DTIC ADA453968: Chlorine Dioxide Disinfection in the Use of Individual Water Purification Devices

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Chlorine  Dioxide  Disinfection  in  the  Use  of 
Individual  Water  Purification  Devices 


Technical  Information  Paper  #31-007-0306 


PURPOSE 

This  information  paper  provides  an  in-depth  review  of  chlorine  dioxide  as  a  disinfectant  in 
potable  water  supplies.  This  paper  is  intended  to  assist  the  reader  in  evaluating  the  disinfection 
capabilities  of  Individual  Water  Purification  Devices  (IWPDs)  using  chlorine  dioxide  to  kill  or 
inactivate  disease-causing  bacteria,  viruses,  and  protozoan  cysts. 

REFERENCES 

Appendix  A  contains  a  list  of  references. 

INTRODUCTION 

Background 

Understanding  the  disinfection  capabilities  of  chlorine  dioxide  to  kill  or  inactivate  disease- 
causing  microorganisms  is  important  in  protecting  soldiers,  who  are  considering  using  this 
technology,  from  acute  health  threats  posed  by  these  microorganisms.  Soldiers  deployed  beyond 
traditional  field  drinking  water  supplies  must  have  access  to  microbiologically  safe  water.  Using 
IWPDs  is  one  way  to  provide  microbiologically  safe  water  in  these  situations.  These  IWPDs 
must  protect  the  Soldier  from  acute  microbial  health  threats.  The  U.S.  Environmental  Protection 
Agency  (EPA)  Guide  Standard  and  Protocol  for  Testing  Microbiological  Water  Purifiers 
(reference  1)  provides  performance  standards  by  which  an  IWPD  using  chlorine  dioxide  can  be 
evaluated.  The  perfonnance  standards  are  a  minimum  6-log  reduction/inactivation  of  bacteria, 
4-log  reduction/inactivation  of  viruses,  and  3-log  reduction/inactivation  of  protozoan  cysts. 
Chlorine  dioxide-using  IWPDs  meeting  these  standards  are  considered  effective  against  disease 
causing  bacteria,  viruses,  and  protozoan  cysts.  Some  IWPD  manufacturers  test  their  devices 
using  this  protocol.  This  is  the  best  way  to  evaluate  the  IWPDs  disinfection  capabilities.  In  the 
absence  of  that  testing  data,  this  infonnation  paper  can  be  used  to  gain  an  understanding  of 
chlorine  dioxide  disinfection  capabilities  and  help  determine  if  an  IWPD  using  chlorine  dioxide 
could  successfully  meet  the  EPA  Guide’s  minimum  performance  standards. 

General 

Chlorine  dioxide  (CIO2)  was  discovered  in  1811  (reference  2).  It’s  widely  used  in  numerous 
industries  including  wood  pulp  processes,  wastewater  treatment,  and  food  processing.  Water 
treatment  plants  in  the  United  States  first  used  chlorine  dioxide  in  the  1940s  for  taste  and  odor 
control  (reference  3).  In  addition  to  taste  and  odor  control,  many  drinking  water  systems 


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1.  REPORT  DATE 

MAR  2006 


2.  REPORT  TYPE 

technical 


3.  DATES  COVERED 

00-10-2005  to  00-03-2006 


7.  PERFORMING  ORGANIZATION  NAME(S)  AND  ADDRESS(ES) 

U.S.  Army  Center  for  Health  Promotion  and  Preventive  Medicine 
(USACHPPM),5158  Blackhawk  Road, APG,MD, 21010 

9.  SPONSORING/MONITORING  AGENCY  NAME(S)  AND  ADDRESS(ES) 


4.  TITLE  AND  SUBTITLE  5a.  CONTRACT  NUMBER 

Chlorine  Dioxide  Disinfection  in  the  Use  of  Individual  Water  Purification  5b  GRANT  NUMBER 

Devices  - 

5c.  PROGRAM  ELEMENT  NUMBER 

6.  AUTHOR(S)  5d.  PROJECT  NUMBER 

Steven  Clarke;  William  Bettin  31-007-0306 

5e.  TASK  NUMBER 
5f.  WORK  UNIT  NUMBER 

7.  PERFORMING  ORGANIZATION  NAME(S)  AND  ADDRESS(ES)  8.  PERFORMING  ORGANIZATION 

U.S.  Army  Center  for  Health  Promotion  and  Preventive  Medicine  report  number 

(USACHPPM),5158  Blackhawk  Road, APG,MD, 21010  TIP  31-007-0306 

9.  SPONSORING/MONITORING  AGENCY  NAME(S )  AND  ADDRESS(ES )  10.  SPONSOR/MONITOR' S  ACRONYM(S) 

11.  SPONSOR/MONITOR'S  REPORT 
NUMBER(S) 

12.  DISTRIBUTION/AVAILABILITY  STATEMENT 

Approved  for  public  release;  distribution  unlimited 

13.  SUPPLEMENTARY  NOTES 

14.  ABSTRACT 

Soldiers  deployed  beyond  traditional  field  drinking  water  supplies  must  have  access  to  microbiologically 
safe  water.  Using  Individual  Water  Purification  Devices  (IWPDs)  is  one  way  to  provide  microbiologically 
safe  water  in  these  situations.  These  IWPDs  must  protect  the  Soldier  from  acute  microbial  health  threats. 
Understanding  the  disinfection  capabilities  of  chlorine  dioxide  to  kill  or  inactivate  disease-causing 
microorganisms  is  important  in  protecting  soldiers,  who  are  considering  using  this  technology,  from  acute 
health  threats  posed  by  these  microorganisms.  This  information  paper  provides  an  in-depth  review  of 
chlorine  dioxide  as  a  disinfectant  in  potable  water  supplies.  This  paper  is  intended  to  assist  the  reader  in 
evaluating  the  disinfection  capabilities  of  IWPDs  using  chlorine  dioxide  to  kill  or  inactivate  disease-causing 
bacteria,  viruses,  and  protozoan  cysts. 

15.  SUBJECT  TERMS 

water;  drinking  water;  water  treatment;  purification;  chlorine  dioxide;  disinfection;  military;  IWP 
(individual  water  purifier);  pathogen  removal 


16.  SECURITY  CLASSIFICATION  OF: 


a.  REPORT 

unclassified 


b.  ABSTRACT 

unclassified 


c.  THIS  PAGE 

unclassified 


17.  LIMITATION  OF 

18.  NUMBER 

ABSTRACT 

OF  PAGES 

14 

RESPONSIBLE  PERSON 


Standard  Form  298  (Rev.  8-98) 

Prescribed  by  ANSI  Std  Z39-18 


TIP  #31-007-0306 


throughout  the  world  today  use  chlorine  dioxide  for  disinfection,  control  of  organic  disinfection 
byproducts  (e.g.,  trihalomethanes),  and  oxidation  of  iron  and  manganese.  Currently,  there  are 
only  a  few  Commercial-Off-The-Shelf  (COTS)  IWPDs  using  chlorine  dioxide  for  disinfection. 

CHLORINE  DIOXIDE  CHEMISTRY  IN  WATER 

General 

Chlorine  dioxide  exists  as  an  undissociated  gas  dissolved  in  water  at  a  near  neutral  pH  range  (pH 
6-9)  (reference  4).  Because  chlorine  dioxide  exists  as  a  gas  it  is  vulnerable  to  volatilization;  it 
can  be  easily  removed  from  water  by  turbulent  aeration,  and  is  destroyed  by  ultraviolet  light 
when  exposed  to  sunlight  (reference  5).  Chlorine  dioxide  is  stable  in  dilute  solution  in  a  closed 
container  in  the  absence  of  light  (reference  5).  One  of  the  advantages  of  using  chlorine  dioxide 
over  chlorine  for  disinfection  is  the  decreased  formation  of  organic  disinfection  byproducts 
(DBPs),  such  as  trihalomethanes  (reference  3).  However,  chlorine  dioxide  is  an  oxidant  and 
reactions  with  organic  matter  form  inorganic  DBPs  including  primarily  chlorite  ion  (CIO2’)  and 
to  a  lesser  extent  chlorate  ion  (CIO3').  Chloride  (CT)  is  also  formed  to  a  lesser  extent.  The 
reaction  of  chlorine  dioxide  in  water  at  pH  6-8  containing  organic  matter  is  suggested  to  be 
(reference  6): 


C102  +  e'  -»•  C102' 

CIO2"  +  H+  <-»  HClOo  (chlorous  acid) 

4HC102  -*■  2C102  +  H+  +  CT  +  HCIO3  +  H20 

Chlorine  dioxide  reacts  rapidly.  In  drinking  water,  where  typical  dosages  are  0.07  -  2.0  mg/L, 
chlorite  is  the  predominant  reaction  product  with  approximately  50-70%  of  chlorine  dioxide 
converted  to  chlorite,  and  30%  converted  to  chlorate  and  chloride  (reference  3).  Manufacturer 
recommended  dosages  for  IWPD  use  may  be  similar  to  those  used  in  water  systems  or  may  be 
much  higher.  Chlorine  dioxide  IWPD  manufacturers  recommend  dosages  from  0.7-4  mg/L  for 
most  waters  and  up  to  7.5  mg/L  when  treating  cold  and/or  cloudy  waters  (references  7  and  8). 

Generation 

Chlorine  Dioxide  Generation  for  Water  Systems 

Chlorine  dioxide  can’t  be  stored  commercially  or  compressed  since  it  is  explosive  under 
pressure.  Therefore,  it  must  be  generated  on-site  (reference  5).  Although  there  are  emerging 
technologies  for  chlorine  dioxide  generation,  the  two  most  common  methods  are  (references  2 
and  5): 


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(1)  sodium  chlorite  -  acid  generation 
5NaC102  +  4HC1  <-►  4C102  +  5NaCl  +2H20 
(2)  sodium  chlorite  -  chlorine  generation 
NaC102  +  Cl2  2C102  +  2NaCl 
Chlorine  Dioxide  Generation  for  IWPDs 

Chlorine  dioxide  must  also  be  generated  on-site  on  a  much  smaller  scale  or  provided  in  dilute 
chlorine  dioxide  solutions  for  IWPD  use.  Currently,  generating  chlorine  dioxide  on-site  for  use 
as  an  IWPD  uses  buffered  sodium  chlorite,  generally  referred  to  as  “stabilized  chlorine  dioxide” 
(references  9  and  10).  The  sodium  chlorite  must  be  “activated”  by  adding  an  acid,  usually 
phosphoric  or  citric  acid,  resulting  in  the  formation  of  chlorine  dioxide  in  a  reaction  similar  to 
the  sodium  chlorite  -  acid  generation  reaction  used  by  water  systems  (shown  earlier).  There  are 
health  concerns  associated  with  the  use  of  “stabilized  chlorine  dioxide.”  “Stabilized  chlorine 
dioxide”  can  potentially  result  in  little  formation  of  chlorine  dioxide,  thereby  reducing 
disinfection  capability,  and  can  also  potentially  result  in  high  concentrations  of  chlorite,  which 
may  cause  adverse  health  effects  when  ingested  and  also  has  no  disinfection  capability 
(references  3  and  1 1).  Dilute  solutions  of  chlorine  dioxide  are  also  used  as  IWPDs.  These 
solutions  lose  chlorine  dioxide  over  time,  but  can  be  stable  for  several  months  and  possibly 
longer.  One  study  showed  dilute  chlorine  dioxide  concentrations  (approximately  35  mg/L) 
exhibited  variable  losses  based  on  the  type  of  container  used  for  storage  (reference  12).  For 
example,  a  35  mg/L  chlorine  dioxide  solution  stored  in  a  high-density  Polyethylene 
Terephthalate  (PETE)  container  for  45  days  resulted  in  a  3%  loss  of  chlorine  dioxide  (34  mg/L). 
In  contrast,  the  same  study  stored  chlorine  dioxide  in  a  clear  glass  container  for  3 1  days  which 
resulted  in  a  12%  gain  of  chlorine  dioxide  (39  mg/L)  possibly  due  to  continuing  formation  of 
chlorine  dioxide  from  chlorite.  Another  study  showed  a  6.2%  overall  gain  in  chlorine  dioxide 
concentration  after  252  days  of  storage  in  a  PETE  container  (reference  12). 

DISINFECTION  CAPABILITIES 

General 

Chlorine  dioxide  is  an  effective  disinfectant  against  bacteria,  viruses,  and  many  cysts  including 
the  capability  to  disinfect  Cryptosporidium  with  realistic  (typical  to  slightly  higher  water  system) 
dosages  (reference  3).  A  comparison  of  CTs  required  for  a  2-log  inactivation  for  E.  Coli 
bacteria,  Poliovirus  1,  and  Giardia  cysts  showed  Giardia  cysts  were  2-5  times  more  resistant 
than  Poliovirus  1  and  16-22  times  more  resistant  than  E.  Coli  bacteria  (reference  13).  The  CT  is 
the  product  of  disinfectant  concentration  (C  in  mg/L)  and  contact  time  (T  in  min).  The  CT 


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product  is  a  useful  way  for  comparing  alternative  disinfectants  and  the  resistance  of  various 
pathogens  (reference  28).  Poliovirus  was  4-11  times  more  resistant  than 

E.  Coli  bacteria  (reference  13).  Cryptosporidium  oocysts  are  the  most  resistant,  being  8-16  times 
more  resistant  than  Giardia  cysts  (reference  5).  Chlorine  dioxide’s  general  disinfection 
capability  with  respect  to  microorganisms  can  be  illustrated  in  the  following  way  from  most 
effective  to  least  effective: 

bacteria  >  viruses  >  Giardia  cysts  >  Cryptosporidium  oocysts 

Chlorine  dioxide  is  similar  to  other  chemical  disinfectants  in  that  its  disinfection  capability 
decreases  with  decreasing  temperature,  its  disinfection  capability  generally  decreases  with 
increasing  turbidity,  and  its  disinfection  capability  is  affected  by  pH  (references  3,  4  and  13). 
Since  chlorine  dioxide  exists  as  an  undissociated  gas  in  water,  volatilization  and  loss  of  chlorine 
dioxide  and  subsequent  disinfecting  capability  is  a  concern  (reference  3).  Because  chlorine 
dioxide  is  an  oxidant  it  will  react  with  organic  matter  in  the  water  forming  primarily  chlorite  and 
to  a  lesser  extent  chlorate  and  chloride.  Both  chlorite  and  chlorate  show  no  disinfection 
capabilities  and  may  cause  adverse  health  effects  in  children,  infants,  and  fetuses  (reference  11). 
Drinking  water  systems  using  chlorine  dioxide  for  disinfection  are  not  generally  able  to  provide 
adequate  disinfection  per  regulations  in  raw  water  with  high  organic  carbon  (i.e.,  organic  matter) 
when  adding  chlorine  dioxide  in  the  raw  water.  This  is  because  the  chlorine  dioxide  is  used  up 
by  reacting  with  organic  matter,  being  reduced  to  primarily  chlorite  and  leaving  no  chlorine 
dioxide  residual  (reference  3).  This  can  be  a  concern  for  IWPDs  when  treating  raw,  unfiltered 
water  supplies.  Higher  dosages  may  be  necessary  to  react  with  organic  matter  and  provide 
disinfection. 

Environmental  Effects  on  Disinfection  Capability 

Effect  of  pH  on  Disinfection  Capability 

Compared  to  chlorine,  chlorine  dioxide  is  a  more  effective  disinfectant  across  a  broader  pH 
range  (roughly  between  5  and  10)  than  free  chlorine  (reference  3).  Several  studies  have  shown 
the  effect  of  pH  on  chlorine  dioxide  disinfection  capability,  with  most  results  indicating 
disinfection  capability  generally  increases  with  increasing  pH  (reference  14).  Numerous  studies 
with  viruses  (e.g.,  poliovirus,  hepatitis  A  virus)  showed  CTs  required  for  a  2-log  virus 
inactivation  were  13-20  times  higher  at  a  pH  of  approximately  6  compared  to  a  pH  of  9  and  10 
(references  13  and  15).  Another  study  showed  CTs  up  to  90-100  times  higher  were  required  for 
a  4-log  virus  inactivation  at  a  pH  of  6  compared  to  a  pH  of  10  (reference  16).  Although  these 
studies  showed  much  higher  CTs  necessary  at  lower  pHs,  CTs  were  still  low  at  the  lower  pHs 
(ranging  from  approximately  3-13  mg-min/L).  This  indicates  chlorine  dioxide  is  a  highly 
effective  disinfectant  over  a  broad  pH  range.  In  contrast  to  the  previous  studies,  a  study  on 
chlorine  dioxide  disinfection  capability  against  Cryptosporidium  oocysts  indicated  pH  does  not 
appear  to  have  a  significant  effect  on  Cryptosporidium  inactivation  (reference  17).  The  degree 


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of  pH  effect  may  be  dependent  on  the  targeted  organism  and  in  general  chlorine  dioxide  shows 
an  increase  in  disinfection  capability  with  increasing  pH.  Chlorine  dioxide  would  likely  be 
effective  over  the  pH  range  (pH  6-9)  for  natural,  untreated  water  sources  likely  to  be  encountered 
when  using  IWPDs. 

Effect  of  Temperature  on  Disinfection  Capability 

Like  most  chemical  disinfectants,  chlorine  dioxide  disinfection  capability  decreases  with 
decreasing  temperatures  (reference  5).  Cold  water  temperatures  slow  disinfection  and  must  be 
compensated  for  by  longer  contact  times  or  higher  dosages  to  achieve  comparable  disinfection  at 
warmer  water  temperatures  (reference  18).  A  two  to  three-fold  increase  in  inactivation  rates  per 
10°  C  water  temperature  increase  seems  a  generally  accepted  rule  (reference  18).  When 
considering  chlorine  dioxide,  the  U.S.  environmental  Protection  Agency  (EPA)  developed  CT 
tables  for  the  Surface  Water  Treatment  Rule  (SWTR)  by  assuming  a  twofold  decrease  in  CT  for 
every  10°  increase  (reference  19).  Research  shows  a  2-log  inactivation  of  E.  Coli  required  four 
times  higher  CT  at  5°  C  compared  to  20°  C  (reference  13).  A  study  using  Naegleria  cysts 
showed  at  5°  C  a  CT  twice  as  high  than  at  20°  C  was  required  to  provide  a  2-log  inactivation 
(reference  5).  Using  a  two-fold  CT  increase  for  every  10°  decrease  in  water  temperature  is  a 
good  estimate  to  use  when  determining  CT  requirements  for  chlorine  dioxide  disinfection 
capability. 

Effect  of  Turbidity  on  Disinfection  Capability 

Turbidity  also  has  an  effect  on  chlorine  dioxide  disinfection  capability.  Turbidity  in  the  form  of 
particulate  matter,  aggregated  or  clumped  microorganisms,  and  dissolved  organic  matter  can 
reduce  the  effectiveness  of  chlorine  dioxide.  One  study  determined  that  bentonite  clay  added  to 
produce  turbidity  levels  up  to  2.3  nephelometric  turbidity  units  (NTUs)  had  no  adverse  effect  on 
chlorine  dioxide  disinfection  of  poliovirus.  However,  at  turbidity  levels  of  3.2  and  14.1  NTU, 
poliovirus  inactivation  was  noticeably  decreased  (references  13  and  20).  The  study  suggested 
that  bentonite  appeared  to  offer  protection  or  shield  the  viruses  from  chlorine  dioxide 
disinfection.  Another  study  using  bentonite  reduced  chlorine  dioxide  disinfection  capability 
against  Naegleria  cysts  by  11%  at  turbidities  less  than  or  equal  to  5  NTU  and  25%  at  turbidities 
between  5  and  17  NTUs  (reference  5).  Clumped  or  aggregated  microorganisms  are  also  shown 
to  be  more  resistant  to  chlorine  dioxide  disinfection  (reference  5).  In  the  presence  of  organic 
matter  chlorine  dioxide  rapidly  oxidizes  the  organic  matter  and  is  converted  to  primarily  chlorite, 
and  to  a  lesser  extent  chlorate  and  chloride  ion  (reference  3).  This  results  in  loss  of  chlorine 
dioxide  residual  and  an  increase  in  chlorite  ion  leading  to  reduced  disinfection  capability. 
Turbidity  does  have  an  effect  on  chlorine  dioxide  disinfection  capability.  Chlorine  dioxide 
disinfection  capability  decreases  in  more  turbid  waters  since  microorganisms  are  protected  by 
solid  particles  in  water,  protected  by  aggregation  or  clumping,  and  protected  by  loss  of  chlorine 


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dioxide  residual  from  oxidation  of  organic  matter.  Higher  chlorine  dioxide  dosages  may  be 
necessary  when  using  IWPDs  to  overcome  organic  matter  oxidation  and  still  provide  disinfection 
when  treating  raw,  unfdtered  water  supplies. 

Bactericidal  Capability 

Chlorine  dioxide  is  an  effective  bactericide.  Research  on  chlorine  dioxide  bactericidal  capability 
shows  bacteria  are  less  resistant  than  viruses  and  cysts  (reference  13).  Studies  using  E.  Coli 
showed  2-log  inactivation  occurred  very  quickly  in  demand-free  waters  (i.e.,  no  organic  matter 
present)  with  CT’s  all  less  than  1.0  mg-min/L,  ranging  from  0.25  -  0.48  mg-min/L,  at  the 
coldest  water  temperatures  (5°  C)  and  lowest  pH  levels  (6.5  -  7.0)  (i.e.,  worst  case  conditions, 
references  13,  21).  Another  study  estimated  CTs  of  1  or  less  at  5°  C  necessary  for  a  4-log 
E.  Coli  inactivation  (reference  22).  Chlorine  dioxide  should  easily  achieve  a  6-log  bacteria 
inactivation  at  low  temperatures  and  low  pHs  if  chlorine  dioxide  is  used  for  disinfection  of  more 
resistant  viruses  and  cysts.  Highly  turbid  water  may  require  higher  CT  (i.e.,  longer  contact  time 
and/or  higher  dose). 

Virucidal  Capability 

Chlorine  dioxide  is  an  effective  virucide.  Research  shows  viruses  are  more  resistant  than 
bacteria  but  less  resistant  than  cysts  (reference  13).  Similar  to  bactericidal  capability,  viruses  are 
rapidly  inactivated  (reference  13).  Experiments  conducted  under  worst  case  conditions  (5°  C 
water  temperature  in  the  6-7  pH  range)  resulted  in  CT’s  of  5.5  mg-min/L  for  a  2-log  Poliovirus 
1  inactivation  and  12.6  mg-min/L  for  a  4-log  Hepatitis  A  virus  inactivation  (references  13  and 
16).  The  SWTR  provides  the  following  CT  values  for  4-log  virus  inactivation  at  various  water 
temperatures  with  pH  6-9  (reference  19): 


Table  1.  EPA  Surface  Water  Treatment  Rule  (SWTR)  Required  CT  Values 

for  4-Log  Inactivation  of  Viruses 
by  Chlorine  Dioxide  for  pH  6-9 

Temperature  (deg  C) 

<=1 _ 5 _ 10 _ 15 _ 20 _ 25 

50.1  33.4  25.1  16.7  12.5  8.4 


The  data  used  to  develop  Table  1  were  based  on  experiments  conducted  in  low  turbidity  waters 
under  otherwise  worst  case  conditions,  5°  C  water  temperature  and  pH  6.  These  CT  values  are 
based  on  low  turbidity  waters  since  it  is  assumed  water  systems  provide  disinfection  after 
filtration,  as  the  last  treatment  step  prior  to  distribution.  Higher  turbidity  waters  may  require 


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higher  CT  to  achieve  the  same  log  inactivation.  Separate  CT  values  for  different  pHs  were  not 
developed  since  chlorine  dioxide  is  generally  a  more  effective  disinfectant  at  higher  pHs. 
Therefore,  these  CT  values  are  more  conservative  at  the  higher  pHs  (reference  19).  A  safety 
factor  of  2  was  applied  to  the  data  to  determine  CT  values  in  Table  1  (reference  19).  The  CT 
values  at  temperatures  other  than  5°  C  in  the  Table  were  detennined  by  using  a  two-fold  increase 
in  CT  for  every  10°  C  decrease  (reference  19).  Even  at  cold  water  temperatures,  low  pHs,  and 
low  turbidity  waters,  CTs  appear  realistic  and  achievable.  Based  on  a  typical  chlorine  dioxide 
dosage  of  2.0  mg/L  for  a  water  system,  contact  times  of  4-25  minutes  are  necessary  to  achieve 
CT  values  in  Table  1.  A  chlorine  dioxide  dose  of  0.8  mg/L  [EPA’s  Maximum  Residual 
Disinfectant  Level  (MRDL)  for  chlorine  dioxide]  results  in  contact  times  of  1 1-63  minutes  which 
are  still  reasonable  for  IWPD  use.  Highly  turbid  water  may  require  higher  CT  (i.e.,  longer 
contact  time  and/or  higher  dose). 

Cysticidal  Capability 

Giardia  Cysts 

Chlorine  dioxide  is  effective  against  Giardia  cysts.  One  study  showed  CTs  ranging  from 
1.7-17.6  mg-min/L  necessary  for  2-log  Giardia  muris  cyst  inactivation  (reference  23).  The 
SWTR  provides  the  following  CT  values  for  3-log  inactivation  of  Giardia  cysts  at  various  water 
temperatures  with  pH  6-9  (reference  19): 


Table  2.  EPA  SWTR  Required  CT  Values  for  3-Log  Inactivation  of  Giardia  Cysts 

by  Chlorine  Dioxide  for  pH  6-9 

Temperature  (deg  C) 

<=1 _ 5 _ 10 _ 15 _ 20 _ 25 

63  26  23  19  15  11 


Data  used  to  develop  Table  2  were  based  on  experiments  conducted  in  low  turbidity  waters  at 
pH  7  and  water  temperatures  ranging  from  1  -  25°  C  for  2-log  Giardia  cyst  inactivation 
(reference  19).  Determining  3-log  inactivation  at  all  temperatures  listed  in  Table  2  required 
extrapolation  using  first  order  kinetics  and  applying  a  safety  factor  of  1.5  (reference  19).  Based 
on  Table  2  it  appears  chlorine  dioxide  is  effective  against  Giardia  cysts  at  realistic  and 
achievable  CT  values.  Based  on  a  typical  chlorine  dioxide  dosage  of  2.0  mg/L  for  a  water 
system,  contact  times  of  6  -  32  minutes,  depending  on  temperature,  are  necessary  to  achieve  the 
CT  values  in  Table  2.  These  contact  times  are  also  reasonable  for  IWPDs.  A  chlorine  dioxide 


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dose  of  0.8  mg/L  (EPA’s  MRDL  for  chlorine  dioxide)  results  in  contact  times  of  14  -  79  minutes 
which  are  still  reasonable  for  IWPD  use.  Highly  turbid  water  may  require  higher  CT  (i.e.,  longer 
contact  time  and/or  higher  dose). 

Cryptosporidium  Oocysts 

Chlorine  dioxide  appears  effective  against  Cryptosporidium  oocysts  at  CT  values  achievable  by 
water  systems.  Studies  show  3-log  Cryptosporidium  inactivation  varied  from  a  CT  of  70  mg- 
min/L  to  400  mg-min/L  under  various  water  quality  conditions  (reference  5).  Cryptosporidium 
is  more  resistant  than  Giardia  cysts;  up  to  8-16  times  more  resistant  (reference  5).  Similar  to 
bacteria,  viruses,  and  other  cysts,  chlorine  dioxide,  in  general,  is  more  effective  against 
Cryptosporidium  oocysts  at  higher  pHs  and  higher  temperatures  (reference  5).  However,  there  is 
data  suggesting  pH  has  a  negligible  effect  on  inactivation  of  Cryptosporidium  (reference  17). 
Pursuant  to  the  Long  Term  2  Enhanced  Surface  Water  Treatment  Rule  (LT2ESWTR),  the  EPA 
proposed  chlorine  dioxide  CT  tables  for  various  log  inactivations  of  Cryptosporidium  (reference 
24)  based  on  studies  conducted  using  low  turbidity  waters.  The  proposed  CT  values  for  3-log 
Cryptosporidium  inactivation  are  shown  in  Table  3.  These  doses  are  conservative  and  were 
developed  using  a  safety  margin  to  account  for  variability  and  uncertainty  in  the  experimental 
data  (reference  24). 


Table  3.  EPA  Proposed  CT  Values  for  3-Log  Inactivation  of  Cryptosporidium  Oocysts 

by  Chlorine  Dioxide  for  pH  6-9 

Temperature  (deg  C) 

1 _ 5 _ H) _ 15 _ 20 _ 25 

1830  1286  830  536  347  226 


Based  on  a  typical  chlorine  dioxide  dosage  of  2.0  mg/L  for  a  water  system,  contact  times  of 
115-915  minutes  (2-15  hours),  depending  on  temperature,  are  necessary  to  achieve  the  CT 
values  in  Table  3.  For  water  systems,  these  CT  values  are  realistic  and  achievable  at  warmer 
water  temperatures.  Higher  than  typical  chlorine  dioxide  dosages  would  be  necessary  for  a  water 
system  to  achieve  the  proposed  CTs  in  colder  waters  (i.e.,  less  than  10°  C).  Based  on  this  Table, 
use  of  an  IWPD  would  be  practical  in  only  wanner  waters  (i.e.,  above  10°  C).  Highly  turbid 
water  may  require  even  higher  CT  values  (i.e.,  longer  contact  time  and/or  higher  dose).  Chlorine 
dioxide  is  effective  against  Cryptosporidium  oocysts  in  wanner,  low  turbidity  waters. 


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CHLORINE  DIOXIDE  TOXICITY 

Health  Effects  of  Chlorine  Dioxide  and  Chlorite 

Chlorine  dioxide  and  its  byproducts,  chlorite  and  chlorate  ion  can  result  in  adverse  health  effects 
when  consumed  at  large  enough  quantities.  The  EPA  regulates  chlorine  dioxide  and  chlorite  ion 
in  drinking  water  for  systems  using  chlorine  dioxide  for  disinfection.  The  EPA  established  a 
MRDL  of  0.8  mg/L  for  chlorine  dioxide  and  a  maximum  contaminant  level  (MCL)  of  1.0  mg/L 
for  chlorite  (reference  25).  The  most  common  adverse  health  effects  of  chlorine  dioxide  and 
chlorite  ion  are  oxidizing  effects  seen  in  the  blood,  either  as  methemoglobinemia  or  hemolytic 
anemia  (reference  3).  Children,  infants,  and  fetuses,  a  more  susceptible  subpopulation  may 
experience  adverse  neurotoxic  effects  (reference  26).  When  a  regulated  water  system  using 
chlorine  dioxide  is  out  of  compliance  with  the  chlorine  dioxide  MRDL  or  chlorite  MCL,  the  EPA 
considers  this  to  have  a  significant  potential  to  have  serious  adverse  health  effects  as  a  result  of 
short-term  exposure  (reference  27).  However,  the  short-term  adverse  health  effects  are  limited  to 
children,  infants,  and  fetuses.  It  is  these  groups  that  may  be  susceptible  to  adverse  nervous 
system  effects  from  short-term  exposure  (reference  27).  Health  effect  data  for  healthy  adults 
appear  to  indicate  that  short-term  exposure  does  not  result  in  adverse  health  effects.  Several 
clinical  studies  assessing  the  acute  and  subchronic  effects  of  chlorine  dioxide,  chlorite,  and 
chlorate  have  been  conducted  (reference  3).  Healthy  adults  consuming  2.5  mg  daily  of  either 
chlorine  dioxide,  chlorite,  or  chlorate  for  12  weeks  showed  no  clinically  significant  adverse 
health  effects  (reference  3).  Another  study  had  healthy  adults  consuming  0.1  to  24  mg/L 
concentrations  of  either  chlorine  dioxide,  chlorite,  or  chlorate  daily  for  3  weeks,  again  resulting 
in  no  clinically  significant  adverse  health  effects.  Based  on  this  information,  it  is  not  likely  that 
healthy  adults  consuming  water  containing  chlorine  dioxide  concentrations  recommended  by 
IWPD  manufacturers  (0.7  -  7.5  mg/L)  for  a  short  duration  (e.g.  ,<3  weeks)  would  experience 
any  adverse  health  effects  from  ingestion  of  chlorine  dioxide,  chlorite,  or  chlorate.  However, 
adverse  health  effects  could  occur  if  higher  chlorine  dioxide  dosages  are  used  for  treating  highly 
turbid  and/or  colder  water  to  kill  Cryptosporidium.  To  avoid  potential  adverse  health  effects, 
longer  contact  times  should  be  used  in  place  of  higher  chlorine  dioxide  dosages,  provided 
sufficient  chlorine  dioxide  remains  after  oxidizing  organic  matter. 

Health  Concerns  of  Stabilized  Chlorine  Dioxide 

The  use  of  “stabilized  chlorine  dioxide”  products  for  IWPD  use  may  expose  the  user  to 
significant  chlorite  concentrations.  The  “activation”  of  stabilized  chlorine  dioxide  (i.e.,  sodium 
chlorite)  with  an  acid  can  result  in  high  levels  of  chlorite  remaining  after  activation  and  relatively 
low  chlorine  dioxide  concentrations  compared  to  typical  chlorine  dioxide  generating  systems 
(reference  3).  Use  of  these  products  may  result  in  the  direct  application  of  several  hundred  mg/L 
of  chlorite  to  the  water,  much  higher  than  typical  drinking  water  chlorite  levels  (reference  3). 


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CONCLUSIONS 

Chlorine  dioxide  as  an  IWPD  can  be  effective  against  bacteria,  viruses,  Giardia  cysts,  and  to  a 
limited  extent,  Cryptosporidium  oocysts.  Very  high  CT  values  are  estimated  for  a  3-log 
Cryptosporidium  inactivation  in  colder  waters,  requiring  very  high  chlorine  dioxide  dosages 
and/or  very  long  contact  times.  Colder  temperatures,  lower  pHs,  and  higher  turbidity  all  tend  to 
have  an  adverse  effect  on  disinfection  capability.  Health  concerns  of  ingesting  chlorine  dioxide 
and  chlorite  ion  are  likely  minimal  for  healthy  adults  over  a  short-term  duration  (e.g.  ,<3  weeks) 
for  IWPD  manufacturer-recommended  chlorine  dioxide  dosages  of  0.7  -  7.5  mg/L.  However, 
adverse  health  effects  could  occur  if  higher  chlorine  dioxide  dosages  are  used  for  treating  highly 
turbid  and/or  colder  water  to  kill  Cryptosporidium.  To  avoid  potential  adverse  health  effects, 
longer  contact  times  should  be  used  in  place  of  higher  chlorine  dioxide  dosages,  provided 
sufficient  chlorine  dioxide  remains  after  oxidizing  organic  matter.  IWPDs  using  “stabilized 
chlorine  dioxide”  may  result  in  exposure  to  high  levels  of  chlorite.  Table  4  provides  a  summary 
of  chlorine  dioxide’s  disinfection  capabilities. 


Table  4.  Chlorine  Dioxide  Disinfection  Capabilities 


Parameter 

Chlorine  Dioxide  Disinfection 

General  Disinfection 
Capability 

Cysts  most  resistant.  Achieving  cyst  inactivation  will 
ensure  adequate  bacteria  and  virus  inactivation. 

Disinfection  capability  generally  follows: 

Bacteria  >  viruses  >  Giardia  >  Cryptosporidium 

Bacteria 

Effective  at  reasonable  CT  values  for  IWPD  use 

Viruses 

Effective  at  reasonable  CT  values  for  IWPD  use.  Use  EPA 
SWTR  CT  table  for  recommended  CT  values  (Table  1). 

Giardia  Cysts 

Effective  at  reasonable  CT  values  for  IWPD  use.  Use  EPA 
SWTR  CT  table  for  recommended  CT  values  (Table  2). 

Cryptosporidium  Oocysts 

Effective  at  high  CT  values.  Use  Table  3  as  guide  for  CT 
values.  If  possible,  use  longer  contact  times  instead  of 
higher  dosages  to  achieve  adequate  CT  values. 

Effect  of  Temperature 

Colder  water  temperatures  require  higher  CT  values.  Use  a 
two-fold  increase  in  CT  for  every  10°  C  decrease.  Use 
longer  contact  time  instead  of  higher  dosages  to  achieve 
higher  CT  values. 

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Effect  of  pH 

Effective  over  typical  pH  levels  for  raw,  untreated  natural 
waters.  Disinfection  capability  generally  increases  with 
increasing  pH. 

Effect  of  Turbidity 

Higher  turbidity  generally  reduces  disinfection  capability. 
Use  longer  contact  time  instead  of  higher  dosages  in  more 
turbid  waters  to  achieve  CT  values.  Higher  dosages  may  be 
necessary  to  ensure  chlorine  dioxide  remains  after  oxidation 
of  organic  matter. 

Health  Effects 

Chlorine  dioxide  and  chlorite  are  potential  health  concerns. 
IWPD  manufacturer-recommended  dosages  are  not  likely 
to  cause  adverse  health  effects  for  healthy  adults.  Exposure 
to  much  higher  chlorite  concentrations  may  occur  when 
using  stabilized  chlorine  dioxide  products. 

PREPARED  BY:  Steven  H.  Clarke,  Environmental  Engineer 
DATED:  March  2006 


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APPENDIX  A 
REFERENCES 


1.  U.S.  Environmental  Protection  Agency  (EPA),  Registration  Division  Office  of  Pesticide 
Program,  Criteria  and  Standards  Division  Office  of  Drinking  Water,  1987.  Guide  Standard  and 
Protocol  for  Testing  Microbiological  Water  Purifiers.  Washington,  D.C. 

2.  Aieta,  E.M.,  &  Berg,  J.D.,  1986.  A  Review  of  Chlorine  Dioxide  in  Drinking  Water 
Treatment.  Journal  of  the  American  Water  Works  Association  (AWWA),  78(6),  62-72. 

3.  Gates,  D.,  1998.  The  Chlorine  Dioxide  Handbook  Water  Disinfection  Series.  AWWA, 
Denver,  CO. 

4.  EPA  Office  of  Research  and  Development,  2001.  Controlling  Disinfection  By-Products  and 
Microbial  Contaminants  in  Drinking  Water.  (EPA/600/R-01/1 10).  Washington,  D.C. 

5.  EPA  Office  of  Water,  1999.  Alternative  Disinfectants  and  Oxidants  Guidance  Manual. 

(EPA  815-R-99-014).  Washington,  D.C. 

6.  Myhrstad,  J.A.  &  Samdal,  J.E.,  1969.  Behavior  and  Determination  of  Chlorine  Dioxide. 
Journal  of  the  AWWA,  61(4),  205-208. 

7.  Disinfection  Technology,  Inc.  Directions  for  Use.  XINIX  AquaCare  Water  Disinfectant. 

La  Jolla,  CA. 

8.  Katadyn  Products,  Inc.  Directions  for  Use.  Micropur  MP  1  Emergency  Drinking  Water 
Tablets.  Minneapolis,  MN. 

9.  Olsen,  N.,  et.  al.  The  Use  of  Chlorine  Dioxide  in  Potato  Storage.  (Bulletin  825).  University 
of  Idaho,  College  of  Agriculture. 

10.  Technical  Advisory  Committee  on  Safe  Drinking  Water,  2004.  Environmental  Public 
Health  Field  Manual  for  Private,  Public  and  Communal  Drinking  Water  Systems  in  Alberta, 

2nd  ed.  Canada  Institute  of  Public  Health  Inspectors  (Alberta  Branch). 

11.  Noss,  C.I.,  &  Olivieri,  V.P.,  1985.  Disinfecting  Capabilities  of  Oxychlorine  Compounds. 
Applied  and  Environmental  Microbiology,  50(5),  1 162-1164. 

12.  Richter,  J.L  &  Kross,  R.,  2005.  P46  Stable  Storage  of  Chlorine  Dioxide  Mouthrinse 
Solutions.  Oral  Diseases,  Supplement  1,  11,  120-121. 


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13.  National  Academy  of  Sciences,  1980.  Drinking  Water  and  Health  Vol.  2.  National 
Academy  Press,  Washington  D.C. 

14.  EPA  Office  of  Drinking  Water,  1984.  Drinking  Water  Microbiology  NATO/CCMS 
Drinking  Water  Pilot  Project  Series  CCMS 128.  (EPA  570/9-84-006).  Washington,  D.C. 

15.  Alvarez,  M.E.,  &  O’Brien,  R.T.,  1982.  Mechanisms  of  Inactivation  of  Poliovirus  by 
Chlorine  Dioxide  and  Iodine.  Applied  and  Environmental  Microbiology,  44(5),  1064-1071. 

16.  Sobsey,  M.D.,  1989.  Inactivation  of  Cell- Associated  and  Dispersed  Hepatitis  A  Virus  by 
Free  and  Combined  Chlorine  and  Chlorine  Dioxide.  Water  Quality  Technology  Conference 
Proceedings,  AWWA. 

17.  Clark,  R.M.,  Sivaganesan,  M.,  Rice,  E.W.,  &  Chen,  J.,  2003.  Development  of  a  CT 
Equation  for  the  Inactivation  of  Cryptosporidium  oocysts  with  Chlorine  Dioxide.  Water- 
Research,  37,  2773-2783. 

18.  Auerbach,  P.S.,  1995.  Wilderness  Medicine  Management  of  Wilderness  and  Environmental 
Emergencies,  3rd  ed.  Mosby-Year  Book,  Inc.,  St.  Louis,  MO. 

19.  EPA  Office  of  Drinking  Water,  Criteria  and  Standards  Division,  Science  and  Technology 
Branch,  1991.  Guidance  Manual  for  Compliance  with  the  Filtration  and  Disinfection 
Requirements  for  Public  Water  Systems  Using  Surface  Water  Sources.  Washington,  D.C. 

20.  Scarpino,  P.V.,  Cronier,  S.,  Zink,  M.L.,  &  Brigano,  F.A.O.,  1977.  Effect  of  Particulates  on 
Disinfection  of  Enteroviruses  and  Coliform  Bacteria  in  Water  by  Chlorine  Dioxide.  Water- 
Quality  Technology  Conference  Proceedings,  AWWA. 

21.  Benarde,  M.A.,  Israel,  B.M.,  Olivieri,  V.P.,  &  Granstrom,  M.L.,  1965.  Efficiency  of 
Chlorine  Dioxide  as  a  Bactericide.  Applied  Microbiology,  13(5),  776-780. 

22.  Benarde,  M.A.,  Snow,  W.B.,  Olivieri,  V.P.,  &  Davidson,  B.,  1967.  Kinetics  and 
Mechanism  of  Bacterial  Disinfection  by  Chlorine  Dioxide.  Applied  Microbiology,  15(2),  257- 
265. 

23.  National  Academy  of  Sciences,  1987.  Drinking  Water  and  Health  Disinfectants  and 
Disinfectant  By-Products  Vol.  7.  National  Academy  Press,  Washington  D.C. 

24.  Federal  Register,  2003.  National  Primary  Drinking  Water  Regulations:  Long  Term  2 
Enhanced  Surface  Water  Treatment  Rule;  Proposed  Rule.  68(154),  47640-47795. 

25.  Title  40,  Code  of  Federal  Regulations,  Part  141,  National  Primary  Drinking  Water 
Regulations,  2004. 


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26.  Federal  Register,  1997.  National  Primary  Drinking  Water  Regulations:  Disinfectants  and 
Disinfection  By-products;  Notice  of  Data  Availability;  Proposed  Rule.  62(212),  59387-59484. 

27.  EPA  Office  of  Water,  2000.  Public  Notification  Handbook.  (EPA  816-R-00-010), 
Washington,  D.C. 

28.  Crittenden,  J.C.  et.  al.,  2005.  Water  Treatment:  Principles  and  Design  Second  Edition. 
John  Wiley  &  Sons,  Inc.,  Hoboken,  NJ. 


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