中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Isotopic constraints on heterogeneous sulfate production in Beijing haze

文献类型:期刊论文

作者He, Pengzhen1; Alexander, Becky7; Geng, Lei1; Chi, Xiyuan1; Fan, Shidong1; Zhan, Haicong1; Kang, Hui1; Zheng, Guangjie2,6; Cheng, Yafang2,3; Su, Hang2,3
刊名ATMOSPHERIC CHEMISTRY AND PHYSICS
出版日期2018-04-23
卷号18期号:8页码:5515-5528
ISSN号1680-7316
DOI10.5194/acp-18-5515-2018
英文摘要

Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter) in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM2.5 sulfate (Delta O-17(SO42-)) collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Through-out the sampling campaign, the 12-hourly averaged PM2.5 concentrations ranged from 16 to 323 mu g m(-3) with a mean of (141 +/- 88 (1 sigma)) mu g m(-3), with SO42- representing 8-25% of PM2.5 mass. The observed Delta O-17(SO42-) varied from 0.1 to 1.6% with a mean of (0.9 +/- 0.3) %. Delta O-17(SO42-) increased with PM2.5 levels in October 2014 while the opposite trend was observed from November 2014 to January 2015. Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM2.5 >= 75 mu g m(-3)) of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68 %. During PDs of Cases I and III-V, heterogeneous sulfate production (Phet) was estimated to contribute 41-54% to total sulfate formation with a mean of (48 +/- 5) %. For the specific mechanisms of heterogeneous oxidation of SO2, chemical reaction kinetics calculations suggested S(IV) (= SO2 center dot H2O + HSO3- + SO32-) oxidation by H2O2 in aerosol water accounted for 5-13% of P-het. The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed Delta O-17(SO42-). Heterogeneous sulfate production via S(IV) oxidation by O-3 was estimated to contribute 21-22% of P-het on average. Heterogeneous sulfate production pathways that result in zero-Delta O-17(SO42-), such as S(IV) oxidation by NO2 in aerosol water andor by O-2 via a radical chain mechanism, contributed the remaining 66-73% of P-het. The assumption about the thermodynamic state of aerosols (stable or metastable) was found to significantly influence the calculated aerosol pH (7.6 +/- 0.1 or 4.7 +/- 1.1, respectively), and thus influence the relative importance of heterogeneous sulfate production via S(IV) oxidation by NO2 and by O-2. Our local atmospheric conditions-based calculations suggest sulfate formation via NO2 oxidation can be the dominant pathway in aerosols at high-pH conditions calculated assuming stable state while S(IV) oxidation by O-2 can be the dominant pathway providing that highly acidic aerosols (pH <= 3) exist. Our local atmospheric-conditions-based calculations illustrate the utility of Delta O-17(SO42-) for quantifying sulfate formation pathways, but this estimate may be further improved with future regional modeling work.

WOS关键词SULFUR-DIOXIDE ; ATMOSPHERIC SULFATE ; FORMATION PATHWAYS ; AEROSOL FORMATION ; MULTIPLE OXYGEN ; NORTH CHINA ; ICE CORE ; OXIDATION ; CHEMISTRY ; OZONE
资助项目National Key Project of MOST[2016YFC0203302] ; NSFC[91544013] ; NSFC[91644218] ; Key Project of CAS[KJZD-EW-TZ-G06-01] ; Atmospheric Pollution Control of the Prime Minister[DQGG0104] ; NSF AGS[1644998] ; National Key Project of MOS[2017YFC0210104]
WOS研究方向Meteorology & Atmospheric Sciences
语种英语
WOS记录号WOS:000430738100003
出版者COPERNICUS GESELLSCHAFT MBH
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/35451]  
专题合肥物质科学研究院_中科院安徽光学精密机械研究所
通讯作者Xie, Zhouqing
作者单位1.Univ Sci & Technol China, Sch Earth & Space Sci, Anhui Prov Key Lab Polar Environm & Global Change, Hefei 230026, Anhui, Peoples R China
2.Max Planck Inst Chem, Multiphase Chem Dept, D-55128 Mainz, Germany
3.Jinan Univ, Inst Environm & Climate Res, Guangzhou 511443, Guangdong, Peoples R China
4.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, Key Lab Environm Opt & Technol, Hefei 230031, Anhui, Peoples R China
5.Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Urban Atmospher Environm, Xiamen 361021, Fujian, Peoples R China
6.Brookhaven Natl Lab, Atmospher Sci Div, Upton, NY 11973 USA
7.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA
推荐引用方式
GB/T 7714
He, Pengzhen,Alexander, Becky,Geng, Lei,et al. Isotopic constraints on heterogeneous sulfate production in Beijing haze[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(8):5515-5528.
APA He, Pengzhen.,Alexander, Becky.,Geng, Lei.,Chi, Xiyuan.,Fan, Shidong.,...&Xie, Zhouqing.(2018).Isotopic constraints on heterogeneous sulfate production in Beijing haze.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(8),5515-5528.
MLA He, Pengzhen,et al."Isotopic constraints on heterogeneous sulfate production in Beijing haze".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.8(2018):5515-5528.

入库方式: OAI收割

来源:合肥物质科学研究院

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