Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain
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. Combine...
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| Veröffentlicht in: | Environmental science & technology 2021-06, Vol.55 (12), p.7818-7830 |
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| creator | Ye, Can Chen, Hui Hoffmann, Erik H Mettke, Peter Tilgner, Andreas He, Lin Mutzel, Anke Brüggemann, Martin Poulain, Laurent Schaefer, Thomas Heinold, Bernd Ma, Zhuobiao Liu, Pengfei Xue, Chaoyang Zhao, Xiaoxi Zhang, Chenglong Zhang, Fei Sun, Hao Li, Qing Wang, Lin Yang, Xin Wang, Jinhe Liu, Cheng Xing, Chengzhi Mu, Yujing Chen, Jianmin Herrmann, Hartmut |
| description | 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 μg 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%. |
| doi_str_mv | 10.1021/acs.est.1c00561 |
| format | Article |
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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 μg 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%.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.1c00561</identifier><language>eng</language><publisher>Easton: American Chemical Society</publisher><subject>Anthropogenic Impacts on the Atmosphere ; Chambers ; Haze ; Hydrogen peroxide ; Irradiation ; Metal ions ; Mixing ratio ; Oxidation ; Particulate matter ; Photochemical reactions ; Photochemicals ; Radiation ; Recombination ; Relative humidity ; Sulfates ; Sulfur dioxide ; Transition metals ; Winter</subject><ispartof>Environmental science & technology, 2021-06, Vol.55 (12), p.7818-7830</ispartof><rights>2021 American Chemical Society</rights><rights>Copyright American Chemical Society Jun 15, 2021</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-4905-3432 ; 0000-0003-0587-1748 ; 0000-0003-2106-9691 ; 0000-0001-7044-2101 ; 0000-0001-5859-3070 ; 0000-0003-4350-0892 ; 0000-0002-7048-2856 ; 0000-0001-6673-7716 ; 0000-0002-3759-9219 ; 0000-0003-4021-4874 ; 0000-0002-9173-1188</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.1c00561$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.1c00561$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,27076,27924,27925,56738,56788</link.rule.ids></links><search><creatorcontrib>Ye, Can</creatorcontrib><creatorcontrib>Chen, Hui</creatorcontrib><creatorcontrib>Hoffmann, Erik H</creatorcontrib><creatorcontrib>Mettke, Peter</creatorcontrib><creatorcontrib>Tilgner, Andreas</creatorcontrib><creatorcontrib>He, Lin</creatorcontrib><creatorcontrib>Mutzel, Anke</creatorcontrib><creatorcontrib>Brüggemann, Martin</creatorcontrib><creatorcontrib>Poulain, Laurent</creatorcontrib><creatorcontrib>Schaefer, Thomas</creatorcontrib><creatorcontrib>Heinold, Bernd</creatorcontrib><creatorcontrib>Ma, Zhuobiao</creatorcontrib><creatorcontrib>Liu, Pengfei</creatorcontrib><creatorcontrib>Xue, Chaoyang</creatorcontrib><creatorcontrib>Zhao, Xiaoxi</creatorcontrib><creatorcontrib>Zhang, Chenglong</creatorcontrib><creatorcontrib>Zhang, Fei</creatorcontrib><creatorcontrib>Sun, Hao</creatorcontrib><creatorcontrib>Li, Qing</creatorcontrib><creatorcontrib>Wang, Lin</creatorcontrib><creatorcontrib>Yang, Xin</creatorcontrib><creatorcontrib>Wang, Jinhe</creatorcontrib><creatorcontrib>Liu, Cheng</creatorcontrib><creatorcontrib>Xing, Chengzhi</creatorcontrib><creatorcontrib>Mu, Yujing</creatorcontrib><creatorcontrib>Chen, Jianmin</creatorcontrib><creatorcontrib>Herrmann, Hartmut</creatorcontrib><title>Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>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 μg 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%.</description><subject>Anthropogenic Impacts on the Atmosphere</subject><subject>Chambers</subject><subject>Haze</subject><subject>Hydrogen peroxide</subject><subject>Irradiation</subject><subject>Metal ions</subject><subject>Mixing ratio</subject><subject>Oxidation</subject><subject>Particulate matter</subject><subject>Photochemical reactions</subject><subject>Photochemicals</subject><subject>Radiation</subject><subject>Recombination</subject><subject>Relative humidity</subject><subject>Sulfates</subject><subject>Sulfur dioxide</subject><subject>Transition metals</subject><subject>Winter</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNpFkE1Lw0AQhhdRsFbPXhc8SursV5oepVRbqDaQFr2FzXZiUsKuZjc_wn9t0hacywvDMx88hNwzmDDg7EkbP0EfJswAqJhdkBFTHCKVKHZJRgBMRDMRf16TG-8PAMAFJCPym-o21KbBKK20R5pWLrgWtQm1s566ki5361VGtd3T7dvK04UPumhqX1FNs9A6-0Uz17UGjyzf8CN62to1OiDNuqYcsrY0VEg_ahuwpe-uDRWdV7XVNG10bW_JVakbj3fnHJPdy2I7X0brzetq_ryOtGBJiKYmjqFUplBsKJjGrFRTLNRelhKkSRAEsiLWXDCFUmhuJAJiT8gZzkoxJg-nvd-t--l6Y_mh_9_2J3OupEiEVInsqccT1Wv9Bxjkg-t8aA6TZ9fiD8EQcs8</recordid><startdate>20210615</startdate><enddate>20210615</enddate><creator>Ye, Can</creator><creator>Chen, Hui</creator><creator>Hoffmann, Erik H</creator><creator>Mettke, Peter</creator><creator>Tilgner, Andreas</creator><creator>He, Lin</creator><creator>Mutzel, Anke</creator><creator>Brüggemann, Martin</creator><creator>Poulain, Laurent</creator><creator>Schaefer, Thomas</creator><creator>Heinold, Bernd</creator><creator>Ma, Zhuobiao</creator><creator>Liu, Pengfei</creator><creator>Xue, Chaoyang</creator><creator>Zhao, Xiaoxi</creator><creator>Zhang, Chenglong</creator><creator>Zhang, Fei</creator><creator>Sun, Hao</creator><creator>Li, Qing</creator><creator>Wang, Lin</creator><creator>Yang, Xin</creator><creator>Wang, Jinhe</creator><creator>Liu, Cheng</creator><creator>Xing, Chengzhi</creator><creator>Mu, Yujing</creator><creator>Chen, Jianmin</creator><creator>Herrmann, Hartmut</creator><general>American Chemical Society</general><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0002-4905-3432</orcidid><orcidid>https://orcid.org/0000-0003-0587-1748</orcidid><orcidid>https://orcid.org/0000-0003-2106-9691</orcidid><orcidid>https://orcid.org/0000-0001-7044-2101</orcidid><orcidid>https://orcid.org/0000-0001-5859-3070</orcidid><orcidid>https://orcid.org/0000-0003-4350-0892</orcidid><orcidid>https://orcid.org/0000-0002-7048-2856</orcidid><orcidid>https://orcid.org/0000-0001-6673-7716</orcidid><orcidid>https://orcid.org/0000-0002-3759-9219</orcidid><orcidid>https://orcid.org/0000-0003-4021-4874</orcidid><orcidid>https://orcid.org/0000-0002-9173-1188</orcidid></search><sort><creationdate>20210615</creationdate><title>Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain</title><author>Ye, Can ; Chen, Hui ; Hoffmann, Erik H ; Mettke, Peter ; Tilgner, Andreas ; He, Lin ; Mutzel, Anke ; Brüggemann, Martin ; Poulain, Laurent ; Schaefer, Thomas ; Heinold, Bernd ; Ma, Zhuobiao ; Liu, Pengfei ; Xue, Chaoyang ; Zhao, Xiaoxi ; Zhang, Chenglong ; Zhang, Fei ; Sun, Hao ; Li, Qing ; Wang, Lin ; Yang, Xin ; Wang, Jinhe ; Liu, Cheng ; Xing, Chengzhi ; Mu, Yujing ; Chen, Jianmin ; Herrmann, Hartmut</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a318t-7c660f5cb5111110761f57eb5d4f404c8e03e1b6a2315e43a2c4e0eeeb549e9f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Anthropogenic Impacts on the Atmosphere</topic><topic>Chambers</topic><topic>Haze</topic><topic>Hydrogen peroxide</topic><topic>Irradiation</topic><topic>Metal ions</topic><topic>Mixing ratio</topic><topic>Oxidation</topic><topic>Particulate matter</topic><topic>Photochemical reactions</topic><topic>Photochemicals</topic><topic>Radiation</topic><topic>Recombination</topic><topic>Relative humidity</topic><topic>Sulfates</topic><topic>Sulfur dioxide</topic><topic>Transition metals</topic><topic>Winter</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ye, Can</creatorcontrib><creatorcontrib>Chen, Hui</creatorcontrib><creatorcontrib>Hoffmann, Erik H</creatorcontrib><creatorcontrib>Mettke, Peter</creatorcontrib><creatorcontrib>Tilgner, Andreas</creatorcontrib><creatorcontrib>He, Lin</creatorcontrib><creatorcontrib>Mutzel, Anke</creatorcontrib><creatorcontrib>Brüggemann, Martin</creatorcontrib><creatorcontrib>Poulain, Laurent</creatorcontrib><creatorcontrib>Schaefer, Thomas</creatorcontrib><creatorcontrib>Heinold, Bernd</creatorcontrib><creatorcontrib>Ma, Zhuobiao</creatorcontrib><creatorcontrib>Liu, Pengfei</creatorcontrib><creatorcontrib>Xue, Chaoyang</creatorcontrib><creatorcontrib>Zhao, Xiaoxi</creatorcontrib><creatorcontrib>Zhang, Chenglong</creatorcontrib><creatorcontrib>Zhang, Fei</creatorcontrib><creatorcontrib>Sun, Hao</creatorcontrib><creatorcontrib>Li, Qing</creatorcontrib><creatorcontrib>Wang, Lin</creatorcontrib><creatorcontrib>Yang, Xin</creatorcontrib><creatorcontrib>Wang, Jinhe</creatorcontrib><creatorcontrib>Liu, Cheng</creatorcontrib><creatorcontrib>Xing, Chengzhi</creatorcontrib><creatorcontrib>Mu, Yujing</creatorcontrib><creatorcontrib>Chen, Jianmin</creatorcontrib><creatorcontrib>Herrmann, Hartmut</creatorcontrib><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ye, Can</au><au>Chen, Hui</au><au>Hoffmann, Erik H</au><au>Mettke, Peter</au><au>Tilgner, Andreas</au><au>He, Lin</au><au>Mutzel, Anke</au><au>Brüggemann, Martin</au><au>Poulain, Laurent</au><au>Schaefer, Thomas</au><au>Heinold, Bernd</au><au>Ma, Zhuobiao</au><au>Liu, Pengfei</au><au>Xue, Chaoyang</au><au>Zhao, Xiaoxi</au><au>Zhang, Chenglong</au><au>Zhang, Fei</au><au>Sun, Hao</au><au>Li, Qing</au><au>Wang, Lin</au><au>Yang, Xin</au><au>Wang, Jinhe</au><au>Liu, Cheng</au><au>Xing, Chengzhi</au><au>Mu, Yujing</au><au>Chen, Jianmin</au><au>Herrmann, Hartmut</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2021-06-15</date><risdate>2021</risdate><volume>55</volume><issue>12</issue><spage>7818</spage><epage>7830</epage><pages>7818-7830</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><abstract>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 μg 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%.</abstract><cop>Easton</cop><pub>American Chemical Society</pub><doi>10.1021/acs.est.1c00561</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0002-4905-3432</orcidid><orcidid>https://orcid.org/0000-0003-0587-1748</orcidid><orcidid>https://orcid.org/0000-0003-2106-9691</orcidid><orcidid>https://orcid.org/0000-0001-7044-2101</orcidid><orcidid>https://orcid.org/0000-0001-5859-3070</orcidid><orcidid>https://orcid.org/0000-0003-4350-0892</orcidid><orcidid>https://orcid.org/0000-0002-7048-2856</orcidid><orcidid>https://orcid.org/0000-0001-6673-7716</orcidid><orcidid>https://orcid.org/0000-0002-3759-9219</orcidid><orcidid>https://orcid.org/0000-0003-4021-4874</orcidid><orcidid>https://orcid.org/0000-0002-9173-1188</orcidid></addata></record> |
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| subjects | Anthropogenic Impacts on the Atmosphere Chambers Haze Hydrogen peroxide Irradiation Metal ions Mixing ratio Oxidation Particulate matter Photochemical reactions Photochemicals Radiation Recombination Relative humidity Sulfates Sulfur dioxide Transition metals Winter |
| title | Particle-Phase Photoreactions of HULIS and TMIs Establish a Strong Source of H2O2 and Particulate Sulfate in the Winter North China Plain |
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