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Photochemical Processing of Inorganic and Organic Species in the Canadian High Arctic Aerosols: Impact of Ammonium Cation, Transition Metals, and Dicarboxylic Acids before and after Polar Sunrise at Alert
ACS Earth and Space Chemistry ( IF 3.4 ) Pub Date : 2021-08-27 , DOI: 10.1021/acsearthspacechem.1c00242
Dharmendra Kumar Singh 1 , Kimitaka Kawamura 2, 3 , Pingqing Fu 4 , Hideki Kasukabe 3 , Ayako Yanase 3 , Leonard A. Barrie 5, 6, 7
Affiliation  

Temporal variations and correlation statistics of major inorganic and organic species and carbonaceous components of the total suspended particulate matter (TSPM) at Alert were concurrently studied. Organic carbon (OC) and water-soluble organic carbon (WSOC) declined from February to mid-March together with elemental carbon (EC), but OC and WSOC increased in April while EC stayed low, suggesting photochemical production of organic aerosols. WSOC/OC ratios peaked in mid-April (89%). The ammonium availability index (AAI) increases from 31% (before sunrise) to 58% (after sunrise). Strong correlations of NH4+ with WSOC and dicarboxylic acids (DCAs) were found, implying the formation of organic salts at polar sunrise. K+ is substantially correlated (R2 = 0.96; p = 0.03) with levoglucosan before sunrise; however, the correlation decreases after. Significant correlations were found for 5 cations (NH4+, Na+, K+, Mg2+, and Ca2+), 2-alkaline earth metals (Ca and Mg), and 3 transition metals (Fe, Cu, and Mn) with DCAs and WSOC during both periods. Fe and Cu are strongly correlated (up to R2 = 0.80; p < 0.05) with DCAs before and after polar sunrise, implying the Fenton reaction both in dark and light periods. On the basis of the significant correlation, we found the plausibility of Fenton chemistry of Fe and Cu with oxalic acid. In the multiple linear regression model, Mn is the most significant predictor of WSOC followed by Cu and Fe after sunrise. This study demonstrates the importance of the photochemical processing of Arctic aerosols that are carried by long-range transport to the Arctic at Alert, and bridges and answers the research gap and some questions raised in our previous study (regarding, for example, the impacts of inorganic species, primarily NH4+ and transition metals on organic aerosols).

中文翻译:

加拿大高北极气溶胶中无机和有机物种的光化学处理:铵阳离子、过渡金属和二羧酸在警报极地日出前后的影响

同时研究了警报的主要无机和有机物种以及总悬浮颗粒物 (TSPM) 的碳质成分的时间变化和相关统计数据。有机碳 (OC) 和水溶性有机碳 (WSOC) 与元素碳 (EC) 一起从 2 月到 3 月中旬下降,但 4 月份 OC 和 WSOC 增加,而 EC 保持在较低水平,表明有机气溶胶的光化学产生。WSOC/OC 比率在 4 月中旬达到峰值 (89%)。铵可用性指数 (AAI) 从 31%(日出前)增加到 58%(日出后)。NH 4 +与WSOC 和二羧酸(DCA)的强相关性被发现,这意味着在极地日出时形成了有机盐。K +显着相关(R2 = 0.96;p = 0.03) 在日出前使用左旋葡聚糖;然而,之后相关性降低。发现 5 种阳离子(NH 4 +、Na +、K +、Mg 2+和 Ca 2+)、2-碱土金属(Ca 和 Mg)和 3 种过渡金属(Fe、Cu 和 Mn)具有显着相关性) 与 DCA 和 WSOC 在这两个时期。Fe 和 Cu 有很强的相关性(高达R 2 = 0.80;p< 0.05) 极地日出前后的 DCA,这意味着在黑暗和光明时期都发生了芬顿反应。在显着相关性的基础上,我们发现了 Fe 和 Cu 与草酸的芬顿化学的合理性。在多元线性回归模型中,Mn 是 WSOC 最重要的预测因子,其次是日出后的 Cu 和 Fe。这项研究证明了在警报时通过远程传输到北极的北极气溶胶的光化学处理的重要性,并弥合和回答了研究差距和我们之前研究中提出的一些问题(例如,关于无机物质,主要是有机气溶胶上的NH 4 +和过渡金属)。
更新日期:2021-10-22
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