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洛杉矶盆地有机碳(OC)来源中 PM 源的长期变化趋势及其对 PM 排放法规的影响。

Long-term trends in the contribution of PM sources to organic carbon (OC) in the Los Angeles basin and the effect of PM emission regulations.

机构信息

University of Southern California, Department of Civil and Environmental Engineering, 3620 S. Vermont Ave. KAP210, Los Angeles, CA 90089, USA.

出版信息

Faraday Discuss. 2021 Mar 1;226:74-99. doi: 10.1039/d0fd00074d. Epub 2020 Nov 26.

Abstract

This study aimed to investigate the long-term variations in the contributions of emission sources to ambient PM organic carbon (OC) in central Los Angeles (CELA) and Riverside using the Chemical Speciation Network (CSN) database in the 2005-2015 period, during which several federal and state PM-based regulations were implemented to reduce tailpipe emissions in the region. The measured concentrations of OC, OC volatility fractions (i.e., OC, OC, and OC), elemental carbon (EC), ozone (O), sulfate, the ratio of potassium ion to potassium (K/K), and selected metal elements were used as the input to the positive matrix factorization (PMF) model. PMF resolved tailpipe emissions, non-tailpipe emissions, secondary organic aerosols (SOA), biomass burning, and local industrial activities as the main sources contributing to ambient OC at both sampling sites. Vehicular exhaust emissions, non-tailpipe emissions, and SOA were dominant sources of OC across our sampling sites, accounting cumulatively for more than 80% of total OC mass throughout the study period. Our findings showed a significant reduction in the absolute and relative contributions of tailpipe emissions to the ambient OC levels in CELA and Riverside over the time period of 2005-2015. The contribution of exhaust emissions to total OC in CELA decreased from 3.5 µg m (49%) in 2005 to 1.5 µg m (34%) in 2015, while similar trends were observed at Riverside during this period. These reductions are mainly attributed to the implementation of several federal, state, and local air quality regulations targeting tailpipe emissions in the area. The implementation of these regulations furthermore reduced the emissions of primary organic precursors of secondary aerosols, resulting in an overall decrease (although not statistically significant, P values ranging from 0.4 to 0.6) in SOA mass concentration in both locations over the study period. In contrast to the tailpipe emissions, we observed an increasing trend (by ∼4 to 14%) in the relative contribution of non-tailpipe emissions to OC over this time period at both sites. Our results demonstrated the effectiveness of air quality regulations in reducing direct tailpipe emissions in the area, but also underpinned the need to develop equally effective mitigation policies targeting non-tailpipe PM emissions.

摘要

本研究旨在利用 2005-2015 年期间化学物质谱网络(CSN)数据库,调查洛杉矶中心(CELA)和河滨市大气 PM 有机碳(OC)排放源长期变化情况,在此期间,该地区实施了几项基于 PM 的联邦和州法规,以减少尾气排放。OC、OC 挥发分数(OC、OC 和 OC)、元素碳(EC)、臭氧(O)、硫酸盐、钾离子与钾(K/K)的比值以及选定金属元素的实测浓度被用作正矩阵因子分解(PMF)模型的输入。PMF 将尾气排放、非尾气排放、二次有机气溶胶(SOA)、生物质燃烧和当地工业活动解析为两个采样点大气 OC 的主要来源。在整个研究期间,机动车尾气排放、非尾气排放和 SOA 是 OC 的主要来源,累计占 OC 总量的 80%以上。研究结果表明,在 2005-2015 年期间,CELA 和河滨市大气 OC 水平的尾气排放的绝对和相对贡献显著降低。CELA 大气 OC 中尾气排放对总 OC 的贡献从 2005 年的 3.5µg/m(49%)下降到 2015 年的 1.5µg/m(34%),同期河滨市也呈现出类似的趋势。这些减少主要归因于该地区实施了几项针对尾气排放的联邦、州和地方法规。这些法规的实施进一步减少了二次气溶胶的主要有机前体的排放,导致研究期间两个地点的 SOA 质量浓度总体下降(尽管无统计学意义,P 值范围为 0.4 至 0.6)。与尾气排放相反,我们观察到在此期间两个站点 OC 中非尾气排放的相对贡献呈上升趋势(增加 4%至 14%)。研究结果表明,空气质量法规在减少该地区直接尾气排放方面的有效性,但也强调需要制定同样有效的针对非尾气 PM 排放的缓解政策。

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