珠三角典型区域臭氧成因分析与VOCs来源解析——以中山为例

doi:10.16258/j.cnki.1674-5906.2023.03.008

生态环境学报 ›› 2023, Vol. 32 ›› Issue (3): 500-513.DOI: 10.16258/j.cnki.1674-5906.2023.03.008

珠三角典型区域臭氧成因分析与VOCs来源解析——以中山为例

温丽容¹^,³(), 江明¹, 黄渤², 袁鸾¹, 周炎¹, 陆炜梅², 张莹¹, 刘明², 张力昀²

1.广东省生态环境监测中心/国家环境保护区域空气质量监测重点实验室，广东广州 510308
2.广州禾信仪器股份有限公司，广东广州 510530
3.广东省环境辐射监测中心，广东广州 510300

收稿日期:2023-01-06 出版日期:2023-03-18 发布日期:2023-06-02
作者简介:温丽容（1975年生），女，副高级工程师，硕士，研究方向为大气环境。E-mail: 105771055@qq.com
基金资助:
广东省重点领域研发计划(2020B1111360003)

Analysis of Ozone Pollution Causes and Source Analysis of VOCs in Typical Areas of Pearl River Delta: A Case Study of Zhongshan City

WEN Lirong¹^,³(), JIANG Ming¹, HUANG Bo², YUAN Luan¹, ZHOU Yan¹, LU Weimei², ZHANG Ying¹, LIU Ming², ZHANG Liyun²

1. State Environmental Key Laboratory of Regional Air Quality Monitoring/Guangdong Environmental Monitoring Center, Guangzhou 510308, P. R. China
2. Guangzhou Hexin Instrument Co., Ltd., Guangzhou 510530, P. R. China
3. Guangdong Environmental Radiation Monitoring Center, Guangzhou 510300, P. R. China

Received:2023-01-06 Online:2023-03-18 Published:2023-06-02

摘要/Abstract

摘要：

近年来，珠三角地区臭氧污染不断加剧，其重要原因之一在于臭氧与其前体物浓度之间存在非线性关系，不平衡的前体物削减会导致臭氧浓度不降反升，深入分析臭氧前体物与臭氧浓度之间的关系及解析VOCs的来源对于臭氧污染控制具有重要意义。中山市作为珠三角城市群的一个代表性城市，目前臭氧污染极其严重。选取当地5个站点，采取在线和离线两种监测方式，于2020年和2021年臭氧污染较严重的9月，开展臭氧前体物VOCs监测，并进行臭氧污染成因分析和VOCs来源解析。结果表明，2021年紫马岭站点的TVOC平均质量浓度达到127.5 μg·m^-3，高于其他站点，且同比上升5.2 μg·m^-3，主要原因是烷烃质量浓度从27.3 μg·m^-3大幅上升到44.6 μg·m^-3；2020年和2021年9月TVOC的质量浓度波动幅度均较大且不规律，中旬和下旬的整体质量浓度水平较高。臭氧敏感性分析表明，2020年9月中山市臭氧污染为明显的VOCs控制区，而2021年9月则为协同控制区。削减分析得出，结合中山市实际污染情况，灵活选择1:3或1:2的ρ_(NO_x₎/ρ_(VOCs)比例进行削减更有利于臭氧治理。观测期间在线和离线监测站点的臭氧生成潜势（OFP）分析显示异戊二烯、间/对-二甲苯、甲苯、邻-二甲苯、1, 2, 4-三甲苯、乙烯为中山市的臭氧污染优控物种。VOCs来源解析表明中山市2020年和2021年VOCs浓度贡献最大的来源均为机动车尾气及油品挥发源，分别占比37.4%和32.4%；OFP贡献最大的来源均为溶剂使用源，分别占比23.6%和22.2%。综上所述，为有效缓解中山市臭氧污染，建议重点对机动车尾气及油品挥发源和溶剂使用源进行控制。

关键词: 臭氧, 前体物, 臭氧生成潜势, EMKA曲线, 光化学箱模型OBM, PMF模型

Abstract:

In recent years, ozone pollution in the Pearl River Delta is getting worse. One of the key reasons is the nonlinear relationship between ozone and its precursor concentration; unbalanced precursor reduction may lead to an increase in ozone concentration. Therefore, research on the relationship between ozone and its precursors, as well as the sources of VOCs is of great significance for ozone pollution control. As a representative city of the Pearl River Delta city group, ozone pollution in Zhongshan is extremely serious. In this study, we launched a monitoring campaign in Zhongshan in September of 2020 and 2021, when ozone pollution is relatively severe. Five monitoring sites were selected to represent the air quality of Zhongshan, and both online and offline monitoring methods were used. The results showed that the average TVOC concentration on the Zimaling site in 2021 was 127.5 μg·m^-3, higher than that on the other sites, and increased by 5.2 μg·m^-3 since 2020, mainly due to the large increase of alkane quality concentration from 27.3 μg·m^-3 to 44.6 μg·m^-3；the quality concentration fluctuations of TVOC in September 2020 and 2021 were both significant and irregular, with overall high quality concentration levels in the middle and late stages. Ozone sensitivity analysis showed that ozone formation in Zhongshan City was VOC-limited in September 2020, while it was controlled by a transition regime in September 2021. According to the precursor reduction simulation, emission cut of NO_x and VOCs following a ratio of 1:3 or 1:2 would be a more conducive measure for ozone control. Analysis of ozone formation potential (OFP) at online and offline monitoring stations during the observation period showed that isoprene, m/p-xylene, toluene, o-xylene, 1, 2, 4-trimethylbenzene, and ethylene were the dominant species for ozone formation in Zhongshan City. Source apportionment results showed that vehicle exhaust and oil volatile were the largest sources of VOCs in Zhongshan City in both 2020 and 2021, accounting for 37.4% and 32.4%, respectively, while solvent use source was the largest source of OFP, accounting for 23.6% and 22.2% in 2020 and 2021, respectively. In summary, in order to effectively alleviate the ozone pollution in Zhongshan City, it is recommended to focus on the control of vehicle exhaust, oil volatile sources and solvent use sources.

Key words: ozone, precursor, ozone formation potential, EMKA curve, photochemical box model OBM, PMF model

中图分类号:

温丽容, 江明, 黄渤, 袁鸾, 周炎, 陆炜梅, 张莹, 刘明, 张力昀. 珠三角典型区域臭氧成因分析与VOCs来源解析——以中山为例[J]. 生态环境学报, 2023, 32(3): 500-513.

WEN Lirong, JIANG Ming, HUANG Bo, YUAN Luan, ZHOU Yan, LU Weimei, ZHANG Ying, LIU Ming, ZHANG Liyun. Analysis of Ozone Pollution Causes and Source Analysis of VOCs in Typical Areas of Pearl River Delta: A Case Study of Zhongshan City[J]. Ecology and Environment, 2023, 32(3): 500-513.

图/表 19

图1 中山市现有的空气监测点位

Figure 1 Existing air monitoring points in Zhongshan City

图2 中山市各监测站点2017-2019年臭氧质量浓度和臭氧超标天数对比

Figure 2 Comparison of ozone mass concentration and pollution days at monitoring stations in Zhongshan City from 2017 to 2019

图3 中山市各监测站点2017-2019年臭氧月均质量浓度对比

Figure 3 Comparison of monthly mass concentrations of ozone at monitoring stations in Zhongshan City from 2017 to 2019

图4 中山市各站点2020年和2021年VOC类别质量浓度对比

Figure 4 Comparison of mass concentrations of VOC category at Zhongshan City stations in 2020 and 2021

图5 中山市紫马岭在线监测VOCs总质量浓度和O3质量浓度变化趋势

Figure 5 Change trend of total VOCs (TVOC) and O3 mass concentration monitored online in Zimaling, Zhongshan City

表1 中山市2020年各站点前10组分的质量浓度

Table 1 Mass concentrations of the top 10 components at each station in Zhongshan City in 2020

前10组分质量浓度/ (μg·m^-3)	紫马岭公园	长江旅游区	张溪	华柏园
乙酸乙酯	15.2	13.6	12.0	11.7
二氯甲烷	8.6	9.3	8.2	9.4
甲苯	8.6	7.7	7.1	7.8
2-丁酮	6.4	7.1	5.6	5.4
间/对-二甲苯	5.1	4.7	5.7	5.8
异戊烷	4.9	4.4	3.2	3.9
正丁烷	3.9	3.4	3.6	4.5
丙烷	3.2	3.0	3.0	3.9
丙醛	3.6	4.4	-	3.5
异丙醇	-	2.7	2.7	-
二氟二氯甲烷	-	-	2.5	2.7
己醛	3.4	-	-	-
总和	62.8	60.3	53.5	58.5
占比	51.0%	51.4%	50.9%	49.1%

表2 中山市2021年各站点前10组分的质量浓度

Table 2 Mass concentrations of the top 10 components at each station in Zhongshan City in 2021

前10组分质量浓度/(μg·m^-3)	紫马岭公园	长江旅游区	中山南区	张溪	华柏园
乙酸乙酯	8.5	12.9	5.2	6.2	5.7
2-丁酮	7.5	5.3	9.4	4.6	6.9
丙醛	3.6	7.2	6.5	6.8	8.2
甲苯	9.2	4.6	3.8	4.3	6.2
二氯甲烷	8.6	4.0	4.1	5.1	5.7
间/对-二甲苯	3.7	3.6	2.9	3.2	5.0
正丁烷	11.8	-	3.1	4.0	4.0
丙烷	9.4	-	3.7	3.6	4.3
己醛	-	3.8	3.1	3.0	3.6
异丁烷	8.4	-	-	3.1	3.8
正丁醛	-	2.9	3.1	-	-
异戊二烯	4.0	-	-	-	-
丙烯醛	-	2.3	-	-	-
二氟二氯甲烷	-	2.1	-	-	-
总和	74.6	48.8	44.7	43.7	53.5
占比	55.4%	55.6%	47.4%	45.8%	45.3%

图6 EKMA曲线图图中粉色圆点所表征的即为该监测期间污染时段内中山市紫马岭监测站点VOCs和NOx的平均质量浓度

Figure 6 EKMA Curve

图7 不同削减比例对基准臭氧浓度的变化影响图中黑色虚线为相较于基准情景需使臭氧质量浓度水平达到160 μg·m-3的基准线，不同颜色代表了不同的ρ(NOx)/ρ(VOCs)削减情景

Figure 7 The impact of different reduction ratios on the change of baseline ozone concentration

表3 中山市2020年各站点OFP排名前10 PAMS组分

Table 3 Top 10 PAMS components of OFP in Zhongshan City in 2020

前10组分OFP/ (μg·m^-3)	紫马岭公园	长江旅游区	张溪	华柏园
间/对-二甲苯	40.2	35.9	43.4	41.7
甲苯	33.8	30.1	27.5	29.2
邻-二甲苯	16.9	14.7	17.9	16.6
1, 2, 4-三甲苯	10.7	8.9	9.0	10.7
异戊二烯	10.5	8.5	6.3	8.8
乙烯	6.8	5.9	5.4	9.0
异戊烷	6.6	6.0	4.4	5.1
丙烯	5.7	5.8	5.4	7.8
乙苯	5.6	5.1	5.8	5.5
1, 3, 5-三甲苯	5.4	5.0	4.5	4.9
总和	142.1	125.9	129.7	139.1
占比	75.9%	75.7%	77.5%	75.7%

表4 中山市2021年各站点OFP排名前10 PAMS组分

Table 4 Top 10 PAMS Components of OFP in Zhongshan City in 2021

前10组分OFP/(μg·m^-3)	紫马岭公园	长江旅游区	中山南区	张溪	华柏园
异戊二烯	41.3	17.6	13.4	28.8	17.0
甲苯	35.8	17.7	16.5	24.2	14.7
间/对-二甲苯	27.8	28.3	24.0	38.2	21.9
邻-二甲苯	13.5	11.1	11.4	19.1	10.1
1, 2, 4-三甲苯	8.0	4.6	6.0	7.9	5.0
乙烯	5.8	4.1	6.7	8.8	7.6
乙苯	-	3.4	3.7	5.4	3.2
丙烯	-	2.4	3.8	5.1	4.9
正丁烷	12.7	-	4.3	-	3.4
异丁烷	9.8	-	3.6	4.5	-
异戊烷	-	2.3	-	4.6	3.6
1, 3, 5-三甲苯	3.9	2.4	-	-	-
丙烷	4.3	-	-	-	-
总和	163.0	93.7	93.4	146.6	91.5
占比	80.6%	80.0%	72.8%	75.4%	73.3%

图8 紫马岭在线站点2020年9月各污染源的VOCs质量浓度成分谱

Figure 8 Quality concentration composition spectra of VOCs from various pollution sources at Zimaling Online Station in September 2020

图9 紫马岭站点（2020年在线）各污染源对VOCs质量浓度和OFP的贡献率

Figure 9 Contribution rate of various pollution sources to VOCs mass concentration and OFP at Zimaling Station (online in 2020)

图10 2020年监测期间OFP贡献前10种VOC组分的各污染源占比

Figure 10 Proportion of each pollution source of the top 10 VOC components contributed by OFP during the monitoring period in 2020

图11 紫马岭在线站点2021年9月各污染源的VOCs质量浓度成分谱

Figure 11 Quality concentration composition spectrum of VOCs from various pollution sources at Zimaling online site in September 2021

图12 紫马岭站点（2021年在线）各污染源对VOCs质量浓度和OFP的贡献占比

Figure 12 Proportion of contribution of various pollution sources to VOCs quality concentration and OFP at Zimaling Station (online in 2021)

图13 2021年监测期间OFP贡献前10种VOC组分的各污染源占比

Figure 13 Proportion of each pollution source of the top 10 VOC components contributed by OFP during the monitoring period in 2021

图14 典型物种实际值与模拟值时间序列

Figure 14 Time series of actual and simulated values of typical species

表5 广东省不同地区来源分布对比

Table 5 Comparison of source distribution in different regions of Guangdong Province

地点	时间	来源分布	相关文章
中山市紫马岭	2020年9月1日-30日	机动车尾气及油品挥发源 (37.4%)、工业排放源 (18.3%)、燃烧源 (14.6%)、石油化工源 (12.8%)、溶剂使用源 (11.4%)、植物源 (5.4%)	本研究
中山市紫马岭	2021年9月1日-30日	机动车尾气及油品挥发源 (32.4%)、溶剂使用源 (16.0%)、燃烧源 (13.2%)、工业排放源 (13.1%)、石油化工源 (12.7%)、植物源 (12.6%)	本研究
广州市中心城区	2020年1月1日-9日	汽车尾气源 (22.4%)、溶剂使用源 (20.5%)、工业排放源 (17.9%)、生物质燃烧源 (16.5%)、油品挥发源 (13.0%)和植物源 (9.7%)	裴成磊等, 2022
广州磨碟沙	2015年10月15日- 11月10日	液化石油气使用 (32%)、机动车尾气 (27%)、工艺过程 (12%)、二次生成源 (9%)、化工行业 (8%)、溶剂涂料使用 (7%)和天然源 (5%)	蒋美青等, 2018
汕头市达濠中学	2019年10月7日-31日	机动车排放源 (38.0%)、汽油泄露与挥发源 (16.5%)、植物排放源 (5.5%)、溶剂使用源 (20.4%)、油燃烧源 (7.9%)、化工排放源 (11.7%)	李娟等, 2021
佛山市狮山镇	2021年4月1日-30日	溶剂使用源 (25.9%)、LPG排放源 (23.2%)、机动车排放源 (18.8%)、燃烧源 (17.4%)、燃料挥发源 (12.1%)和植物排放源 (2.7%)	李瑞瑜等, 2021

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珠三角典型区域臭氧成因分析与VOCs来源解析——以中山为例

Analysis of Ozone Pollution Causes and Source Analysis of VOCs in Typical Areas of Pearl River Delta: A Case Study of Zhongshan City

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