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共存的 NaSO 对不同 RH 下 CaCO 颗粒上异相吸收 NO 的影响。

The effects of coexisting NaSO on heterogeneous uptake of NO on CaCO particles at various RHs.

机构信息

State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.

State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China.

出版信息

Sci Total Environ. 2017 May 15;586:930-938. doi: 10.1016/j.scitotenv.2017.02.072. Epub 2017 Feb 16.

Abstract

Atmospheric particles can undergo nucleation, coagulation, chemical-aging, dissolution-precipitation or other atmospheric processes, resulting in complex multicomponent aerosols. The coexisting species have potentially important consequences in the heterogeneous reactions of multicomponent aerosol particles with polluted gases, which are still poorly understood. The effect of coexisting NaSO on heterogeneous uptake of NO on CaCO particles is investigated in a broad RH range. The combination of DRIFTS, Raman, SEM and IC provides qualitative and quantitative information about the formation of nitrate and other surface species. Ca(NO) and NaNO are generated on mixed CaCO-NaSO particles under dry condition. Both the amount of NO formed and the NO formation rates for the mixtures can be predicted based on the linear addition of those for pure CaCO and NaSO particles under dry condition. The further reaction of Ca(NO) with NaSO could lead to the formation of crystal NaNO and CaSO·0.5HO at 30% RH. Coagulation between Ca and SO in surface adsorbed water is observed after part conversion of CaCO to Ca(NO), resulting in the formation of CaSO·2HO at 80% RH. The amount of NO formed on the mixtures is dramatically enhanced relative to the predictions at 30% and 80% RH. The findings presented here highlight the role of coexisting species in the heterogeneous reactions of trace gases with multicomponent aerosols due to the complexity of atmospheric particles.

摘要

大气颗粒可经过成核、凝聚、化学老化、溶解-沉淀或其他大气过程,从而形成复杂的多组分气溶胶。共存物种在多组分气溶胶颗粒与污染气体的非均相反应中具有潜在的重要影响,但目前人们对此仍知之甚少。本研究在较宽的相对湿度范围内考察了共存的 NaSO 对 CaCO 颗粒上 NO 非均相吸收的影响。DRIFTS、拉曼、SEM 和 IC 的结合为硝酸盐和其他表面物种的形成提供了定性和定量信息。在干燥条件下,混合的 CaCO-NaSO 颗粒上会生成 Ca(NO)和 NaNO。基于干燥条件下纯 CaCO 和 NaSO 颗粒的线性加和,可以预测混合物中形成的 NO 量和形成速率。进一步的反应可能导致在 30% RH 下形成结晶的 NaNO 和 CaSO·0.5HO。在 CaCO 部分转化为 Ca(NO)后,观察到表面吸附水中的 Ca 和 SO 之间的凝聚,从而在 80% RH 下形成 CaSO·2HO。与 30%和 80% RH 下的预测相比,混合物上形成的 NO 量大大增加。本研究结果突出了共存物种在痕量气体与多组分气溶胶的非均相反应中的作用,这是由于大气颗粒的复杂性所致。

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