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Pollution Characteristics and Health Risk Assessment of Summertime Atmospheric Volatile Halogenated Hydrocarbons in a Typical Urban Area of Beijing, China

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Pollution Characteristics and Health Risk Assessment of Summertime Atmospheric Volatile Halogenated Hydrocarbons in a Typical Urban Area of Beijing, China atmosphere Article Pollution Characteristics and Health Risk Assessment of Summertime Atmospheric Volatile Halogenated Hydrocarbons in a Typical Urban Area of Beijing, China 1,2, 1,3, 1, 1 4 1,5 Yuanyuan Ji y, Linghong Xu y, Hong Li *, Chuhan Wang , Dongyao Xu , Lei Li , Hao Zhang 1, Jingchun Duan 1, Yujie Zhang 1, Xuezhong Wang 1, Weiqi Zhang 1 , Fang Bi 1, Yizhen Chen 1, Yanting Yu 6 and Lingshuo Meng 1 1 State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China; [email protected] (Y.J.); [email protected] (L.X.); [email protected] (C.W.); [email protected] (L.L.); [email protected] (H.Z.); [email protected] (J.D.); [email protected] (Y.Z.); [email protected] (X.W.); [email protected] (W.Z.); [email protected] (F.B.); [email protected] (Y.C.); [email protected] (L.M.) 2 College of Earth Sciences, Jilin University, Changchun 130061, China 3 Daishan Environmental Protection Bureau, Zhoushan 316200, China 4 School of Chemical & Environmental Engineering, China University of Mining and Technology, Beijing 100083, China; [email protected] 5 Academy of Environmental Planning and Design, Co., Ltd., Nanjing University, Nanjing 210093, China 6 Puyang Research Institute of Environmental Sciences, Puyang 457000, China; [email protected] * Correspondence: [email protected] These authors contributed equally to this work. y Received: 16 August 2020; Accepted: 16 September 2020; Published: 23 September 2020 Abstract: Twenty-three atmospheric volatile halogenated hydrocarbons (VHHs) were detected in a typical urban area of Beijing, China from 24 August to 4 September, 2012. The mean and range in daily mass concentrations of the 23 VHHs were 30.53 and 13.45–76.33 µg/m3, respectively. Seven of those VHHs were controlled ozone-depleting substances in China, with a mean of 12.95 µg/m3, accounting for 42.43% of the total. Compared with other national and international cities, the concentrations of the selected 11 VHHs in this study were relatively higher. Dichloroethane had the highest mass concentration, followed by difluorochloromethane. Maxima of total VHHs occurred within the period 8:30–9:00 a.m., while minima occurred during 1:30–2:00 p.m. Source apportionment suggested that the main sources of VHHs in the study area were solvents usage and industrial processes, leakage of chlorofluorocarbons banks, refrigerants, and fumigant usage. Among the selected 7 VHHs, trichloromethane, tetrachloromethane, 1,2-dichloroethane, and 1,4-dichlorobenzene posed potential carcinogenic risks to exposed populations, while none of the selected 11 VHHs posed appreciable non-carcinogenic risks to exposed populations. The carcinogenic risks from atmospheric VHHs in Beijing are higher than in other Chinese cities, indicating that it is necessary to implement immediate control measures for atmospheric VHHs in Beijing. Keywords: ambient air; volatile halogenated hydrocarbons; pollution status; sources; health risk assessment; Beijing Atmosphere 2020, 11, 1021; doi:10.3390/atmos11101021 www.mdpi.com/journal/atmosphere Atmosphere 2020, 11, 1021 2 of 19 1. Introduction Volatile halogenated hydrocarbons (VHHs) in the atmosphere include ozone-depleting substances (ODS) such as chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs) as well as toxic and harmful VHHs (THVHHs; e.g., chlorobenzene, chloroform, and chloroethylene). ODS could deplete the stratospheric ozone layer, enhancing the greenhouse effect [1], while THVHHs are generally irritating and corrosive, causing damage to human skin, liver, heart, kidney, pancreas, and the central nervous system [2–4]. Some THVHHs are recognized as carcinogenic, teratogenic, and mutagenic compounds [4–6]. Compared with other atmospheric pollutants, little research has been carried out on the characterization or the health risk assessment of VHHs in China [7–19]. Previous studies have shown that in some Chinese cities, especially Hong Kong and Guangzhou, the concentrations of VHHs in ambient air are higher than those in other international cities [9,11]. In particular, some species of VHHs identified in urban monitoring sites in Chinese cities pose a carcinogenic risk to exposed populations [12]. Given that the environmental management strategy in China is transitioning from “Passive Response” to “Active Prevention and Control”, control measures for VHHs should now be emphasized to improve air quality. Beijing, the center of politics, culture, and economics, is featured with a dense population, huge vehicle amounts, many industry factories, and complicated air pollutants emissions. Recently, increasing occurrences of the haze with a wide area range and long duration in Beijing have attracted great attention from the central government, municipal government, and general public. In order to formulate accurate prevention and control measures for protecting the stratospheric ozone layer and human health, it is necessary to study the characteristics and health risks of VHHs. In this paper, ambient VHHs samples were collected in an urban area of Beijing from 24 August to 4 September 2012. Ambient concentrations, temporal variations, and sources of VHHs were analyzed and health risks of selected THVHHs were assessed. These data support further recognition of the health risks of VHHs and implementation of effective control measures for VHH pollution in Beijing in the near future. 2. Materials and Methods 2.1. Sample Collecting Air samples were collected on the roof of the Supersite for Urban Air Comprehensive Observation and Research at the Chinese Research Academy of Environmental Sciences in the northeastern urban area of Beijing (40◦020 N, 116◦250 E) (Figure1). This site is located 15 m above the ground, about 2 km north of the North Fifth Ring Road, 3.6 km from the Olympic park, 200 m east of Subway Line 5 and Beiyuan Road, and 100 m north of Chunhua Road. The site is in a residential and commercial area, and there are no obvious local air pollution sources nearby. The population density surrounding the sampling site is 8038 people per square kilometer [20]. Thus, our air pollution monitoring results can reflect the ambient air quality of the resident urban population in this area. Therefore, these monitoring data can be used to investigate pollution levels and to determine health risks of VHHs in the ambient air for this typical urban area of Beijing. Atmosphere 2020, 11, 1021 3 of 19 Atmosphere 2020, 11, x FOR PEER REVIEW 3 of 19 Figure 1. Location of sampling site and surroundings [[21].21]. Samples were were collected collected from from 24 Au 24gust August to 4 September to 4 September 2012 over 2012 four over 30-min four periods: 30-min 8:30–9:00 periods: 8:30–9:00a.m., 1:30–2:00 a.m., 1:30–2:00p.m., 6:00–6:30 p.m., 6:00–6:30 p.m., and p.m., 10:00–10:30 and 10:00–10:30 p.m. However, p.m. However, sampling sampling was postponed was postponed from fromnoon noonon 1 onSeptember 1 September to the to themorning morning of 2 of September 2 September because because of of rain. rain. In In total, total, 43 43 air air samples samples were collected in SUMMA canisters (Entech Instruments, Inc., Simi Valley, CA,CA, USA);USA); thirtythirty canisterscanisters had volumes ofof 3.23.2 L,L, whilewhile thethe others others had had volumes volumes of of 3.0 3.0 L. L. The The recommended recommended TO-15 TO-15 sampling sampling method method of theof the US US Environmental Environmental Protection Protection Agency Agency (US (US EPA) EPA) was was used used as ouras our sampling sampling method method [22 ].[22]. Before sampling, all canisters were cleaned using a canister cleaner (3100A, Entech Instruments, Inc., SimiSimi Valley,Valley, CA,CA, USA) California, and vacuumed USA) and to vacuumed 50 mtorr. to The 50 sampling mtorr. The speed sampling was controlled speed was by acontrolled flow-limiting by a valve. flow-limiting The canisters valve. were The placed canisters 1.5 mwere above placed the rooftop. 1.5 m Meteorologicalabove the rooftop. data atMeteorological the sampling data site, at including the sampling wind site, direction, including wind wind speed, direction, temperature, wind speed, dew point temperature, temperature, dew solarpoint radiation,temperature, ultraviolet solar radiation, radiation, ultraviolet and visibility, radiation, were monitored and visibility, hourly were using monitored an automatic hourly weather using stationan automatic (Vaisala weather Inc., Helsinki, station (Vaisala Finland) Inc., from Helsinki, 28 August Finland) to 4 September from 28 August 2012. to 4 September, 2012. 2.2. Sample Analysis All air samplessamples werewere analyzedanalyzed usingusing cryogeniccryogenic coldcold traptrap preconcentrationpreconcentration followed by gas chromatography (GC) coupled with mass spectrometryspectrometry (MS) and flameflame ionization detection (FID) withinwithin 1515 days.days. Each volatile organic compound (VOC) sample was enriched and concentrated by passing it through the Entech 7100A pre-concentratio pre-concentrationn system system (Entech (Entech Instruments, Instruments, Inc., Inc., Simi Simi Valley, Valley, CA, USA), whereby waterwater andand COCO22 were also removed from the sample. VOCs were rapidly gasifiedgasified and fed intointo thethe GC-MSGC-MS/FID/FID systemsystem (GC,(GC, HP-7890A, HP-7890A, Agilent Agilent Technology, Technology, Inc., Inc., Santa California, Clara, California,USA; MS, USA;HP-5975C, MS, HP-5975C,Agilent Technology, Agilent Technology, Inc., California, Inc., SantaUSA) Clara,to be separated California, and USA) quantitatively to be separated analyzed and quantitatively[23]. Ninety-seven analyzed VOCs, [23 ].including Ninety-seven 25 VHHs, VOCs, were including separated 25 VHHs, by the were DB-624 separated chromatographic by the DB-624 chromatographic column (60 m 0.25 mm 1.8 µm; J&W Scientific, Folsom, CA, USA) and the PLOT column (60 m × 0.25 mm × 1.8 µm;× J&W Scientific,× Folsom, CA, USA) and the PLOT chromatographic chromatographic column (30 m 0.25 mm 3.0 µm; J&W Scientific, Folsom, CA, USA).
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