Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain
文献类型:期刊论文
作者 | Ye, Can; Chen, Hui; Hoffmann, Erik H.; Mettke, Peter; Tilgner, Andreas; He, Lin; Mutzel, Anke; Brueggemann, Martin; Poulain, Laurent; Schaefer, Thomas |
刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY |
出版日期 | 2021-06-15 |
卷号 | 55期号:12页码:7818-7830 |
ISSN号 | 0013-936X |
关键词 | haze air pollution H2O2 HULIS chamber TMI photochemistry sulfate CAPRAM |
英文摘要 | During haze periods in the North China Plain, extremely high NO concentrations have been observed, commonly exceeding 1 ppbv, preventing the classical gas-phase H2O2 formation through HO2 recombination. Surprisingly, H2O2 mixing ratios of about 1 ppbv were observed repeatedly in winter 2017. Combined field observations and chamber experiments reveal a photochemical in-particle formation of H2O2, driven by transition metal ions (TMIs) and humic-like substances (HULIS). In chamber experiments, steady-state H2O2 mixing ratios of 116 +/- 83 pptv were observed upon the irradiation of TMI- and HULIS-containing particles. Correspondingly, H2O2 formation rates of about 0.2 ppbv h(-1) during the initial irradiation periods are consistent with the H2O2 rates observed in the field. A novel chemical mechanism was developed explaining the in-particle H2O2 formation through a sequence of elementary photochemical reactions involving HULIS and TMIs. Dedicated box model studies of measurement periods with relative humidity >50% and PM2.5 >= 75 mu g m(-3) agree with the observed H2O2 concentrations and time courses. The modeling results suggest about 90% of the particulate sulfate to be produced from the SO2 reaction with OH and HSO3- oxidation by H2O2. Overall, under high pollution, the H2O2-caused sulfate formation rate is above 250 ng m(-3) h(-1), contributing to the sulfate formation by more than 70%. |
WOS研究方向 | Engineering, Environmental ; Environmental Sciences |
源URL | [http://ir.rcees.ac.cn/handle/311016/45623] |
专题 | 生态环境研究中心_大气污染控制中心 |
作者单位 | 1.Leibniz Inst Tropospher Res TROPOS, Atmospher Chem Dept ACD, D-04318 Leipzig, Germany 2.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China 3.Leibniz Inst Tropospher Res TROPOS, Modeling Atmospher Proc Dept, D-04318 Leipzig, Germa 4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 5.Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Inst Atmospher Sci, Shanghai 200438, People 6.Eurofins Inst Dr Appelt Leipzig GmbH, D-04317 Leipzig, Germany |
推荐引用方式 GB/T 7714 | Ye, Can,Chen, Hui,Hoffmann, Erik H.,et al. Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2021,55(12):7818-7830. |
APA | Ye, Can.,Chen, Hui.,Hoffmann, Erik H..,Mettke, Peter.,Tilgner, Andreas.,...&Herrmann, Hartmut.(2021).Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain.ENVIRONMENTAL SCIENCE & TECHNOLOGY,55(12),7818-7830. |
MLA | Ye, Can,et al."Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain".ENVIRONMENTAL SCIENCE & TECHNOLOGY 55.12(2021):7818-7830. |
入库方式: OAI收割
来源:生态环境研究中心
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