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Chemicals  in  the  Indoor  Environment    

New  Threats  on  the  Horizon  

Veena  Singla,  Ph.D.  Staff  Scien2st  

Health  &  Environment  Program  

Disclosures  

•  I  have  nothing  to  disclose  

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Natural  Resources  Defense  Council  

MISSION  STATEMENT  To  safeguard  the  Earth:  its  people,  its  plants  and  animals  and  the  natural  systems  on  which  all  life  depends.    

Sustainable  communiHes  

Clean  energy  

Climate  change  

Oceans  

Water  

Endangered  wildlife  and  wild  places  

Health  &  PolluHon  

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Work  of  NRDC’s  Health  &  Environment  Program  

ACOG  Opinion:    Exposure  to  Toxic  Environmental  Agents  

“Exposure  to  environmental  chemicals  and  metals  in  air,  water,  soil,  food  and  consumer  products  is  ubiquitous.”  

“Prenatal  exposure  to  environmental  chemicals  is  linked  to  various  adverse  health  consequences,  and  pa2ent  exposure  at  any  point  in  2me  can  lead  to  harmful  reproduc2ve  health  

outcomes.”  

“Preven2on:  ACOG  and  ASRM  join  numerous  other  health  professional  organizaHons  in  calling  for  

Hmely  acHon  to  idenHfy  and  reduce  exposures  to  toxic  environmental  agents.”  

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Environmental  health  issues  I  focus  on  

Chemicals  in  consumer  products  &  building  materials  

Agricultural  pesHcide  use  

Outline  

•  Public  health:  Why  is  the  indoor  environment  important?  

•  Flame  retardant  chemicals  •  Consumer  product  chemicals  in  U.S.  indoor  dust  

•  ImplicaHons  for  human  health  •  What  can  you  do?  

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People  in  developed  countries  spend    ~90%  of  2me  indoors  

Klepeis 2001

Indoor  environments  are  unique  microenvironments  

Radon  Mold  Pest  allergens  Structural  &  indoor  pes2cides  Lead  

Formaldehyde  Benzene  Flame  retardants  Phthalates  

Weschler & Nazaroff, 2008; Weschler 2009; Bradman 2012; Bolden 2015

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Chemicals  from  products  affect    indoor  environmental  quality  

•  Furniture  •  Electronics  •  Wire  &  Cable  •  Flooring  •  Wall  

Coverings  •  Paint  •  Personal  care  

products  •  Beauty  

Products  •  Adhesives  •  Stain  &  water  

resistance  

•  Formaldehyde  •  Benzene  •  Toluene  

•  Flame  retardants  

•  Phthalates  •  Fluorinated  

chemicals  •  Phenolic  

chemicals  •  Fragrance  

Weschler 2009; Rudel 2009; Bolden 2015

VOCs  

SVOCs  

Exposure  in  the  indoor  environment:    Product  à  Emission  à  Exposure  

Weschler & Nazaroff, 2008; Weschler 2012; Rudel 2003

InhalaHon  Air-­‐to-­‐skin  

A  I  R  

D  U  S  T  

InhalaHon  IngesHon  (hand  to  mouth)  Dust-­‐to-­‐skin  

Direct  product  contact  

VOCs  

SVOCs  

SVOCs  

SVOCs  

SVOCs  

SVOCs  

SVOCs  

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Chemicals  from  products:  exposure  and  health  impacts  

~2,000  chemicals  Strongest  predictor  of  detecHon  in  human  biomonitoring:  Indoor/  consumer  product  use  

Wambaugh 2013; Gore 2015, Rudel 2009; Robinson 2015

What  are  flame  retardant  chemicals?  

•  Chemicals  added  to  products  to  meet  flammability  standards  

•  Goal  is  to  prevent,  slow  fires  •  Used  in  products  since  the  1970’s  •  Many  associated  with  health,  environmental  impacts  

•  EffecHveness  quesHonable    

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Flame  retardants  used  to  meet  Technical  BulleHn  117  (TB117)  standard  

1975  California  standard  for  furniture,  juvenile  products  

Test  of  filling  inside  products  

Flame  retardants  added  to  pass  the  test  

TB117  label  on  products  

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PBDE  flame  retardants  used  in  wide  variety  of  products  since  1970’s  

PolyBrominated  Diphenyl  Ethers  

Foam  inside  furniture,  baby  products  

Electronics  cases   TexHles  

PBDE  flame  retardant  levels  rising  in  people  

Sjodin 2004; EPA PBDE Biomonitoring Report 2012

with an additional 8 mL hexane. The sampleextracts were then evaporated to 0.5 mL andquantitatively transferred to GC vials that hadbeen fortified with recovery standards. Thesamples were finally evaporated to approxi-mately 10 µL in the GC vials using the vacuumevaporator.

Final analytical measurements of targetanalytes were performed using GC-IDHRMS,as described above and by Sjödin et al.(2003b, in press). All concentration datareported are background corrected for averageamount of analyte detected in blank samples(n = 3 per 24 unknowns). The limit of detec-tion when contaminants were detectable inblank samples was defined as three times thestandard deviation of the blank samples. Asignal-to-noise (S:N) ratio of 10 was used todefine the instrumental limit of detectionwhen no contaminants were detectable in theblank samples.

Calculation of population half-lives. Theobserved decay half-lives for CB-153 andBB-153 were estimated for the population byusing a single compartment model with first-order kinetics (Yang and Andersen 1994).The relationship between chemical concentra-tion (C) and time (t) of sampling with first-order kinetics is expressed in Equation 1,where kel represents the decay rate or theelimination rate constant:

Ct = C0e-kelt [1]

The terminal log-linear phase of eliminationin this model was used to determine the half-life (t1/2) using Equation 2. The eliminationrate constant (kel) is defined by Equation 3,where C and t represent the chemical concen-tration and the time at which the specimenwas collected, respectively.

[2]

[3]

ResultsWe determined six PBDEs (tetraBDE tohexaBDE), BB-153, and CB-153 in humanserum pools collected during 1985–2002. Themedian and range of concentrations in thesepools with respect to the BFRs and CB-153are shown in Table 1, stratified according to5-year collection periods. Time of sample col-lection is plotted against concentration datafor BDE-47, the sum of PBDEs (ΣPBDEs),BB-153, and CB-153 in Figure 1.

Correlation coefficients for the individualtarget analytes and the ΣPBDEs versus thetime of sample collection are shown inTable 2.

The concentrations determined for allPBDEs with the exception of BDE-85increased significantly during the study period,with BDE-47 being the dominating congener.The median level of BDE-47 increased from5.4 ng/g lipid in 1985–1989 to 34 ng/glipid for 2000–2002 (Table 1). In contrast,decreasing levels were observed for BB-153and CB-153 throughout the study period.

The summary parameters for the linearregression analysis of the logarithmic chemicalconcentration versus time for CB-153 andBB-153 in 40 samples are presented in Table 3.For CB-153, the observed decay rate wasdetermined to be 0.065/year, and the observeddecay half-life was 11 years. For BB-153, theobserved decay rate was 0.058/year, and thedecay half-life was 12 years.

DiscussionConcentrations of PBDEs are well known tohave been increasing in Europe from studiesconducted in Sweden (Meironyté et al. 1999;Meironyté Guvenius 2002), Norway (Thomsenet al. 2002), and Germany (Schröter-Kermaniet al. 2000). More recently, similar findingshave been reported for Japan (Akutsu et al.2003). However, during recent years a decreasein concentration has been indicated in Sweden,probably because of a decrease in use of thelower brominated PBDEs in Europe, as shownby recent use figures [Bromine Science andEnvironmental Forum (BSEF) 2003].Estimated use of the pentaBDE mixture inEurope was 150 metric tons/year in 2001. Useof the same product in North America wasestimated at 7,100 metric tons in 2001, corre-sponding to 95% of the total world demandfor this product (BSEF 2003).

Information about current and historicconcentrations of PBDEs in humans is lackingor limited for North America. However, arecent review in which previously publishedconcentration data on PBDEs were used toconstruct a time trend, we (Sjödin et al.2003a) reported increasing levels of PBDEs inNorth America. The average concentration ofBDE-47 in earlier studies was 0.63 ng/g lipid(range, < 0.4–24; n = 12) in serum in 1988(Illinois; Sjödin et al. 2002); 33 ng/g lipid inbreast adipose tissue (range, 7–200; n = 23) inthe late 1990s (California Bay, California; Sheet al. 2002); 83 ng/g lipid (n = 19) in a milkpool in 1997 (New York; Betts 2002);130 ng/g lipid in a milk pool in 2000 (Austin,

k = C – Ct tel

ln ln–

1 2

1 2

( )( )

tk1 2

0 693/

.=

el

Article | Sjödin et al.

656 VOLUME 112 | NUMBER 6 | May 2004 • Environmental Health Perspectives

Figure 1. Linear regression trends for concentrations (ng/g lipid) of (A) BDE-47, (B) the ΣPBDEs,(C) CB-153, and (D) BB-153 in serum pools plotted against the year of sample collection.

A120

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Table 2. Spearman’s rank order correlation coeffi-cients and p-levels for the correlation of the meas-ured organohalogen compounds in the UnitedStates versus collection year (1985–2002).

Compound R p-Value

PBDEs2,2´,4,4´-TetraBDE (BDE-47) 0.61 < 0.01*2,2´,3,4,4´-PentaBDE (BDE-85) 0.22 0.182,2´,4,4´,5-PentaBDE (BDE-99) 0.59 < 0.01*2,2´,4,4,6-PentaBDE (BDE-100) 0.57 < 0.01*2,2´,4,4´,5,5´-HexaBDE (BDE-153) 0.61 < 0.01*2,2´,4,4´,5,6-HexaBDE (BDE-154) 0.34 < 0.05ΣPBDEs 0.55 < 0.01*PCBs

2,2´,4,4´,5,5´-HexaCB (CB-153) –0.70 < 0.01*PBBs

2,2´,4,4´,5,5´-HexaBB (BB-153) –0.51 < 0.01*

*Statistically significant at p < 0.05.

Table 3. Regression of the logarithm of CB-153 andBB-153 on time in 40 samples.

Coefficient SE p-Value

CB-153Intercept 58 8.2 < 0.001Time –0.028 0.0041 < 0.001

BB-153Intercept 51 13 < 0.001Time –0.025 0.0068 < 0.001

2004  97%  of  samples  contained  PBDEs  

PBDEs  in  blood,  breast  milk,  fat  Hssue  

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Flame  retardants  conHnuously  migrate  out  of  products  

Weschler & Nazaroff 2008

①   Not  chemically  bonded  to  plasHc  materials  

②  Chemicals  off-­‐gas  Alach  to  parHcles  in  air  

③  Contaminated  parHcles  selle  in  house  dust  

Flame  retardants  enter  people’s  bodies  in  contaminated  air  and  dust  

Frederiksen 2009

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California  has  highest  levels  of  flame  retardants  in  dust  

0  

0.5  

1  

1.5  

2  

2.5  

3  

3.5  

4    ug  BD

E-­‐99/  g

 dust  

Zota 2008 LA!I+1*7*1#+"(+?)1"/&%(")+53"1.%*(+)%*+*1*7)'*.+P"'3+3"43*#'+1*7*1#+"(+%)5")1T*'3("5+2"(&%"'"*#+

+"#,*,$*()F*KSJS*8265'"21,2$()*@&5,2&,*[*Q,&-2")"0?M*@$(3),$"2*,$*()F*KSST*8265'"21,2$()*@&5,2&,*[*Q,&-2")"0?M*X42%,'*,$*()F*KSJS*8265'"21,2$()*@&5,2&,*[*Q,&-2")"0?M*_52%-(1*,$*()F**KSJS*8265'"21,2$()*+,#,('&-*b,1(5)*&"11425&($5"2c*

0

20

40

60

80

100

120

140

160

180

200

U.S. California

Adults Children (aged 2-5)

Med

ian

PBD

E co

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trat

ion

in s

erum

(ng/

g lip

id)

Occupational exposures (foam workers)

0

20

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60

80

100

120

Whites Asians Hispanic Blacks

Med

ian

PBD

E co

ncen

trat

ion

in s

erum

(ng/

g lip

id)

California girls aged 6-8 years

Program on Reproductive Health and the Environment

Children  are  vulnerable  to  chemical  exposures  from  dust  

Adults

Children (aged 2-5)

Courtesy, Ami Zota Lunder 2010; Rose 2010; Stapleton 2008, Windham 2010 U.S. California

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DispariHes  by  race  and  socio-­‐economic  status  (SES)  

•  Highest  PBDE  levels  found  in:  – Dust  in  low  SES  homes  – Non-­‐white  children  – Low  SES  children  

•  May  be  associated  with:  – Older  furniture/  electronics  – Building  characterisHcs  – More  Hme  spent  indoors  

Quiros-Alcala 2011; Windham 2010; Zota 2010; Bradman 2012

Adverse  health  effects  of  PBDEs:  animal  studies  

•  Endocrine  disrupHon:  thyroid  hormones  •  Affect  brain  development  •  Affect  reproducHve  development  and  ferHlity  •  Affect  immune  funcHon  •  Cancer  

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Epidemiological  studies:  human  health  associaHons  

Main 2007; Akutsu 2008; Meeker 2009; Eskenazi et al, 2010, 2011, 2012

Higher PBDE levels associated with

lower birth weight impaired attention

poorer coordination lowered IQ

longer time to get pregnant altered thyroid hormones

hormone changes decreased sperm quality, testis size

PBDEs  are  the  “new  lead”  

Courtesy, Ami Zota

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Good  news:  PBDE  bans/phase  out  à    declining  levels  in  dust  and  people  

PBDEs  in  pregnant  women  San  Francisco  

Dodson  2012;  Zota  2013    

pentaBDE  (BDE  47)  2006   2011  

BDE  47  con

centraHo

n  in  dust  (ng/g)  

PBDEs  in  repeat  CA  house  dust  samples  

Bad  news:  many  “regrelable  subsHtuHon”  replacement  flame  retardants  

Dodson  2012  

House  du

st  con

centraHo

n  (ng/g)  

BDE  47  2006   2011  

“Firemaster  550”  (EH-­‐TBB)  2006   2011  

Also  found:  TDCIPP  TCEP  TCIPP  TPHP  HBCD  DBDE  BTBDE  -­‐  -­‐  -­‐  

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Dust:  a  window  into  SVOC  chemicals  from  products  and  potenHal  human  exposures  

SVOC  in  air  

Par2cles  

Modified from Weschler & Nazaroff, 2008

Consumer  product  chemicals  in  indoor  dust:  a  quan2ta2ve  meta-­‐analysis  of  U.S.  studies  

Susanna  D.  Mitro,  Robin.  E.  Dodson,  Veena  Singla,  Gary  Adamkiewicz,  

Angelo  F.  Elmi,  Monica  Kaitz,  Ami  R.  Zota  

 Submi4ed,  2016  

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Our  approach  

SystemaHc  literature  search  and  meta-­‐analysis  

SystemaHc  literature  search:  172  chemicals  

•  Found  1,561  published  papers  and  abstracts  

•  Aser  exclusions,  34  papers  +  2  unpublished  datasets  included  

Literature  Search  

Descrip/ve  Sta/s/cs  

Meta-­‐Analysis  

Intake  Assessment  

Hazard  Iden/fica/on  

13   24   25   47   62  

RFRs

Phthalates

Phenols

Fragrance PFASs

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DescripHve  staHsHcs:  74  chemicals  

•  Chemicals  measured  in  ≥2  datasets  

•  Methods  and  descripHve  staHsHcs  

 

Literature  Search  

Descrip/ve  Sta/s/cs  

Meta-­‐Analysis  

Intake  Assessment  

Hazard  Iden/fica/on  

11   19   1   20   23  RFRs

Phthalates

Phenols

Fragrance PFASs

Meta-­‐analysis:  45  chemicals  

•  Chemicals  measured  in  ≥3  datasets  

•  Geometric  Mean  (GM)  and  Geometric  Standard  DeviaHon  (GSD)  available  

•  Calculated  pooled  GM  and  95%  Confidence  Interval    

Literature  Search  

Descrip/ve  Sta/s/cs  

Meta-­‐Analysis  

Intake  Assessment  

Hazard  Iden/fica/on  

8   11   1   15   10  RFRs

Phthalates

Phenols

Fragrance PFASs

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Samples  taken  in  14  states  

Samples  mostly  from  home  environments  

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Ten  chemicals  consistently  detected  across  all  studies  

Chemical # datasets Detected

DEHP 8 100% DEHA 4 100% HHCB 3 100% BBzP 8 98-100% TPHP 8 98-100% TDCIPP 14 95-100% DnBP 7 95-100% DiBP 7 95-100% HBCD (and isomers) 10 92-100% MeP 3 90-100%

RFRs Phthalates

Phenols Fragrance

Pooled  concentraHons  

in  dust  

RFRs Fragrance

Phthalates Phenols

PFASs

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Intake  Assessment:  44  chemicals  

•  EsHmated  total  residenHal  intake  

•  Adult  female  •  Child  (3-­‐6  years  old)  

Literature  Search  

Descrip/ve  Sta/s/cs  

Meta-­‐Analysis  

Intake  Assessment  

Hazard  Iden/fica/on  

Child:  Highest  esHmated  residenHal  intake  of  flame  retardants  and  phthalates  

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Hazard  IdenHficaHon:  35  chemicals  

•  California  Safer  Consumer  Products  Candidate  Chemical  list  

•  Hazard  traits  idenHfied  by  authoritaHve  bodies  

Literature  Search  

Descrip/ve  Sta/s/cs  

Meta-­‐Analysis  

Intake  Assessment  

Hazard  Iden/fica/on  

High  intake  chemicals  have  mul2ple  hazards  

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MulHple  chemicals  associated  with    reproduc2ve,  endocrine,  developmental  toxicity  

5   7  

10  

11  

15  

16  20  

22  

25  

Neurotoxicant  Respiratory  Toxicant  

Persistent  or  BioaccumulaHve  

Hepatotoxicant  

Immunotoxicant  

Carcinogen  Developmental  Toxicant  

Endocrine  Toxicant  

ReproducHve  Toxicant  

Some  dust  levels  exceed  EPA  screening  guidelines  

Pooled

 GM  (n

g/g),  95%

 CI  

TDCIPP

 

TCEP  

DEHP

 

BBzP  

DEHA

 

EPA  carcinogenic  soil  screening  level  

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Summary  and  future  direcHons  

•  Wide  array  of  chemicals  from  consumer  products  and  building  materials  in  indoor  environments  

•  People  likely  co-­‐exposed  to  similar  chemicals  in  indoor  environments  

•  Phthalates  and  phenols-­‐  highest  levels  in  dust  •  Phthalates  and  RFRs  -­‐highest  esHmated  intakes  •  Phthalates  and  PFASs-­‐  most  hazard  traits  •  Policy  acHons  focused  on  phthalates  

California  SB  1019  requires  labeling  for  added  flame  retardants  in  2015!  

Senator  Mark  Leno  

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RecommendaHons  for  clinicians  

“ACOG  and  ASRM  call  on  their  members  to  advocate  for  policies  to  idenHfy  and  reduce  exposure  to  environmental  toxic  agents  while  

addressing  the  consequences  of  such  exposure.”  

“Reproduc2ve  care  providers  can  be  effec2ve  in  preven2ng  prenatal  exposures  to  environmental  threats  to  health  

because  they  are  uniquely  poised  to  intervene  before  and  during  pregnancy,  which  is  a  cri2cal  window  of  human  

development.”  

General  recommendaHons  to  reduce  indoor  exposures  

Reduce  contaminated  dust  and  dust  contact  

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Resources  

Health  professionals  advocate  for  policy  to  protect  health  

Over  60  doctors,  nurses  and  scienHsts  

write  to  EPA  in  support  of  pesHcide  

restricHons  

AAP  and  NHMA  pe22on  Consumer  Product  Safety  Commission  for  flame  retardant  restric2ons  

3/10/16  

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1.  Which  of  the  following  factors  have  a  significant  effect  on  flame  retardant  exposures?  

A.  Age  B.  Geographic  locaHon  C.  Socio-­‐economic  status  D.  All  of  the  above  

2.  Consumer  products  commonly  contain  the  following  kinds  of  semi-­‐volaHle  organic  chemicals:  

A.  Formaldehyde,  lead,  and  benzene  B.  Phthalates,  flame  retardants  and  fluorinated  

chemicals  C.  Radon,  pesHcides  and  lead  D.   None  of  the  above  

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3.  In  which  of  the  following  would  you  expect  to  find  the  most  similar  chemical  profile?  

A.  A  home  in  New  York  city  and  a  park  in  New  York  city  

B.  A  park  in  New  York  city  and  Yosemite  NaHonal  Park  

C.  A  home  in  New  York  city  and  a  home  in  San  Francisco  

D.  These  would  all  have  vastly  different  chemical  profiles  

THANK  YOU