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东亚沙尘期间大气中盐水矿物颗粒表面上硝酸铵的高效非均相生成。

Efficient Heterogeneous Formation of Ammonium Nitrate on the Saline Mineral Particle Surface in the Atmosphere of East Asia during Dust Storm Periods.

机构信息

Key Lab of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 210062, China.

State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China.

出版信息

Environ Sci Technol. 2020 Dec 15;54(24):15622-15630. doi: 10.1021/acs.est.0c04544. Epub 2020 Nov 30.

Abstract

To understand the chemical evolution of dust in the current East Asian atmosphere, the chemistry of PM and size-resolved aerosols in Shanghai, China, during the 2019 dust storm event was investigated. Our results showed that concentrations of SO in the city during the event highly correlated with Ca and Na due to the direct emissions of CaSO and NaSO from the upwind deserts. In contrast, during the event, NO linearly correlated with NH at a molar ratio close to 1:1, and both almost entirely stayed in coarse particles, suggesting they accumulated on the dust surface as NHNO. Based on the field observations and laboratory smog chamber simulations, we found that NO and O in Shanghai during the dust period reacted to form NO, which subsequently hydrolyzed into HNO on the surface of saline mineral dusts (e.g., CaSO and NaSO) and was further neutralized by NH as NHNO. The relative abundances of NO and NH in Shanghai during the dust event were notably higher than those a decade ago, indicating that this heterogeneous formation of NHNO on dust was enhanced by the abundantly coexisting NO, O, and NH in the current East Asian atmosphere, which should be considered in future modeling studies.

摘要

为了了解当前东亚大气中尘埃的化学演化过程,研究了 2019 年沙尘事件期间中国上海 PM 和粒径分辨气溶胶的化学性质。研究结果表明,由于上风沙漠中 CaSO 和 NaSO 的直接排放,沙尘事件期间城市中 SO 的浓度与 Ca 和 Na 高度相关。相比之下,在事件期间,NO 与 NH 呈线性相关,摩尔比接近 1:1,且两者几乎全部存在于粗颗粒中,表明它们作为 NHNO 积聚在尘埃表面。基于现场观测和实验室烟雾箱模拟,我们发现沙尘期间上海的 NO 和 O 反应形成 NO,随后在盐性矿物尘埃(如 CaSO 和 NaSO)表面水解生成 HNO,并进一步被 NH 中和为 NHNO。沙尘事件期间上海的 NO 和 NH 的相对丰度明显高于十年前,这表明当前东亚大气中大量共存的 NO、O 和 NH 增强了 NHNO 在尘埃上的非均相形成,这在未来的建模研究中应加以考虑。

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