临汾市臭氧污染时期VOCs来源解析研究

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摘要本文通过基于光化学年龄的参数方法,估算了山西临汾市2021年4月18日~7月31日在线监测的VOCs初始体积分数数据,矫正其光化学损耗影响;然后利用正定矩阵因子分解(PMF)模型进行了其来源解析.结果表明,研究期间临汾市环境总VOCs(TVOCs)的平均体积分数为17.1×10^-9;其中白天TVOCs的平均初始体积分数为27.2×10^-9,其化学损耗达到10.6×10^-9,化学损耗率约为39.0%.相比与其它VOCs类别,烯烃化学损耗率最高(66.0%),其中异戊二烯(3.16×10^-9)、1,3-丁二烯(1.27×10^-9)和乙烯(1.19×10^-9)的化学损耗明显高于其它物种.臭氧污染时期TVOCs化学损耗达到15.1×10^-9,是非臭氧污染时期的1.6倍.臭氧污染时期烯烃的化学损耗率最高(81.7%),其中异戊二烯、1,3-丁二烯、反-2-丁烯和反-2-戊烯的化学损耗分别达到5.05×10^-9、1.85×10^-9、1.59×10^-9和1.10×10^-9,显著高于其它物种.基于初始体积分数的PMF来源解析(IC-PMF)结果发现,石化相关企业排放(36.4%)、天然气(17.2%)、柴油车排放和溶剂使用混合源(12.9%)、汽油车排放(9.6%)、液化石油气(8.6%)、植物排放(8.6%)和燃烧源(6.7%)是研究期间临汾市环境VOCs的主要贡献源类.相比于基于观测体积分数的PMF解析结果(OC-PMF),植物排放贡献被低估了83.3%,其被低估量明显高于其它源类;其次是柴油车排放和溶剂使用混合源以及石化相关企业排放,分别被低估了22.2%和19.7%.同时,IC-PMF结果表明臭氧污染期间贡献较高的源类是石化相关企业排放和植物排放,分别达到24.1%和21.7%.基于IC-PMF的解析结果,利用臭氧生成潜势(OFP)模型的估算结果表明,石化相关企业排放是臭氧生成潜势(OFP)最高的贡献源类,其对总OFP贡献率达到50.7%,其次为植物排放以及柴油车排放和溶剂使用混合源,其对总OFP的贡献率分别达到24.8%和10.4%;其中臭氧污染期间对于OFP的贡献较高的源类为植物排放和石化相关企业排放,分别达到52.6%和27.8%.

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关键词 ：临汾, 挥发性有机化合物, 光化学损耗, 初始体积分数, 源解析

Abstract：This study estimated the initial volume mixing ratios of the ambient VOCs measured from 18 April to 31 July 2021 in Linfen, Shanxi Province, using a photochemical age-based parameterization method, and corrected photochemical loss effects. Positive matrix factorization (PMF) was used to conduct the initial-data source apportionment. The results showed that the average volume mixing ratio of total VOCs (TVOCs) during the study period was 17.1×10^-9. The average initial volume mixing ratio of TVOCs in the daytime was 27.2×10^-9, with chemical loss of 10.6×10^-9 and loss rate was approximately 39.0%. Compared with other VOC groups, alkenes had the highest loss rate (66.0%). The chemical losses of isoprene (3.16×10^-9), 1,3-butadiene (1.27×10^-9), and ethylene (1.19×10^-9) were higher than any other species. During the ozone pollution (OP) period, the chemical loss of TVOCs was 15.1×10^-9, which was 1.6times higher than during the non-ozone pollution (NOP) period. During the OP period, the loss rate of alkenes was the highest (81.7%) than the other VOC groups. The losses of isoprene, 1,3-butadiene, trans-2-butene, and trans-2-pentene were 5.05×10^-9, 1.85×10^-9, 1.59×10^-9, and 1.10×10^-9, respectively, substantially higher than any other species. The PMF apportioned results based on the initial volume mixing ratios (i.e., IC-PMF) showed that petrochemical-related enterprise emissions (36.4%), natural gas (17.2%), the mixed source of diesel vehicle emissions and solvent usage (12.9%), gasoline vehicle emissions (9.6%), liquefied petroleum gas (8.6%), biogenic emissions (8.6%), and combustion sources (6.7%) were the main contributors to the ambient VOCs in Linfen during the study period. Compared to the PMF apportioned results based on the observed volume mixing ratios (i.e., OC-PMF), the contribution of biogenic emissions was underestimated by 83.3%, which was substantially higher than those of other sources; followed by the mixed sources of diesel vehicle emissions and solvent usage (22.2%) and the petrochemical-related enterprise emissions (19.7%). Meanwhile, the IC-PMF results suggested that the sources with higher contributions during the OP period were the petrochemical-related enterprise emissions and biogenic emissions, accounting for 24.1% and 21.7%, respectively. According to the IC-PMF apportioned results, the estimated results using the ozone formation potential (OFP) model showed that petrochemical-related enterprise emissions was the highest contributor to the OFP, with the contribution of 50.7% to the total OFP, followed by biogenic emissions (24.8%) and the mixed source of diesel vehicle emissions and solvent usage (10.4%). The emission sources with higher contributions to the OFP during OP period were biogenic emissions and petrochemical-related enterprise emissions, reaching 52.6% and 27.8%, respectively.

Key words： Linfen volatile organic compounds (VOCs) photochemical loss initial volume mixing ratio source apportionment

收稿日期: 2024-06-17

PACS:

X511

基金资助:国家重点研发计划项目(2023YFC3705801);国家自然基金资助面上项目(42177085)

通讯作者: 刘保双,副教授,lbsnankai@foxmail.com E-mail: lbsnankai@foxmail.com

作者简介: 段丽琴(1974-),女,山西临汾人,工程师,学士,研究方向为环境监测与数据分析.发表论文4篇.dlq740113a@126.com.

引用本文:

段丽琴, 吴雨彤, 刘保双. 临汾市臭氧污染时期VOCs来源解析研究[J]. 中国环境科学, 2025, 45(1): 78-92. DUAN Li-qin, WU Yu-tong, LIU Bao-shuang. Source apportionment of ambient VOCs during ozone pollution periods in Linfen. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(1): 78-92.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2025/V45/I1/78

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