[Characteristics and Source Apportionment of Atmospheric Volatile Organic Compounds in Zhengzhou During O3 Campaign Period].

Q2 Environmental Science Huanjing Kexue/Environmental Science Pub Date : 2024-10-08 DOI:10.13227/j.hjkx.202310136
Si Chen, Jing-Wei Ni, Yi-Jin Qi, Tian-Tian Ji, Ling-Ling Wang, Xiao-Na Shan, Shan-Ling Gong
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Abstract

An online gas chromatograph (GC5000) was used to monitor the volatile organic compounds (VOCs) in the atmospheric environment of Zhengzhou City during the ozone campaign period from May to September of 2022. The relationship between O3 and its precursors as well as meteorology was analyzed and the pollution characteristics of VOCs during the O3 exceeding and non-exceeding the standard days were compared and explored. Different VOC activity evaluation methods of OFP and L·OH were utilized to compare and analyze the key active components and species and the ratio analysis (RA) and positive matrix factorization (PMF) analysis models were used to study the apportionment contribution of VOCs. The results showed that the O3 pollution in June and September in Zhengzhou was mainly due to the adverse meteorological conditions of high temperature and low humidity, strong radiation, and low wind speed, superimposed by the prominent concentrations of local VOCs and NO2, resulting in frequently high and excessive O3 occurrences. The VOCs concentration in Zhengzhou during the campaign period was an average of (68.3 ± 18.4) μg·m-3, whereas it was 75.7 μg·m-3 during O3 exceeding standard days and 13.4 μg·m-3 during O3 non-exceeding days, respectively. Among the VOC species, the OVOCs was 31.6%, accounting for the highest mass fraction, followed by halogenated hydrocarbon, alkane, and aromatic hydrocarbon, and the major species were ethane, n-butane, dichloromethane, propane, isopentane, toluene, chloromethane, 1,2-dichloroethane, and acetylene. VOC diurnal variation indicated that the emission of VOC pollution sources in the morning, evening peak, and at night should be paid more attention. The contribution of VOCs to OFP during the campaign period was (130.5 ± 46.4) μg·m-3, and the L·OH was (6.5 ± 2.9) s-1, among which the top 15 species with high activity were primarily acetaldehyde, isoprene, ethylene, m/p-xylene, toluene, hexal, isopentane, propanal, propylene, trans-2-butene, etc. In particular, the contributions of acetaldehyde, isoprene, ethylene, and hexal species were prominent during the O3 exceeding days. Ratio analysis showed that the B/T ratio in Zhengzhou from May to September ranged from 0.05 to 5.3, with an average value of 1.1 ± 0.6, and the regional VOCs was mainly controlled by the aging air mass with possible long-distance transports. The analysis of the PMF model showed that the major pollution sources to VOC concentration in Zhengzhou were motor vehicle exhaust emission sources and industrial solvent and secondary conversion sources, contributing 25.6% and 25.8%, respectively. The contribution rates of solvent coating sources, oil and gas volatile sources, plant emission sources, industrial solvents, and secondary conversion sources during O3 exceeding days were 5.4%, 4.7%, 3.3%, and 0.7% higher than those during O3 non-exceeding days, respectively. The research showed that the management of VOCs and NOx pollution sources should be strengthened to reduce their contribution to the O3 generation when O3 exceeds the standard.

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[O3 活动期间郑州大气挥发性有机化合物的特征和来源分配]。
使用在线气相色谱仪(GC5000)监测挥发性有机化合物(VOCs用于监测 2022 年 5 月至 9 月臭氧行动期间郑州市大气环境中的挥发性有机物(VOCs)。在2022年5月至9月臭氧行动期间,对郑州市大气环境中的挥发性有机物(VOCs)进行了监测。分析了 O3 与其前体物以及气象之间的关系,比较并探讨了 O3 超标日和非超标日 VOCs 的污染特征。利用OFP和L-OH不同的挥发性有机物活性评价方法对主要活性组分和物种进行了比较和分析,并利用比值分析法(RA)和正矩阵因式分解(PMF)分析模型来研究挥发性有机化合物的比例贡献。结果表明,郑州 6 月和 9 月的 O3 污染主要是由于高温低湿、强辐射、低风速等不利气象条件,叠加本地 VOCs 和 NO2 浓度突出,导致 O3 频繁偏高和超标。活动期间,郑州的 VOCs 浓度平均为(68.3±18.4)μg-m-3,而 O3 超标日为 75.7 μg-m-3,非超标日为 13.4 μg-m-3。在 VOC 种类中,OVOCs 占 31.6%,质量分数最高,其次是卤代烃、烷烃和芳香烃,主要种类有乙烷、正丁烷、二氯甲烷、丙烷、异戊烷、甲苯、氯甲烷、1,2-二氯乙烷和乙炔。VOC 的昼夜变化表明,应更多地关注早、晚高峰和夜间 VOC 污染源的排放情况。活动期间,VOCs 对 OFP 的贡献率为(130.5 ± 46.4)。μg-m-3,L-OH 为(6.5 ± 2.9)s-1,其中活性最高的 15 个物种主要是乙醛、异戊二烯、乙烯、间/对二甲苯、甲苯、己醛、异戊烷、丙醛、丙烯、反式-2-丁烯等。其中,乙醛、异戊二烯、乙烯和己醛的贡献在 O3 超标日尤为突出。比值分析表明,郑州 5-9 月的 B/T 比值在 0.05 至 5.3 之间,平均值为 1.1 ± 0.6,区域 VOCs 主要受老化气团控制,可能存在长距离输送。PMF 模型分析表明,郑州市 VOC 浓度的主要污染源为机动车尾气排放源和工业溶剂及二次转化源,贡献率分别为 25.6% 和 25.8%。在 O3 超标日,溶剂涂装源、油气挥发源、工厂排放源、工业溶剂和二次转化源的贡献率分别比 O3 非超标日高 5.4%、4.7%、3.3% 和 0.7%。研究表明,应加强对挥发性有机物和氮氧化物污染源的管理,以减少它们在 O3 超标时对 O3 生成的贡献。
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Huanjing Kexue/Environmental Science
Huanjing Kexue/Environmental Science Environmental Science-Environmental Science (all)
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