Article pubs.acs.org/est
Organophosphorus Flame Retardants and Plasticizers in Building and Decoration Materials and Their Potential Burdens in Newly Decorated Houses in China Yan Wang,*,† Minmin Hou,† Qiaonan Zhang,† Xiaowei Wu,† Hongxia Zhao,† Qing Xie,† and Jingwen Chen† †
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Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China S Supporting Information *
ABSTRACT: Organophosphorus flame retardants (OPFRs) have been increasingly used in various building and decoration materials to fulfill fire safety standards since the phasing out of polybrominated diphenyl ethers. We determined OPFR concentrations in the most commonly used building and decoration materials available in local markets and online in China. The OPFR concentrations varied significantly, from 14.78 ng/g (putty powder) to 9649000 ng/g (expanded polystyrene panel (EPS)). Relatively high concentrations of OPFRs were found in foam samples, followed by nonwoven and polyvinyl chloride (PVC) wallpaper, PVC pipes, sealing materials, boards, and paints. Low concentrations were found mostly in wall decoration powders, suggesting that no OPFRs had been added to these powders. Tris(1-chloro-2-propyl) phosphate and tris(1,3-dichloro-2-propyl) phosphate were the most detected halogenated OPFRs, while tri-n-butyl phosphate and tris(2-butoxyethyl) phosphate were the dominant nonhalogenated OPFRs, implying that they are commonly used in building and decoration materials. The estimated OPFR burden in interior decoration using nonwoven wallpaper was 330- and 2110-fold higher than that using latex paint and diatomite, respectively. The emission periods of OPFRs from nonwoven and PVC wallpaper may be greater than 13 years. We estimated that the total burden of OPFRs for decoration using wallpaper in newly decorated houses in China is ∼63 t/y. Significantly higher concentrations of OPFRs in interior decoration materials, especially nonwoven wallpaper, pose potential health risks to the people using the buildings. typically spend over 20 h per day.16 Chlorinated OPFRs are suspected carcinogens, while tricresyl phosphate (TCrP) and tributyl phosphate (TnBP) have been shown to be potential thyroid hormone disruptors and can cause reproductive toxicity.17,18 Previous studies found an increase in organic flame retardant (OFR) concentrations in indoor air when OFR-containing products were installed in the room19 and demonstrated significant relationships between housing characteristics (e.g., number of consumer products and flooring materials) and PBDE and hexabromocyclododecane (HBCD) levels in indoor air,20 as well as OPFR levels in indoor dust.21 Furthermore, significant associations have been detected between OFR levels in house dust and their burdens in the human body.22,23 Building decoration materials and household products are postulated sources of OFRs in indoor air and dust.11,24 Given
1. INTRODUCTION Due to their persistence, bioaccumulation, and toxicity,1,2 penta- and octa-polybrominated diphenyl ethers (PBDEs) are listed as persistent organic pollutants (POPs) by the Stockholm Convention in 2009 and are gradually being phased out from the market.3,4 Organophosphorus flame retardants (OPFRs) have been widely used as suitable alternatives in consumer products and building materials in recent years. The total annual global consumption of OPFRs was 210000 tons in 2004,5 while the yield of OPFRs in China reached 70000 tons in 2007 and is projected to increase by 15% annually.6 OPFRs are frequently present as additives rather than chemically bonded to the final products, which allows their easy release into the environment via abrasion, volatilization, and leaching during their lifetime.6,7 Hence, OPFRs have been widely detected in various environmental matrices, including air, water, sediment, and soil,8−10 as well as air and dust in indoor environments.11,12 Furthermore, OPFRs have also been detected in human breast milk13,14 and blood.15 Human exposure to OPFRs occurs mainly via inhalation, ingestion, and dermal absorption in the indoor environment where people © 2017 American Chemical Society
Received: Revised: Accepted: Published: 10991
July 3, 2017 August 25, 2017 September 2, 2017 September 3, 2017 DOI: 10.1021/acs.est.7b03367 Environ. Sci. Technol. 2017, 51, 10991−10999
Article
Environmental Science & Technology Table 1. Concentrations of OPFRs in Wall Decoration Materials wallpaper C (ng/g) N = 23 TnBP TCEP TCPP TDCPP TBEP TPhP EHDPP TEHP TPPO TCrP total
nonwoven n=7 102400 67.42 422.1 17.14 74631 93.55 457.4 164.4 135.1 31.17 179200
± ± ± ± ± ± ± ± ± ± ±
124500 64.09 658.2 29.72 92830 112.2 907.1 231.0 306.9 46.06 113300
PVC n=3 13.80 1703 1124 102.6 10.17 171.7 118.8 9984 39.04 126.8 44460
± ± ± ± ± ± ± ± ± ± ±
2.04 2806 1831 175.8 16.92 86.86 105.4 12830 33.65 114.9 48470
powder pure paper n=2 49.58 9.50 177.9 1.64 35.75 1.99 7.61 1.68 5.41 2.53 4352
± ± ± ± ± ± ± ± ± ± ±
gypsum n=2
28.58 2.69 225.4 1.47 33.91 1.18 10.35 0.28 2.81 0.02 5307
29.78 7.79 36.60 0.30 2.79 0.37 0.93 0.51 0.95 0.51 80.52
± ± ± ± ± ± ± ± ± ± ±
8.79 0.31 3.10 0.001 2.58 0.13 0.02 0.15 0.36 0.01 3.11
paint
putty
diatomite
n=2
n=1
± ± ± ± ± ± ± ± ± ± ±
2.17 1.05 5.18 2.42 0.74 0.33 0.94 0.69 1.12 0.69 15.34
3.07 1.41 5.84 1.86 0.74 0.45 0.93 0.88 0.55 0.61 16.34
0.01 0.02 0.56 2.09 0.30 0.17 0.08 0.18 0.13 0.05 2.20
latex paint n=6 117.4 13.28 31.92 156.7 18.91 11.73 27.26 17.15 21.37 12.35 428.1
± ± ± ± ± ± ± ± ± ± ±
105.1 7.84 7.83 81.37 12.00 10.37 28.09 9.31 11.54 17.85 64.54
sealing materials were first evenly coated on a precleaned glass pane (baked at 450 °C for 4 h), dried in a vacuum desiccator, and then broken into small pieces (
