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在中国西南部一个大城市,尽管人为排放显著减少,但能见度改善受阻:在普遍高相对湿度条件下,增强的二次无机气溶胶形成与吸湿增长之间的相互作用。

Hindered visibility improvement despite marked reduction in anthropogenic emissions in a megacity of southwestern China: An interplay between enhanced secondary inorganics formation and hygroscopic growth at prevailing high RH conditions.

作者信息

Wan Fenglian, Hao Yuhang, Huang Wei, Wang Xinyu, Tian Mi, Chen Jing

机构信息

College of Environment and Ecology, Chongqing University, Chongqing, China.

National Meteorological Center, China Meteorological Administration, Beijing, China.

出版信息

Sci Total Environ. 2023 Oct 15;895:165114. doi: 10.1016/j.scitotenv.2023.165114. Epub 2023 Jun 26.

Abstract

The PM-bound visibility improvement remains challenging in China despite vigorous control on anthropogenic emissions in recent years. One critical issue could exist in the distinct physicochemical properties especially of secondary aerosol components. Taken the COVID-19 lockdown as an extreme case, we focus on the relationship between visibility, emission cuts, and secondary formation of inorganics with changing optical and hygroscopic behaviors in Chongqing, a representative city characterized with humid weather and poor diffusion conditions in Sichuan Basin, southwest of China. It is found that the increased secondary aerosol abundance (e.g., PM/CO and PM/PM as a proxy) with enhanced atmospheric oxidative capacity (e.g., O/Ox, Ox = O + NO), combined with insignificant meteorological dilution effect, might partly offset the benefit on the improved visibility from substantial reduction in anthropogenic emissions during the COVID-19 lockdown. This is in line with the efficient oxidation rates of sulfur and nitrogen (i.e., SOR, NOR), increasing more significantly with PM and relative humidity (RH) in comparison to O/Ox. The resulted larger fraction of nitrate and sulfate (i.e., f) would promote the optical enhancement (i.e., f(RH)) and mass extinction efficiency (MEE) of PM, especially under highly humid conditions (e.g., RH > 80 %, with approximately half of the occurrence frequency). This could further facilitate secondary aerosol formation via aqueous-phase reaction and heterogeneous oxidation, likely due to enhanced water uptake and enlarged size/surface area upon hydration. In combination of gradually increased atmospheric oxidative capacity, this positive feedback would in turn inhibit the visibility improvement particularly at high RH environment. Considering the current air pollution complex status over China, further work on the formation mechanisms of major secondary species (e.g., sulfate, nitrate, and secondary organics), size-resolved chemical and hygroscopic properties, together with their interactions are highly recommended. Our results are hoping to assist in the atmospheric pollution complex mitigation and prevention in China.

摘要

尽管近年来中国大力控制人为排放,但细颗粒物(PM)相关的能见度改善仍然具有挑战性。一个关键问题可能存在于尤其是二次气溶胶成分的独特物理化学性质中。以新冠疫情封锁作为一个极端案例,我们聚焦于中国西南部四川盆地一个以潮湿天气和扩散条件差为特征的代表性城市——重庆,研究能见度、排放削减与无机物二次生成之间的关系,以及光学和吸湿行为的变化。研究发现,随着大气氧化能力增强(如O/Ox,Ox = O + NO),二次气溶胶丰度增加(如以PM/CO和PM/PM作为指标),再加上气象稀释效应不显著,可能会部分抵消新冠疫情封锁期间人为排放大幅减少对能见度改善带来的益处。这与硫和氮的有效氧化率(即SOR、NOR)相符,与O/Ox相比,它们随PM和相对湿度(RH)的增加更为显著。由此导致的硝酸盐和硫酸盐更大比例(即f)会促进PM的光学增强(即f(RH))和质量消光效率(MEE),尤其是在高湿度条件下(如RH > 80%,出现频率约为一半)。这可能会通过水相反应和非均相氧化进一步促进二次气溶胶的形成,这可能是由于水吸收增强以及水合后粒径/表面积增大。结合大气氧化能力的逐渐增强,这种正反馈反过来会抑制能见度的改善,尤其是在高RH环境下。考虑到中国目前空气污染的复杂状况,强烈建议进一步开展关于主要二次物种(如硫酸盐、硝酸盐和二次有机物)的形成机制、粒径分辨的化学和吸湿性质及其相互作用的研究。我们的研究结果希望有助于中国大气污染的综合缓解和预防。

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