硝酸盐PM2.5来源解析及机理分析：OH和N2O5的时空变化相互作用

IF 8 1区环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES

Science of the Total Environment Pub Date : 2025-06-11 DOI:10.1016/j.scitotenv.2025.179813

Li-Ti Chou , Yan-Syuan Lin , Ta-Chih Hsiao , Pei-Ling Wang , Li-Hao Young , Kai-Hsien Chi , Stephen M. Griffith

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引用次数: 0

摘要

在污染期间，颗粒物硝酸盐是PM2.5的重要组成部分，为了有效的空气质量管理，需要精确的污染源分配。本研究利用2020年8月和10月在台中市宗明（ZM）市区和东海（TH）郊区采集的PM2.5样本（包括东海的日间采样），通过双同位素分析探讨了硝酸盐的形成机制。硝酸盐同位素组成（δ15N-NO3−和δ18O-NO3−）在采样点之间具有空间异质性，TH在其12 h测量中表现出较高的δ15N-NO3−平均值（2.6±2.4‰）和明显的日变化规律，而ZM的日综合样品平均值为0.6±2.1‰。相似的δ18O-NO3−模式在两个地点表明类似的氧化机制。oh介导的氧化及其产物在白天和夜间对PM2.5硝酸盐的贡献都很大，夏季占主导地位（81 - 83%），秋季随着N2O5途径的增加而下降（77±13%）。在夜间湿度升高的情况下，N2O5途径的有效性增强，与PM2.5浓度密切相关（R2 = 0.52）。使用MixSIAR进行的源分析发现，生物质燃烧和煤炭燃烧是氮氧化物的主要来源，另外还有车辆和生物土壤排放。这些发现强调了在制定有针对性的空气质量控制策略时，考虑形成机制的昼夜和季节变化的重要性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Source apportionment and mechanistic analysis of PM2.5 nitrate: interplay of OH and N2O5 in spatial and temporal variations

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Source apportionment and mechanistic analysis of PM2.5 nitrate: interplay of OH and N2O5 in spatial and temporal variations

Particulate nitrate, a substantial component of PM_2.5 during pollution episodes, requires precise source apportionment for effective air quality management. This study investigated nitrate formation mechanisms through dual-isotope analysis at an urban ZongMing (ZM) and suburban TungHai (TH) site in Taichung City, Taiwan, with PM_2.5 samples collected during August and October 2020, including diurnal sampling at TH. Analysis of nitrate isotopic compositions (δ¹⁵N-NO₃⁻ and δ¹⁸O-NO₃⁻) revealed spatial heterogeneity between the sampling sites, with TH exhibiting elevated mean δ¹⁵N-NO₃⁻ values (2.6 ± 2.4 ‰) and distinct diurnal patterns in its 12-h measurements, while daily integrated samples at ZM showed mean values of 0.6 ± 2.1 ‰. Similar δ¹⁸O-NO₃⁻ patterns at both sites indicated comparable oxidation mechanisms. OH-mediated oxidation and its products maintained substantial contributions to PM_2.5 nitrate during both day and night periods, dominating in summer (81–83 %) before declining in autumn (77 ± 13 %) as the N₂O₅ pathway increased. The N₂O₅ pathway showed enhanced effectiveness under elevated nocturnal humidity, correlating strongly with PM_2.5 concentrations (R² = 0.52). Source apportionment using MixSIAR identified biomass burning and coal combustion as primary NO_x sources, with additional contributions from vehicular and biogenic soil emissions. These findings emphasize the importance of considering both diurnal and seasonal variations in formation mechanisms for developing targeted air quality control strategies.

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来源期刊

Science of the Total Environment 环境科学-环境科学

CiteScore

17.60

自引率

10.20%

发文量

8726

审稿时长

2.4 months

期刊介绍： The Science of the Total Environment is an international journal dedicated to scientific research on the environment and its interaction with humanity. It covers a wide range of disciplines and seeks to publish innovative, hypothesis-driven, and impactful research that explores the entire environment, including the atmosphere, lithosphere, hydrosphere, biosphere, and anthroposphere. The journal's updated Aims & Scope emphasizes the importance of interdisciplinary environmental research with broad impact. Priority is given to studies that advance fundamental understanding and explore the interconnectedness of multiple environmental spheres. Field studies are preferred, while laboratory experiments must demonstrate significant methodological advancements or mechanistic insights with direct relevance to the environment.