Organic aerosol formation and aging processes in Beijing constrained by size-resolved measurements of radiocarbon and stable isotopic C-13 | |
Ni, Haiyan1,2; Huang, Ru-Jin1,3; Yao, Peng2; Cosijn, Max M.2; Kairys, Norbertas2; Zhong, Haobin1; Dusek, Ulrike2 | |
通讯作者 | Huang, Ru-Jin(rujin.huang@ieecas.cn) ; Dusek, Ulrike(u.dusek@rug.nl) |
2022 | |
发表期刊 | ENVIRONMENT INTERNATIONAL |
ISSN | 0160-4120 |
卷号 | 158页码:10 |
摘要 | This study investigates the sources and atmospheric processes of size-resolved carbonaceous aerosols in winter 2018 in urban Beijing, based on analysis of dual-carbon isotopes (i.e., radiocarbon and the stable isotope C-13). We found a size dependence of fossil source contributions to elemental carbon (EC), but no clear size dependence for organic carbon (OC). Comparable fossil source contributions to water-insoluble OC (WIOC; 55 +/- 3%) and to water-soluble OC (WSOC; 54 +/- 4%) highlight the importance of secondary aerosol formation, considering that fossil sources emit only small amounts of primary WSOC. OC concentrations increased during high PM2.5 pollution events, with increased fossil and non-fossil WSOC concentrating at larger particles (0.44-2.5 mu m) than WIOC (0.25-2.5 mu m), highlighting the aqueous-phase chemistry as an important pathway for OC production. The ratio of C-13/C-12 (expressed as delta C-13) of total carbon (-27.0 parts per thousand to -23.3 parts per thousand) fell in the range of anthropogenic aerosol, reflecting small biogenic influence. delta C-13 of OC increased with desorption temperature steps (200 degrees C, 350 degrees C and 650 degrees C). The strongly enriched delta C-13(OC, 650) (-26.9 parts per thousand to -20.3 parts per thousand) and large mass fraction of OC650 degrees C in total desorbed OC, both increasing with the increase of particle sizes, were caused by photochemical aging, especially during low and moderate PM2.5 pollution events, when regional, aged aerosol played an important role. During low pollution events, higher delta C-13(OC, 650) and WSOC/OC ratios reflect a larger contribution and more extensive chemical processing of aged aerosol. In contrast, relatively low delta C-13(OC, 200) (-27.2 parts per thousand to -25.7 parts per thousand) suggests the influence of secondary OC formation on the more volatile OC desorbed at 200 degrees C. delta(13)C(OC, 20)0 was similar for all particle sizes and for different pollution events, pointing to an internal mixture of local and aged regional OC. Our results show that the organic aerosol in Beijing arises from a mixture of various sources and complex formation processes, spanning local to regional scales. Particle sizes < 250 nm show strong contribution from local secondary OC formation, whereas refractory OC in particles around 1 mu m shows strong evidence for regional aging processes. In summary, primary emission, secondary and aqueous-phase formation, and (photo-) chemical aging all need to be considered to understand organic aerosol in this region and their importance varies with particle size. |
关键词 | Size-resolved aerosol PM2.5 pollution Dual-carbon isotopes Source apportionment Fossil source contribution Aqueous-phase chemistry |
DOI | 10.1016/j.envint.2021.106890 |
关键词[WOS] | CARBON-ISOTOPE ; PARTICULATE MATTER ; SEVERE HAZE ; ATMOSPHERIC AEROSOLS ; SOURCE APPORTIONMENT ; ELEMENTAL CARBON ; BACKGROUND SITE ; FOSSIL SOURCES ; WINTER HAZE ; SECONDARY |
收录类别 | SCI ; SCI |
语种 | 英语 |
资助项目 | National Key Research and Development Program of China[2017YFC0212701] ; National Natural Science Foundation of China[41925015] ; Chinese Academy of Sciences[ZDBS-LY-DQC001] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDB40000000] ; KNAW[530-5CDP30] ; Cross Innovative Team fund from the State Key Laboratory of Loess and Quaternary Geology[SKLLQGTD1801] |
WOS研究方向 | Environmental Sciences & Ecology |
项目资助者 | National Key Research and Development Program of China ; National Natural Science Foundation of China ; Chinese Academy of Sciences ; Strategic Priority Research Program of Chinese Academy of Sciences ; KNAW ; Cross Innovative Team fund from the State Key Laboratory of Loess and Quaternary Geology |
WOS类目 | Environmental Sciences |
WOS记录号 | WOS:000705024800001 |
出版者 | PERGAMON-ELSEVIER SCIENCE LTD |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.ieecas.cn/handle/361006/17107 |
专题 | 粉尘与环境研究室 第四纪科学与全球变化卓越创新中心 |
通讯作者 | Huang, Ru-Jin; Dusek, Ulrike |
作者单位 | 1.Chinese Acad Sci, Ctr Excellence Quaternary Sci & Global Change, State Key Lab Loess & Quaternary Geol, Key Lab Aerosol Chem & Phys,Inst Earth Environm, Xian 710061, Peoples R China 2.Univ Groningen, Energy & Sustainabil Res Inst Groningen ESRIG, Ctr Isotope Res CIO, NL-9747 AG Groningen, Netherlands 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
推荐引用方式 GB/T 7714 | Ni, Haiyan,Huang, Ru-Jin,Yao, Peng,et al. Organic aerosol formation and aging processes in Beijing constrained by size-resolved measurements of radiocarbon and stable isotopic C-13[J]. ENVIRONMENT INTERNATIONAL,2022,158:10. |
APA | Ni, Haiyan.,Huang, Ru-Jin.,Yao, Peng.,Cosijn, Max M..,Kairys, Norbertas.,...&Dusek, Ulrike.(2022).Organic aerosol formation and aging processes in Beijing constrained by size-resolved measurements of radiocarbon and stable isotopic C-13.ENVIRONMENT INTERNATIONAL,158,10. |
MLA | Ni, Haiyan,et al."Organic aerosol formation and aging processes in Beijing constrained by size-resolved measurements of radiocarbon and stable isotopic C-13".ENVIRONMENT INTERNATIONAL 158(2022):10. |
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