  In  the
drinking water for 30, 60 or 90 days were unremarkable (Olxon et al.,  1979).
    Groups  of  eight male Fischer  or  eight  female Sprague-Oawley rats  were
subjected to  behavioral  tests that  assessed coordination,  locomotor  activity
and learning  at different points throughout a  12-week period  In  which  0.2%
aluminum (as aluminum chloride) was  administered In the diet (CommissarIs et
al.,  1982).  Significantly   depressed   locomotor  activity  occurred  In  the
OlMh                               -10-                             11/04/86

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 females;  the males  only showed  a  trend 1n  this  effect.   If  1t Is assumed
 that rats consume the equivalent of  5X of  their weight In food per day, the
 dally dosage was  100 mg  alumlnum/kg/day.
     Dietary  administration  of  0.1%  aluminum  (as  aluminum  chloride)  for 11
 months depressed  locomotor  activity  and learning  (acquisition of avoidance
 behavior)  1n Sprague-Dawley rats (Commissar 1s  et  al.,  1982).  This exposure
 corresponds  to  SO mg/kg/day  If  It  assumed that  rats consume the equivalent
 of  5% of  their  weight 1n  food per day.
 3.1.2.    Inhalation.   Gross et  al.  (1973)  exposed  groups  of  14-30  guinea
 pigs,  rats   and  hamsters  to five metallic  aluminum  powders  (pyro,  atomized
 and  flaked)  at  air  concentrations  of 15, 30,  50 or  100 mg/m3, 6 hours/day,
 5  days/week  for  6   months.   Alveolar  protelnosls  occurred  1n  all  three
 species  after  2  months  of exposure  but other  adverse  pulmonary  effects,
 Including flbrosls,  did not develop.
     Groups   of  35 Fischer   rats/sex  and  35  Hartley  guinea  pigs/sex  were
 exposed  to   0.25,  2.5  or  25 mg/m3 aluminum  chlorohydrate,  6  hours/day,  5
 days/week for  6  and 12  months   (Cavender et  al.,  1978).   After 6  months,
 alveolar  macrophages were Increased at all three  exposure levels; decreased
 body  weight, Increased  lung-to-body  weight  ratios  and  multlfocal  granulo-
 matous  pneumonia  also  occurred  at  25 mg/m3.  Granulomas  occurred  In  the
 lungs  of  2.5 mg/m3  animals  (both species)  after 12  months  of  exposure.   It
 should be noted that the actual  structure  of  aluminum chlorohydrate  Is  not
 known, but   1s  considered to be  a  complex  of  basic  aluminum  chloride  and
 propylene glycol.
     Information  regarding effects  of exposure  to  soluble salts  of  aluminum
 (e.g., chloride and  sulfate)  could  not  be  located.   It appears,  however,
OlHh                               -11-                             06/03/87

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that  for  soluble  salts  of  aluminum,  effects  may  be acute  In nature  and
associated with  the  corresponding add formed by hydrolysis of  the  aluminum
compound.   Reflecting  this,  the  TIV for  soluble  aluminum salts of 2  mg/m3
Is  based  on  the  TLV  for  hydrochloric  acid  assuming  1 mol  of  aluminum
chloride  yields  3  mol  of  HC1  on  hydrolysis  and assuming  similar   toxic
potencies for the acids formed by hydrolysis of different  aluminum salts.
3.2.   CHRONIC
3.2.1.   Oral.   Aluminum  chloride was administered  to  groups  of 10 mice  1n
drinking  water  at  an  average  dose  of  0  or  19.3 mg  alumlnum/kg/day  In  a
3-generatlon  study (Ondrelcka  et  al., 1966).   The parental  generation  was
treated for  180-390  days  and unspecified  numbers of weanlings were  similarly
treated from 4  weeks of age.  Decreased  body weight In the second and  third
generations  was  the only effect  of  treatment.   Erythrocyte  counts,   hemo-
globin levels  and histology of  the liver, spleen  and  kidneys  In mice from
the first  and third generation were  similar  to controls.  The  significance
of  the  decreased  weight  gain  Is  difficult to  assess,  however, since food
consumption  was  not  reported;   decreased food  Intake  was   observed  with
aluminum exposure 1n other studies Included 1n the  same report.
    Schroeder and MUchener  (1975a) administered 5  ppm  aluminum  (as  aluminum
potassium sulfate) 1n the drinking water  of 52  Long-Evans  rats/sex  for  life.
Exposed  rats did  not   differ  from  controls  with  respect to  body weight,
survival,  selected  serum  chemistries  (glucose,   cholesterol,   uric   add)
selected  urlnalysls  parameters  (protein,  glucose,  pH) or tissue histology
(heart, lung, kidney, liver or  spleen).
    Groups of  54 weanling Swiss mice/sex were  exposed to 0 or  5 mg aluml-
num/i  (as  aluminum potassium  sulfate)   In  the  drinking water  for  life
(Schroeder and MUchener,  1975b).   If It Is assumed that  mice consume  water
equivalent to  17% of their  weight  per day, the dosage Is 0.85 mg/kg  day.

0114H                               -12-                             11/04/86

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 Treatment  had no  effect on  body  weight, survival, edema,  blanching of the
 Incisor  teeth,  or  tissues  as  Indicated by  gross and  limited hlstologlcal
 ("some  sections" were  made  of  the heart,  lung,  liver,  kidney  and spleen)
 examinations.
 3.2.2.   Inhalation.   Pulmonary flbrosls  has been  associated with  occupa-
 tional exposure  to  aluminum powder (metallic aluminum covered with a complex
 oxide/hydroxide  coating)  or alumina  (Al_0») dust  1n  a  number  of  reports
 (U.S. EPA,  1984a);  however, U.S.  EPA (1984a) demonstrated that these reports
 are  Inconclusive because confounding factors  such  as  concurrent exposure to
 other chemicals  (e.g.,  alloying agents, chemicals used  1n the production of
 fireworks,  Inks  and paints  or  silica),  cigarette  smoking (which contributed
 directly to the lung burden of aluminum and  silicon)  or  previous workplace
 exposures  were  not  always  evaluated.   ACGIH  (1986)  and  U.S. EPA  (1984a)
 report  that  there  Is  no  evidence of  flbrogenlc activity  of aluminum or
 alumina  at  exposure  levels  currently  recommended  by  the  ACGIH   (10  mg/m3
 for  dust,  5 mg/m3  for  powder)  and suggest that they  be classified as  Inert
 (nuisance)   partlculates.    Past  exposures  associated  with  flbrotlc  lung
 changes  occurred at extremely high concentrations  In  poorly or uncontrolled
 occupational  environments;   Insufficient monitoring data preclude  estimation
 of typical TWA concentrations of aluminum.
    Aluminum powders  have  been  administered to humans 1n  known exposures In
 the  treatment  of  slllcosls.  Stoklnger  (1981)  reviewed  data  1n   which  >42
million  aluminum  treatments (-150,000  man-years)  had  been  given  over  a
27-year  period  ending   1n  1971.    Inhalation of  ~350  mg/m3  of  resplrable
alumina powder for  10 minutes/day  did not  result  In  lung damage or other 111
effects;  this  exposure  reportedly  Is equivalent to an 8-hour  TWA  concentra-
tion of  7  mg/m3 (U.S.  EPA, 1984a).  The data  from  this study were  used as
the basis for the TLV (Stoklnger,  1981;  ACGIH, 1986).    .

0114h                               -13-                             02/11/87

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    Exposure  to 2.18  rag/m3 aluminum  fibers,  6  hours/day,  5  days/week  for
up  to 86  weeks  produced slight  Increases  In alveolar  macrophages  and  some
Irritation  of  the  nasal passages In a  group  of  50 Alderly Park rats (Plgott
et  al.,  1981).   Lung edema, pneumonia  and  pleurisy were observed In 107/145
rats  that  died   from  exposure  to  33  g/m3  aluminum  oxide  (Al 0.),  5
                                                                     fc O
hours/day  for up to 285/402 days (Klosterkotter, 1960).
    The  responses  observed  1n  the  above  animal  studies  are  typically
elicited by nuisance participate exposure.
3.3.   TERATOGEN1CITY AND OTHER REPRODUCTIVE EFFECTS
3.3.1.   Oral.  Groups  of 31 male  Sprague-Dawley  rats  were  administered 0,
5.  50 or  500  mg  aluminum/I (as  aluminum  chloride)  1n the drinking water
(Dlxon et  al.,  1979).   Seven rats  from  each  group were sacrificed  after  30,
60  and  90  days   for   plasma   lutenlzlng   hormone  and  follicle-stimulating
hormone  determinations,  and  hlstologlcal  examination   of  the  testes.   The
remaining  10 males  from each group were mated after  90 days  of treatment;  a
different  female was  paired with  each  male every  7  days  for a  total of 70
days.  Treatment-related effects  on reproductive  capacity  as  Indicated  by
the above  evaluation were not observed.   Endpolnts  In the  reproduction study
Included pregnancy  rate,  Implantation  sites,  corpora lutea,  resorptlon sites
and live and dead Implants.
    Decreased spermatozoa counts and  sperm motllHy reportedly  occurred In
rats  that  were  exposed  to  2.5  mg alumlnum/kg/day  (as  aluminum chloride) by
gavage  but not  at  lower  doses  (0.0025  or   0.25  mj/kg/day)  for  6  months
(Krasovskll et  al., 1979).   Hlstologlcal  and  hlstochemlcal  alterations  In
the testes  were also  observed  at  the  2.5  mg/kg/day dose.  As Indicated In
Section 3.1.1., aspects of this  report are Inadequate.
0114h                               -14-                             11/04/86

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     Anderson et al. (1985) exposed sperm-positive Holtzman rats to plain tap
 water  (four rats)  or  to a Maalox  TC-tap water mixture at  a 1:4 ratio (six
 rats)  beginning on  day  2 of gestation until weaning  to  test the effects of
 high Ingested  levels  of  aluminum on reproductive performance.  Water  Intake
 was  not  measured and .aluir, num Intake was not estimated.  At  parturition, one
 control  and one  treated   Hter  were cross-fostered to  evaluate the effects
 of  high  levels of  Ingest  J aluminum on maternal  care.  One  aluminum-exposed
 Utter  was  aborted,  but  11 control  dams delivered  normally.  Body weights
 were reduced  (p<0.05,  Ne nan-Kenls test) In aluminum-exposed  rats  at birth
 and  at  time points  up tc 70 days  postpartum (p<0.01) In Utters maintained
 with dams  exposed  until  weaning.   Body weights  of pups from  treated dams
 recovered  1f the  pups  wen cross-fostered by  an untreated dam.
 3.3.2.   Inhalation.   Per Inent  data could not  be located  In  the available
 literature.
 3.4.   TOXICANT INTERACTi: NS
     As  Indicated In Sect')n 2.1.,  aluminum Interacts  with  phosphorus In the
 gastrointestinal  tract    o  form  Insoluble  aluminum  phosphate,  which  1s
 readily  excreted (U.S. E: \, 1984a).   Fluoride  has also been shown  to react
 with aluminum  1n the gast. :>Intestinal tract (U.S. EPA, 1984a).
OlHh                               -15-                             11/04/86

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                              4.  CARCINOGENICITY
4.1.   HUNAN DATA
4.1.1.   Oral.   Pertinent  data  could  not  be  located  In  the  available
literature.
4.1.2.   Inhalation.    Occupational   exposure  -to  aluminum  has  not  been
associated with  pulmonary  or  systemic neoplastlc alterations  In humans  (U.S.
EPA, 1984a; ACGIH, 1986; Stoklnger, 1981).
4.2.   8IOASSAYS
4.2.1.   Oral.   Schroeder  and  HHchener  (1975a)  administered drinking water
containing 5  mg/i aluminum (as  aluminum potassium sulfate) to  groups of  52
Long-Evans weanling  rats/sex  for life.  Effects  on body weight  or  longevity
were not  observed,  but 13  males and 14  females  died  at age 20 months  from
nontreatment-related  pneumonia.   Gross  and  limited   (heart,  lung,  kidney,
liver, spleen, tumors) hlstologlcal examinations  were  conducted.
    The  Incidence  of  total   gross   tumors  (all  sites)  was  significantly
(p<0.005)  Increased  In  treated  males   (13/25  vs.  4/26).  -Incidences   of
specific types  of  tumors were  not  specified,  but Incidences of tumors con-
sidered  malignant  (multiple  tumors   In  the same  animal)  were  6/25 In  the
treated  and  2/26  In the  controls.   The authors  considered  aluminum to  be
Innocuous.   Schroeder  and  MUchener  (1975b)  also   administered   aluminum
potassium  sulfate  In the  drinking water (5 mg  alumlnum/i)  of   groups of  54
Swiss  mice/sex  for   life.   Treatment  had  no  effect  on  body  weights   or
survival.  Gross pathological  and  limited hlstologlcal  examinations  revealed
an  Increased  Incidence of  lymphoma  leukemia  1n  the  treated females  (10/41
vs. 3/47, p<0.025);  however, the authors  did not  consider  the compound to  be
tumorIgenlc.
0114h                               -16-                             02/11/87

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 4.2.2.    Inhalation.   Groups of 35  rats  and  guinea pigs/sex were exposed by
 Inhalation to 0.25,  2.5  or 25 mg/m3  of  aluminum chlorohydrate 6 hours/day,
 5  days/week  for  6-12  months  (Cavender et  al.,  1978).   Lung  granulomas
 occurred  1n  both  species  following  exposure to  25  mg/m3 for  6  months and
 2.5  mg/m3  for 12 months.
     Granulomatous  nodules  were  also observed  In male  hamsters  that were
 exposed  6  hours/day,  5 days/week  for  20  or  30 exposures to average aluminum
 chlorohydrate concentrations   of   52  mg/m3   (Drew   et  al.,  1974).   These
 alterations  persisted up  to  6 weeks postexposure  but  only minor  changes (a
 few   foci  of  macrophages  and  heterophlls)   occurred  after  10  exposures.
 Groups  of  four  exposed  and four control hamsters  were sacrificed after 10,
 20  and  30 exposures  and  2, 4  and  6 weeks  postexposure}.   The granulomatous
 foci  consistently  developed  at  the  bifurcation  of the  bronchloloalveolar
 ducts, a probable  site of  partlculate deposition.
 4.3.   OTHER  RELEVANT DATA
     Administration  of  aluminum  or  aluminum  compound   (aluminum  hydroxide,
 oxide  or  phosphate)  by   different  routes  (Intratracheal,  Intraperltoneal,
 Intravenous,  subcutaneous  Implant)  In  rats, guinea pigs and hamsters did not
 elicit  treatment-related  tumor  formation (O'Gara  and  Brown, 1967;  Shublch
 and  Hartwell, 1969;  Wagner et al.,  1973;  Stenback  et  al., 1976;  Turk  and
 Parker, 1977).
     Elemental  aluminum dissolved  1n  DMSO  was  not mutagenlc In  Salmonella
 typhlmurlum strains TA98,  TA1535  and TA1538 (Mllvy and  Kay, 1978).  Aluminum
 chloride  (A1C1.) did  not  produce  effects In  a  ONA damage/repair  assay with
 Bacullus  subtllls  strains  M45  (rec~)   and   H17   (rec*)  (Nlshloka,  1975),
 but  did  produce chromatId breaks  and  gaps   In  mouse  bone  marrow  cells  In
 vitro (Manna and Das, 1972).


0114h                               -17-                             11/04/86

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4.4.   WEIGHT OF EVIDENCE
    Aluminum  potassium  sulfate  was  administered  1n  the drinking water  of
rats  (Schroeder and  MHchener,  1975a)  and  mice  (Schroeder and  Kitchener,
19755)  at a  concentration of 5  mg aluminum/I  for  life.  The  Incidence  of
total tumors  was  significantly Increased 1n  the male  rats  but  Incidences  or
characterization of  specific types of  tumors were not  reported.   The  Inci-
dence of  lymphoma  leukemia was  significantly Increased  In the  female  mice.
Granulomas developed  In the  lungs  of rats  and guinea  pigs  that  Inhaled  2.5
mg/m3 aluminum  chlorohydrate, 6  hours/day,  5 days/week  for 12 months  or  25
mg/m3  for 6  months  (Cavender et  al.,  1978).   Exposure to 52 mg/m3  alumi-
num  chlorohydrate  (20-30  exposures,  6  hours/day, 5  days/week)  produced  a
similar response  In hamsters  (Drew et al.,  1974).   These  responses  cannot
deflnately be  attributed  solely  to  aluminum,  however, because the  actual
structure of  aluminum  chlorohydrate Is  not known  (see  Section  3.1.2.).   The
available data  are Inadequate  for  evaluating the carclnogenlclty  of  alumi-
num.  Aluminum  1s, therefore, most  appropriately categorized  In  IARC  Group 3
and  CAG  Group  C  according to  the guidelines for  evaluating  the  weight  of
evidence of human carcinogenic potential (U.S. EPA, 1986).
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                     5.  REGULATORY STANDARDS ANO CRITERIA

     The ACGIH (1986) currently recommends 8-hour TWA TLVs of 10,  5,  5, 2 and
 2 mg  alumlnum/m3  for  occupational  exposure  to  aluminum metal  dusts, pyro
 powders,  welding fumes,  soluble  salts and alkyls, respectively.
0114H                               -19-                             06/03/87

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                              6.  RISK ASSESSMENT
6.1.    SUBCHRONIC REFERENCE DOSE (RfD$)
6.1.1.   Oral  (RfOSQ).   As  discussed  1n  Sections  3.1.1.  and  3.1.2.,  the
mechanism  of aluminum  toxlclty  appears to  be  Indirect, resulting  from  the
Interaction  of aluminum  and  phosphate.   Excessive  exposure  to aluminum  1s
associated   with  phosphate   depletion,  resulting   In  bone   resorptlon,
osteomalacla  and  hypercaldurla.   Results  of the  Greger  and  Baler  (1983a,b)
study  Indicate  that  absorption  of aluminum  occurs 1n  healthy  humans treated
with  125  mg aluminum/day without  retention  1n  the body  and  that effects  on
phosphorus  absorption  1n the  gastrointestinal  tract  at  this  dose  are  very
small  and  physiologically  Insignificant.    Although  homeostatlc control  of
aluminum appears to  be  effective at  125 mg aluminum/day, the  minimal effects
on  phosphorus  absorption Indicate  that this Intake  may represent  a  NOAEL.
In  humans,  1ngest1on  of  1 g aluminum (14.3 mg/kg/day)  Is  associated  with
significant  Interaction  with  phosphorus 1n  healthy  Individuals (Insogna  et
al.,  I960).   In subchronlc  animal  tests,  2.5  mg alumlnum/kg/day   has  been
associated  with decreased  serum  alkaline  phosphatase  and  depressed  motor
reflexes 1n  rats  (Krasovskll  et al.,  1979)  and  100  mg/kg/day  with  depressed
locomotor activity In rats (Commissar 1s et  al.,  1982).
6.1.2.   Inhalation  (RfD^,).    Subchronlc  data  regarding  the  toxlclty   of
aluminum,  soluble  salts  of  aluminum,  and  aluminum  alkyls are  Insufficient
for derivation of an RfO-, for these compounds.
6.2.   REFERENCE DOSE (RfD)
6.2.1.   Oral  (RfDQ).    The  aval'able data  were deemed Insufficient  for
RfDQ calculation.
    Long-term  Intake  of  aluminum  compounds (e.g.,   aluminum  hydroxide  In
antacids)  In  amounts  of  -1  g  aluminum/day or   more may  cause   phosphate
depletion,  which  can  eventually  lead to  osteomalacla  (U.S.  EPA,  1980b).

OIHh                               -20-                             06/03/87

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 Smaller amounts of aluminum will cause decreased uptake of phosphate that Is
 not  severe  enough to elicit  adverse  effects.   Higher  dosages  (~3 g alumi-
 num/day),  administered to persons with severe reduction of renal function to
 prevent hyperphosphatemla,  can lead to accumulation of aluminum 1n the brain
 and  dialysis encepalopathy.  A  CS  can  be calculated for aluminum by regard-
 Ing  the 1 g aluminum/day Intake as  the MED for  phosphorus  depletion.   The
 RV.  associated  with  this  MED  1s  1.    If  phosphate  depletion  potentially
 resulting  1n adverse  physiological  effects  1s  assigned an RV   of  7, the CS
 1s 7.
 6.2.2.   Inhalation  (RfD.).   As  discussed In  Section  3.1.2.,  there Is  no
 evidence  of  flbrogenlc activity  or  other nonreverslble pulmonary effects of
 aluminum  powders or alumina  dusts  at  the TLVs (5  mg/m3  for  pyro powder, 10
 mg/m3  for  dust)  (ACGIH,  1986).   TWA  concentrations  reflect  possible  human
 NOAELs  but  cannnot  be used  to  calculate an RfD,  for  aluminum.   It should
 be  noted  that  local  pulmonary  effects of  aluminum  are  presumed to  be
 Independent  of  homeostatlc regulation.
    Granulomatous  pneumonia  occurred   1n rats  and  guinea  pigs  that  were
 exposed  to  0.25,  2.5 or  25  mg/m3  aluminum  chlorohydrate by  Inhalation,  6
 hours/day,  5 days/week  for  6 months  (Cavender  et  al.,  1978);  granulomas
 developed  after 12  months  exposure to  25 mg/m3.   These data  are  Inappro-
 priate  for  RfDoj calculation  because  the effects have  not been  observed 1n
 humans  at  comparable  or  higher  exposures  and.  furthermore,  because  the
 effects cannot definitely be attributed to aluminum.
    Although  ACGIH (1986)  provides TLV  values  for  fumes,  soluble  salts  and
 alkyl compounds  of aluminum,  since  the  TLVs are not based on  extensive  human
 data and  Inhalation toxlclty  data  on  these  forms  of  aluminum  are  lacking,
     values  for these forms of aluminum cannot be derived.
0114h                               -21-                             06/03/87

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     Derivation  of  a CS for  Inhaled  aluminum  1s  complicated  by the fact that
specific  Information  regarding pulmonary  effect  levels  In humans 1s limited.
It  Is  apparent, however,  that exposures  exceeding  the  TLV by many times  are
necessary  to elicit  adverse  effects.  F1bros1s  Is  an equivocal  effect  of
aluminum  exposure  1n  humans  and has  not been produced  1n  exposed animals.
Lung alterations consistent  with Inhalation  of nuisance participates (poten-
tially  reversible   effects),  therefore,  appear  to  be  the  most  appropriate
basis  for  a  CS.   Since  these  types  of  alterations have been  produced  In
animals at known exposures,  animal  effect levels  (see Section 3.2.2.)  can be
used to calculate  the CS.  Lung edema, pneumonia  and pleurisy sufficient to
Induce  death   occurred   In  rats  exposed  to  33  g/m3  of   aluminum  oxide
(-17.2 g  alumlnum/m3), 5  hours/day for  up  to 285/402  days (Klosterkotter,
1960).  Slight  Increases   1n  alveolar  macrophages  and  some  nasal Irritation
were observed  1n  rats exposed  to  2.18  mg/m3  of  aluminum  fibers, 5  days/
week for  up  to  86 weeks  (Plgott et  al.,  1981), but these effects seem mini-
mally  adverse.   The  17.2 g  alumlnum/m3  FEL  1s equivalent  to  1.6  g/kg/day
If  It   Is  assumed that  the  respiratory rate  was  0.223  mVday  and  body
weight was 0.35 kg.   Multiplying this dose by the  cube root of  the ratio of
animal weight to human body  weight  (assumed  70 kg)  gives a human MED of 19.2
g/day  for  a   70 kg man.   The  RV.  associated  with  the dose  Is  1  since  log
MEO  1s  >3.   The mortality associated  with  this  exposure  1s given  an  RV   of
10.  A  CS of 10.  the  product of   the  RVd  and RVe>  results.   Since  the  CS
associated with Inhalation exposure to aluminum  1s greater  than  that  asso-
ciated with  oral  exposure,  the  Inhalation  CS of 10  1s  adopted  to represent
the toxlclty of aluminum.   A CS of 10 corresonds to an RQ of  1000.
01 Hh                               -22-                             06/03/87      ™

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                                7.  REFERENCES

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Clarkson.  E.M..  V.A. Luck, W.V. Hynson, et  al.   1972.   The effect of alumi-
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Krasovskll,  G.N.,  UY.   Vasukovlch  and  0.6.  Charle.   1979.   Experimental
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