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解析沿海气团中大气棕碳的吸收特性及驱动机制。

Unraveling the absorption properties and driving mechanisms of atmospheric brown carbon in coastal air masses.

作者信息

Li Siyuan, Liu Dantong, Wu Yangzhou, Hu Kang, Zhao Shitong, Jiang Xiaotong, Tian Ping, Xu Bin

机构信息

State Key Laboratory of Spatial Datum, College of Remote Sensing and Geoinformatics Engineering, Faculty of Geographical Science and Engineering, Henan University, Zhengzhou, 450046, China; Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou, 310058, China.

Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou, 310058, China.

出版信息

Environ Pollut. 2025 Oct 1;382:126713. doi: 10.1016/j.envpol.2025.126713. Epub 2025 Jun 20.

Abstract

Light-absorbing organic aerosols, optically defined as brown carbon (BrC), strongly absorb short visible solar wavelengths, significantly influencing regional climate and atmospheric environments. However, the relationship between the light-absorption properties of BrC and the chemical characteristics and sources of organic aerosols (OA) remains poorly understood. This study systematically investigated the light-absorption properties of BrC and their driving mechanisms in the Zhoushan coastal region, based on field observations, positive matrix factorization (PMF) source apportionment, and a random forest (RF) model. The results demonstrate that the light absorption of BrC is significantly influenced by air mass origins, OA factors, and chemical composition. Northern polluted air masses, characterized by high concentrations of particulate matter and OA, substantially enhanced the light absorption of BrC. OA with a high N/C ratio was found to strengthen BrC light absorption, while the O/C ratio exhibited a nonlinear relationship with BrC absorption, initially enhancing and subsequently weakening it, reflecting the dual role of atmospheric oxidation processes. Vessel-emission-related OA contributed the most to BrC light absorption, whereas highly oxidized OA likely reduced its absorption capacity due to photobleaching effects. The RF model significantly improved the prediction accuracy of BrC light absorption (R increased from 0.60 to 0.69) compared to traditional multiple linear regression (MLR) methods, effectively capturing the complex nonlinear relationships between BrC absorption and multiple variables. These findings reveal the importance of emissions, transportation, and atmospheric oxidation in the formation and evolution of BrC, providing new insights for optimizing air quality management in coastal areas.

摘要

光吸收有机气溶胶,光学上定义为棕碳(BrC),强烈吸收短可见光太阳波长,对区域气候和大气环境有显著影响。然而,BrC的光吸收特性与有机气溶胶(OA)的化学特征和来源之间的关系仍知之甚少。本研究基于实地观测、正定矩阵因子分解(PMF)源解析和随机森林(RF)模型,系统地研究了舟山沿海地区BrC的光吸收特性及其驱动机制。结果表明,BrC的光吸收受气团来源、OA因子和化学成分的显著影响。以高浓度颗粒物和OA为特征的北方污染气团显著增强了BrC的光吸收。发现高N/C比的OA增强了BrC的光吸收,而O/C比与BrC吸收呈非线性关系,最初增强随后减弱,反映了大气氧化过程的双重作用。与船舶排放相关的OA对BrC光吸收的贡献最大,而高度氧化的OA可能由于光漂白效应降低了其吸收能力。与传统多元线性回归(MLR)方法相比,RF模型显著提高了BrC光吸收的预测精度(R从0.60提高到0.69),有效捕捉了BrC吸收与多个变量之间复杂的非线性关系。这些发现揭示了排放、传输和大气氧化在BrC形成和演化中的重要性,为优化沿海地区空气质量管理提供了新的见解。

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