从白令海到北太平洋西部夏季大气中二次有机气溶胶的时空分布及影响因素
Spatiotemporal distribution and influencing factors of secondary organic aerosols in the summer atmosphere from the Bering Sea to the western North Pacific.
作者信息
Hu Chengge, Yue Fange, Zhan Haicong, Leung Kenneth M Y, Liu Hongwei, Gu Weihua, Zhang Runqi, Chen Afeng, Wang Xinming, Xie Zhouqing
机构信息
Anhui Key Laboratory of Polar Environment and Global Change, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China; Suzhou Institute for Advanced Study, University of Science and Technology of China, Suzhou, China.
Anhui Key Laboratory of Polar Environment and Global Change, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
出版信息
Sci Total Environ. 2023 Feb 10;859(Pt 1):160138. doi: 10.1016/j.scitotenv.2022.160138. Epub 2022 Nov 12.
To better understand the formation process of biogenic and anthropogenic secondary organic aerosols (BSOA and ASOA) in the marine atmosphere under the background of global warming, aerosol samples were collected over three summers (i.e., 2014, 2016 and 2018) from the Bering Sea (BS) to the western North Pacific (WNP). The results showed that temporally, atmospheric concentrations of isoprene-derived SOA (SOA) tracers were the lowest in 2014 regardless of the marine region, while atmospheric concentrations of monoterpenes-derived SOA (SOA) tracers in this year were the highest and the aerosols were more aged than those in the other two years. In comparison, the concentrations of β-caryophyllene-derived and toluene-derived SOA (SOA and SOA) tracers were relatively low overall. Spatially, the concentrations of SOA tracers were significantly higher over the WNP than over the BS, with SOA tracers over the BS mainly coming from marine sources, while the WNP was strongly influenced by terrestrial inputs. In particular, for land-influenced samples from the WNP, NO-channel products of SOA were more dependent on O and SO relative to HO-channel product, and the high atmospheric oxidation capacity and SO could promote the formation of later-generation SOA products. The extent of terrestrial influence was further quantified using a principal component analysis (PCA)-generalized additive model (GAM), which showed that terrestrial emissions explained more than half of the BSOA tracers' concentrations and contributed almost all of the ASOA tracer. In addition, the assessment of secondary organic carbon (SOC) highlighted the key role of anthropogenic activities in organic carbon levels in offshore areas. Our study revealed significant contributions of terrestrial natural and anthropogenic sources to different SOA over the WNP, and these relevant findings help improve knowledge about SOA in the marine atmosphere.
为了更好地理解全球变暖背景下海洋大气中生物源和人为源二次有机气溶胶（BSOA和ASOA）的形成过程，在三个夏季（即2014年、2016年和2018年）从白令海（BS）到北太平洋西部（WNP）采集了气溶胶样本。结果表明，在时间上，无论海洋区域如何，异戊二烯衍生的SOA（SOA）示踪剂的大气浓度在2014年最低，而该年份单萜衍生的SOA（SOA）示踪剂的大气浓度最高，且气溶胶比其他两年的气溶胶老化程度更高。相比之下，β-石竹烯衍生和甲苯衍生的SOA（SOA和SOA）示踪剂的浓度总体上相对较低。在空间上，WNP上的SOA示踪剂浓度明显高于BS上的，BS上的SOA示踪剂主要来自海洋源，而WNP则受到陆地输入的强烈影响。特别是，对于来自WNP的受陆地影响的样本，SOA的NO通道产物相对于HO通道产物更依赖于O和SO，高大气氧化能力和SO可以促进后期SOA产物的形成。使用主成分分析（PCA）-广义相加模型（GAM）进一步量化了陆地影响的程度，结果表明陆地排放解释了超过一半的BSOA示踪剂浓度，并且几乎贡献了所有的ASOA示踪剂。此外，对二次有机碳（SOC）的评估突出了人为活动在近海地区有机碳水平中的关键作用。我们的研究揭示了陆地自然源和人为源对WNP上不同SOA的重大贡献，这些相关发现有助于增进对海洋大气中SOA的了解。
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