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解析上海碳质气溶胶的消光特性及其影响因素。

Deconvolving light absorption properties and influencing factors of carbonaceous aerosol in Shanghai.

机构信息

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China.

Shanghai Environmental Monitoring Center, Shanghai 200235, China.

出版信息

Sci Total Environ. 2022 Sep 15;839:156280. doi: 10.1016/j.scitotenv.2022.156280. Epub 2022 May 27.

Abstract

Black carbon (BC) and brown carbon (BrC) have intensive impacts on atmospheric visibility and global climate change. In this study, PM samples were collected at Pudong (PD) and Qingpu (QP) of Shanghai in 2017, and characterized typical organic molecular tracers by gas chromatography-mass spectrometer. The light absorption (Abs) of carbonaceous aerosol and water-soluble organic matter was analyzed by a multi-wavelength thermal/optical carbon analyzer and a long-range ultraviolet-visible spectrophotometer. An improved two-component model integrated with both optical and chemical fingerprints of carbonaceous aerosol was applied to analyze the Abs of BC, water-soluble organic carbon (WSOC) and water-insoluble organic carbon (WISOC), with which the potential influencing factors including emission source and atmospheric aging were investigated. Results indicated that BrC contributed 19% at PD and 16% at QP of the total light absorption of the carbonaceous aerosol at 405 nm wavelength. Meanwhile, Abs/Abs showed significant seasonal variations (27-50%) at both sites. Positive matrix factorization (PMF) analysis showed that vehicle emissions (60-61%) and biomass combustion (38-39%) were the major contributors to Abs, while biomass burning (34-40%), nitrate-relevant secondary processes (22-23%), vehicle emissions (18-19%) and biogenic SOA (13-19%) were major contributors to Abs. Hybrid combustion source (94-96%) had a predominant contribution to Abs. Statistical analysis showed that biomass burning had a great impact on the enhancement of Abs. Absorption Ångström exponent (AAE) and mass absorption efficiency (MAE) of each factor (source) using PMF analysis indicated that WSOC from combustion sources had higher AAE values (8.11 and 8.29 for coal and biomass burning, respectively) and MAE values (0.63-0.99) compared to other sources. Atmospheric aging process can lower the MAE value (0.24-0.52). Overall, our study facilitates a better understanding of the relationships among source, optical properties, and atmospheric transformation processes of the carbonaceous aerosols in Shanghai.

摘要

黑碳(BC)和棕碳(BrC)对大气能见度和全球气候变化有强烈影响。本研究于 2017 年在上海浦东(PD)和青浦(QP)采集 PM 样本,利用气相色谱-质谱仪对典型有机分子示踪剂进行了特征描述。利用多波长热/光碳分析仪和长程紫外-可见分光光度计分析了碳质气溶胶和水溶性有机物质的光吸收(Abs)。应用一种改进的双组分模型,结合碳质气溶胶的光学和化学指纹,分析了 BC、水溶性有机碳(WSOC)和水不溶性有机碳(WISOC)的 Abs,探讨了排放源和大气老化等潜在影响因素。结果表明,PD 和 QP 站点 405nm 波长下,BC 对碳质气溶胶总吸光的贡献分别为 19%和 16%。同时,两个站点的 Abs/Abs 均表现出显著的季节性变化(27-50%)。正定矩阵因子分析(PMF)表明,机动车排放(60-61%)和生物质燃烧(38-39%)是 Abs 的主要贡献源,而生物质燃烧(34-40%)、硝酸盐相关二次过程(22-23%)、机动车排放(18-19%)和生物源 SOA(13-19%)也是 Abs 的主要贡献源。混合燃烧源(94-96%)对 Abs 有主要贡献。统计分析表明,生物质燃烧对 Abs 的增强有重大影响。PMF 分析得到的每个因子(源)的吸收 Ångström 指数(AAE)和质量吸收效率(MAE)表明,来自燃烧源的 WSOC 具有更高的 AAE 值(煤炭和生物质燃烧分别为 8.11 和 8.29)和 MAE 值(0.63-0.99),高于其他源。大气老化过程会降低 MAE 值(0.24-0.52)。总之,本研究有助于更好地理解上海碳质气溶胶的源、光学特性和大气转化过程之间的关系。

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