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北京冬季单个含有机物颗粒的日变化化学组成和形成过程的特征。

Distinct diurnal chemical compositions and formation processes of individual organic-containing particles in Beijing winter.

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing Key Laboratory of Indoor Air Quality Evaluation and Control, Tsinghua University, Beijing 100084, China.

Support Center for Scientific Instrument Renovation and Custom Fabrication, Osaka University, Osaka, 560-0043, Japan; Project Research Center for Fundamental Sciences, Graduate School of Science, Osaka University, Osaka, 560-0043, Japan.

出版信息

Environ Pollut. 2023 Feb 1;318:120846. doi: 10.1016/j.envpol.2022.120846. Epub 2022 Dec 7.

Abstract

Organic aerosols (OA) are major components of fine particulate matter, yet their formation mechanism remains unclear, especially in polluted environments. In this study, we investigated the diurnal chemical compositions and formation processes of OA in carbonaceous particles during winter in Beijing using aerosol time-of-flight mass spectrometry. We found that 84.5% of the measured carbonaceous particles underwent aging processes, characterized by larger diameter and more secondary species compared to fresh carbonaceous particles, and presented different chemical compositions of OA in the daytime and nighttime. During the day, under high O concentrations, organosulfates and oligomers existed in the aged carbonaceous particles, which were mixed with a higher signal of nitrate compared with sulfate. At night, under high relative humidity, distinct spectral signatures of hydroxymethanesulfonate and organic nitrogen compounds, and minor signals of other hydroxyalkylsulfonates and high molecular weight organic compounds were present in the aged carbonaceous particles, which were mixed with a higher signal of sulfate compared with nitrate. Our results indicated that photochemistry contributed to OA formation in the daytime, while aqueous chemistry played an important role in OA formation in the nighttime. The findings can help improve the performance of air quality and climate models on OA simulation.

摘要

有机气溶胶 (OA) 是细颗粒物的主要组成部分,但它们的形成机制仍不清楚,特别是在污染环境中。本研究利用气溶胶飞行时间质谱仪,在冬季对北京地区碳质颗粒中 OA 的日变化化学组成和形成过程进行了研究。结果表明,84.5%的实测碳质颗粒经历了老化过程,与新鲜碳质颗粒相比,老化颗粒的直径更大,且含有更多的二次产物;并且,碳质颗粒中的 OA 在白天和夜间呈现出不同的化学组成。在白天,高浓度的 O 存在时,老化的碳质颗粒中存在有机硫酸盐和低聚物,与硫酸盐相比,它们与更高浓度的硝酸盐混合存在。在夜间,高相对湿度下,老化的碳质颗粒中存在羟甲基磺酸和有机氮化合物的特征谱峰,以及其他羟基烷基磺酸和高分子量有机化合物的微弱信号,与硝酸盐相比,它们与更高浓度的硫酸盐混合存在。研究结果表明,光化学在白天有助于 OA 的形成,而水化学在夜间对 OA 的形成起着重要作用。这些发现有助于提高空气质量和气候模型对 OA 模拟的性能。

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