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, Can5,6; Chen, Hui7; Hoffmann, Erik H.8; Mettke, Peter8; Tilgner, Andreas8; He, Lin8; Mutzel, Anke8,9; Brueggemann, Martin8; Poulain, Laurent8; Schaefer, Thomas8 |
| 刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
 |
| 出版日期 | 2021-06-15 |
| 卷号 | 55 |
| ISSN号 | 0013-936X |
| 关键词 | haze air pollution H2O2 HULIS chamber TMI photochemistry sulfate CAPRAM |
| DOI | 10.1021/acs.est.1c00561 |
| 通讯作者 | Mu, Yujing(yjmu@rcees.ac.cn) ; Chen, Jianmin(jmchen@fudan.edu.cn) ; Herrmann, Hartmut(herrmann@tropos.de) |
| 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关键词 | TIANJIN-HEBEI REGION ; HYDROGEN-PEROXIDE ; PHOTOCHEMICAL FORMATION ; AUTHENTIC CLOUD ; ATMOSPHERIC PEROXIDES ; AEROSOL FORMATION ; POLLUTION LEVELS ; SULFUR-DIOXIDE ; NITROUS-ACID ; HAZE EVENTS |
| 资助项目 | Ministry of Science and Technology of China[2016YFC0202700] ; National Natural Science Foundation of China[91544211] ; National Natural Science Foundation of China[91843301] ; National Natural Science Foundation of China[91743202] ; National Natural Science Foundation of China[41722501] ; National Natural Science Foundation of China[91544212] ; National Natural Science Foundation of China[21976106] ; National Research Program for Key Issues in Air Pollution Control[DQGG0102] ; National Research Program for Key Issues in Air Pollution Control[DQGG0103] ; Marie Sklodowska-Curie Actions[690958-MARSU-RISE-2015] ; EFRE[3000582010] ; European Union's Horizon 2020 research and innovation programme through the EUROCHAMP-2020 Infrastructure Activity[730997] ; Deutsche Bundesstiftung Umwelt (DBU)[20016/424] |
| WOS研究方向 | Engineering ; Environmental Sciences & Ecology |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000663939900007 |
| 资助机构 | Ministry of Science and Technology of China ; National Natural Science Foundation of China ; National Research Program for Key Issues in Air Pollution Control ; Marie Sklodowska-Curie Actions ; EFRE ; European Union's Horizon 2020 research and innovation programme through the EUROCHAMP-2020 Infrastructure Activity ; Deutsche Bundesstiftung Umwelt (DBU) |
| 源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/123613]  |
| 专题 | 中国科学院合肥物质科学研究院 |
| 通讯作者 | Mu, Yujing; Chen, Jianmin; Herrmann, Hartmut |
| 作者单位 | 1.Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China 2.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, Key Lab Environm Opt & Technol, Hefei 230031, Peoples R China 3.Univ Sci & Technol China, Sch Earth & Space Sci, Hefei 230026, Peoples R China 4.Shandong Univ, Sch Environm Sci & Engn, Qingdao 266237, Peoples R China 5.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China 6.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 7.Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Inst Atmospher Sci, Shanghai 200438, Peoples R China 8.Leibniz Inst Tropospher Res TROPOS, Atmospher Chem Dept ACD, D-04318 Leipzig, Germany 9.Eurofins Inst Dr Appelt Leipzig GmbH, D-04317 Leipzig, Germany 10.Leibniz Inst Tropospher Res TROPOS, Modeling Atmospher Proc Dept, D-04318 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. |
| 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. |
| 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(2021). |
入库方式： OAI收割
来源：合肥物质科学研究院
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。