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氮同位素表明,2018 年 12 月,农业和非农业源对北京城区的 NH 和 NH 贡献相当。

Nitrogen isotopes suggest agricultural and non-agricultural sources contribute equally to NH and NH in urban Beijing during December 2018.

机构信息

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

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

出版信息

Environ Pollut. 2023 Jun 1;326:121455. doi: 10.1016/j.envpol.2023.121455. Epub 2023 Mar 17.

Abstract

Agricultural and non-agricultural sources emission contribute to atmospheric ammonia (NH) and particulate ammonium (NH). However, our understanding on the sources of NH and NH in PM (particles smaller than 2.5 μm) during the winter period in the urban atmosphere is limited. Here, we measured the concentrations and stable nitrogen isotopic composition (δN) of NH and NH in parallel during December 2018 in urban Beijing to assess the non-agricultural and agricultural sources contributions to NH and NH in ambient air based on the Chemical Transport Model (CTM), a Bayesian isotope mixing model (SIMMR), and the δN signatures that we developed. Our study found weekly NH and NH concentrations were on average 2.5 ± 1.4 μg m and 3.8 ± 1.7 μg m, respectively during December 2018. Weekly concentration weighted δN(NH) values ranged from 4.5‰ to 13.7‰ with an average value of 8.2 ± 3.9‰ during December 2018. After accounting for nitrogen isotopic fractionation from NH gas to NH conversion, initial δN(NH) values ranged from -22.5‰ to -12.8‰ with an average value of -17.4 ± 3.5‰. Further, weekly measured δN(NH) values ranged from -22.2‰ to -10.2‰ (after correction) with an average value of -15.6 ± 5.3‰ during December 2018. Results from two different isotope-based method showed non-agricultural sources contributed 31.2%-63.1%, with an average value of 47.5 ± 14.6%, to NH and 32.3%-71.2%, with an average of 53.4 ± 16.1%, to ambient NH during December 2018 in Beijing. Results from CMAQ-ISAM suggest non-agricultural sources contributed on average 66.2 ± 1.9% to ambient NH and 66.4 ± 1.9% to ambient NH during December 2018. Results from this study suggest that agricultural and non-agricultural sources nearly equally contributed to NH and NH in urban Beijing during December 2018 with an uncertainty range of 13%-19% between isotope-based methods and CTM method.

摘要

农业和非农业源排放贡献了大气氨(NH)和颗粒态铵(NH)。然而,我们对城市大气冬季期间 PM(粒径小于 2.5μm 的颗粒)中 NH 和 NH 的来源的理解是有限的。在这里,我们在 2018 年 12 月平行测量了北京城区大气中 NH 和 NH 的浓度和稳定氮同位素组成(δN),基于化学输送模型(CTM)、贝叶斯同位素混合模型(SIMMR)以及我们开发的 δN 特征,评估非农业和农业源对环境空气中 NH 和 NH 的贡献。我们的研究发现,2018 年 12 月,NH 和 NH 的周平均浓度分别为 2.5±1.4μg/m 和 3.8±1.7μg/m。2018 年 12 月,周加权浓度 δN(NH)值范围为 4.5‰至 13.7‰,平均值为 8.2±3.9‰。在考虑从 NH 气体到 NH 转化的氮同位素分馏后,初始 δN(NH)值范围为-22.5‰至-12.8‰,平均值为-17.4±3.5‰。此外,2018 年 12 月,每周测量的 δN(NH)值范围为-22.2‰至-10.2‰(经修正后),平均值为-15.6±5.3‰。两种不同同位素方法的结果表明,非农业源在 2018 年 12 月对 NH 的贡献为 31.2%-63.1%,平均值为 47.5±14.6%,对环境 NH 的贡献为 32.3%-71.2%,平均值为 53.4±16.1%。CMAQ-ISAM 的结果表明,非农业源在 2018 年 12 月对环境 NH 的贡献平均为 66.2±1.9%,对环境 NH 的贡献平均为 66.4±1.9%。本研究结果表明,在 2018 年 12 月,农业和非农业源对北京城区大气中的 NH 和 NH 贡献几乎相等,同位素方法和 CTM 方法之间的不确定性范围为 13%-19%。

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