基于多同位素的珠三角PM2.5中二次无机气溶胶来源解析

doi:10.16258/j.cnki.1674-5906.2023.09.012

生态环境学报 ›› 2023, Vol. 32 ›› Issue (9): 1654-1662.DOI: 10.16258/j.cnki.1674-5906.2023.09.012

基于多同位素的珠三角PM_2.5中二次无机气溶胶来源解析

温丽容¹^,³(), 林勃机², 李婷婷², 张子洋², 张正恩², 江明¹, 周炎¹, 张涛¹, 李军²^,^*(), 张干²

1.国家环境保护区域空气质量监测重点实验室/广东省生态环境监测中心，广东广州 510308
2.广东省环境资源利用与保护重点实验室/有机地球化学国家重点实验室/中国科学院广州地球化学研究所，广东广州 510640
3.广东省环境辐射监测中心，广东广州 510300

收稿日期:2023-05-19 出版日期:2023-09-18 发布日期:2023-12-11
通讯作者: ^*李军。E-mail: junli@gig.ac.cn
作者简介:温丽容（1975年生），女，副高级工程师，硕士，主要研究方向环境空气质量监测与研究。E-mail: 105771055@qq.com
基金资助:
广东省重点领域研发计划项目(2020B1111360003);国家自然科学基金项目(41977177)

Source Apportionment of Ammonium in Atmospheric PM_2.5 in the Pearl River Delta Based on Nitrogen Isotope

WEN Lirong¹^,³(), LIN Boji², LI Tingting², ZHANG Ziyang², ZHANG Zhengen², JIANG Ming¹, ZHOU Yan¹, ZHANG Tao¹, LI Jun²^,^*(), ZHANG Gan²

1. National Key Laboratory for Regional Air Quality Monitoring of Environmental Protection/Guangdong Ecological Environment Monitoring Center, Guangzhou 510308, P. R. China
2. Guangdong Province Key Laboratory of Environmental Protection and Resources Utilization/State Key Laboratory of organic geochemistry/Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, P. R. China
3. Guangdong Environmental Radiation Monitoring Center, Guangzhou 510300, P. R. China

Received:2023-05-19 Online:2023-09-18 Published:2023-12-11

摘要/Abstract

摘要：

二次无机气溶胶（SIA，Secondary inorganic aerosol）是PM_2.5中的重要组成部分，其快速形成是导致大气能见度下降的重要原因。二次无机气溶胶主要包括硫酸根、硝酸根和铵根离子，其来源广、生成途径复杂，识别其来源存在一定的挑战。最近，基于稳定同位素（δ³⁴S-SO₄²⁻、δ¹⁵N-NO₃⁻、δ¹⁸O-NO₃⁻、δ¹⁵N-NH₄⁺）的源解析方法被应用到相应污染物的来源解析。选取珠三角鹤山大气超级站作为研究地点，开展了为期1年的大气PM_2.5样品采集，在分析了70个样品的水溶性离子、痕量金属元素、有机碳、无机碳的基础上，选取其中的37个大气PM_2.5样品，分析了相应的δ³⁴S-SO₄²⁻、δ¹⁵N-NO₃⁻和δ¹⁸O-NO₃⁻、δ¹⁵N-NH₄⁺同位素值，结合稳定同位素平衡和优化的贝叶斯模型进行源解析，定量了各污染源对二次无机气溶胶的影响。结果表明，PM_2.5年平均质量浓度为39.8 μg•m⁻³。PM_2.5中SIA占比年均29.8%，呈现春季>冬季>夏季>秋季的季节变化规律，冬季二次污染程度较2013年明显下降；年均各SIA对颗粒质量浓度贡献顺序为硫酸根>硝酸根>铵根。δ³⁴S-SO₄²⁻值范围为1.8‰－9.6‰，平均值为4.5‰±1.7‰。源解析结果显示采样期间燃煤、燃油、生物成因硫排放对鹤山SO₄²⁻分别贡献了41.8%、32.9%、25.3%。δ¹⁵N-NO₃⁻范围为0.8‰－8.3‰，平均值为4.7‰±2.0‰。贝叶斯源解析结果显示，燃煤排放是鹤山NO₃⁻最主要来源，年均贡献率达到41.6%，其余污染源年均贡献率排序为，生物质燃烧 (BB)>汽油车>船舶>土壤微生物，贡献率依次为20.9%、15.6%、13.9%、8.0%。将各SIA浓度与对应的源解析结果合并，结果表明非化石源对总SIA贡献最大，为37.2%，其次为燃煤源及燃油源，分别为35.6%、27.2%。排放清单法可能低估了非化石源对SIA的贡献，在珠三角地区低估值约为10%。清洁大气时期燃油对SIA的贡献显著高于轻度污染与重度污染时期，最高可达48.4%。

关键词: 珠三角, PM_2.5, 二次无机气溶胶, 氮同位素, 硫同位素, 贝叶斯模型

Abstract:

Secondary inorganic aerosol (SIA) is an important element of PM_2.5, and its rapid formation is a significant cause of the decline of atmospheric visibility. Sulfate, nitrate and ammonium ions primarily constitute secondary inorganic aerosols, which have a wide range of sources and complex generation pathways, making it challenging to quantify their origins. Recently, stable isotopes (δ³⁴S-SO₄²⁻, δ¹⁵N-NO₃⁻, δ¹⁸O-NO₃⁻, δ¹⁵N-NH₄⁺) have been used to determine the sources of corresponding pollutants through source apportionment. In this study, we collected atmospheric PM_2.5 samples for one year at the Pearl River Delta Heshan Atmospheric Supersite. Based on the analysis of 70 samples, including water-soluble ions, trace metal elements, organic carbon and elemental carbon, we selected 37 samples for further isotopic analysis ( δ³⁴S-SO₄²⁻, δ¹⁵N-NO₃⁻, δ¹⁸O-NO₃⁻ and δ¹⁵N-NH₄⁺). We combined stable isotope balance and Bayesian model to quantify the relative contribution of various pollution sources to secondary inorganic aerosols. The results showed that the annual average PM_2.5 mass concentration was 39.8μg•m⁻³, with total SIA accounting for 29.8% of the annual average PM_2.5 mass concentration. Seasonal variation patterns showed that spring> winter>summer>autumn, with a significant decrease in winter compared to that in 2013. The order of contribution of SIA to particle mass concentration was sulfate>nitrate>ammonium. The δ³⁴S-SO₄²⁻ values ranged from 1.8‰ to 9.6‰, with an average of 4.5‰±1.7‰. The results of source apportionment showed that coal combustion, oil combustion and biogenic sulfur accounted for 41.8%, 32.9% and 25.3% respectively of SO₄²⁻ in Heshan. The δ¹⁵N-NO₃⁻ values ranged from 0.8‰ to 8.3‰, with an average of 4.7‰±2.0‰. The Bayesian isotope mixing model revealed that coal combustion was the main source of NO₃⁻ in Heshan, with an average annual contribution rate of 41.6%. The relative contribution of other pollution sources was ranked as biomass burning (BB)>gasoline vehicle>ship emission>biogenic soil emission, with percentages of 20.9%, 15.6%, 13.9% and 8.0%, respectively. The combined results of SIA analysis and source apportionment showed that non-fossil source contributed the most to total SIA (37.2%), followed by coal combustion (35.6%) and oil combustion (27.2%). The contribution of oil combustion to SIA was higher in the clean atmosphere period (up to 48.4%) than in the light and heavy pollution periods. The emission inventory method may have underestimated the contribution of non-fossil sources to SIA, by approximately 10% in the PRD region. Overall, the findings highlight the significance of non-fossil sources and the varying contribution of oil combustion to SIA.

Key words: Pearl River Delta, PM_2.5, secondary inorganic aerosol, nitrogen isotope, sulfur isotope, Bayesian model

中图分类号:

Q948
X17

温丽容, 林勃机, 李婷婷, 张子洋, 张正恩, 江明, 周炎, 张涛, 李军, 张干. 基于多同位素的珠三角PM_2.5中二次无机气溶胶来源解析[J]. 生态环境学报, 2023, 32(9): 1654-1662.

WEN Lirong, LIN Boji, LI Tingting, ZHANG Ziyang, ZHANG Zhengen, JIANG Ming, ZHOU Yan, ZHANG Tao, LI Jun, ZHANG Gan. Source Apportionment of Ammonium in Atmospheric PM_2.5 in the Pearl River Delta Based on Nitrogen Isotope[J]. Ecology and Environment, 2023, 32(9): 1654-1662.

图/表 9

图1 各季节SIA对PM2.5贡献占比

Figure 1 Proportion of secondary inorganic aerosols in PM2.5

图2 采样期间SIA对PM2.5贡献占比变化与PM2.5质量浓度变化

Figure 2 Changes in the proportion of secondary inorganic aerosols in PM2.5 and the time series of PM2.5 concentration during the sampling period

表1 采样期间PM2.5中SIA质量浓度

Table 1 Concentration of SIA in PM2.5 during the sampling period μg•m−3

统计项目	PM_2.5	NO₃⁻	SO₄²⁻	NH₄⁺
平均值	39.8	4.45	4.96	2.85
标准差	22.6	4.97	2.88	2.22
最小值	11.6	0.34	0.86	0.07
最大值	109	28.1	13.0	10.9

表2 采样期间鹤山SIA对PM2.5质量浓度相对贡献

Table 2 Relative contribution of SIA to PM2.5 mass concentration in Heshan during the sampling period %

采样时段	SIA/PM_2.5	NO₃⁻/PM_2.5	SO₄²⁻/PM_2.5	NH₄⁺/PM_2.5
全年	29.8	9.5	13.5	6.8
春季	36.9	12.9	14.8	9.1
夏季	26.6	6.2	15.5	5.0
秋季	26.3	7.1	12.8	6.5
冬季	30.1	12.7	10.8	6.7

表3 采样期间鹤山SO42−主要来源占比

Table 3 Source apportionments of sulfate aerosols in Heshan during the sampling period %

采样时段	燃煤	燃油	生物成因硫
全年	41.8±5.76	32.9±9.3	25.3±4.2
春季	37.5±5.2	39.7±9.5	22.8±4.9
夏季	32.9±8.6	45.3±11.0	21.8±2.3
秋季	45.7±2.4	26.5±4.5	27. 8±3.0
冬季	44.5±3.2	29.1±4.5	26.4±2.6

表4 采样期间鹤山NO3−主要来源占比

Table 4 Source apportionments of nitrate aerosols in Heshan during the sampling period %

采样时期	船舶	汽油车	生物质燃烧	燃煤	土壤微生物
全年	13.9±3.0	15.6±2.7	20.9±1.5	41.6±9.4	8.0±2.4
春季	12.7±2.9	14.7±2.5	20.6±1.7	44.9±8.9	7.1±2.0
夏季	14.6±3.2	16.4±2.5	21.6±0.7	39.0±9.0	8.4±2.6
秋季	15.3±2.3	16.9±2	21.6±1.0	37.2±6.9	8.9±1.8
冬季	13.5±3.6	15.0±3.3	20.5±1.8	43.0±11.5	8.0±3.2

表5 采样期间鹤山SIA的主要污染源占比

Table 5 Relative contribution of various pollution sources to SIA in Heshan during the sampling period %

采样时段	燃煤	燃油	非化石源
全年	35.6	27.2	37.2
春季	33.7	29.0	37.3
夏季	29.9	37.6	32.5
秋季	36.5	24.7	38.8
冬季	38.1	25.9	36.0

图3 中国典型区域基于同位素方法和排放清单方法的非化石源对SIA贡献对比

Figure 3 Comparison of non-fossil source contributions to SIA based on isotope and emission inventory methods in typical regions of China

图4 采样期间鹤山不同PM2.5污染程度下燃油对SIA的相对贡献

Figure 4 Boxplot of the relative contribution of oil combustion to SIA under different PM2.5 pollution stages in Heshan during the sampling period

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基于多同位素的珠三角PM_2.5中二次无机气溶胶来源解析

Source Apportionment of Ammonium in Atmospheric PM_2.5 in the Pearl River Delta Based on Nitrogen Isotope

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基于多同位素的珠三角PM2.5中二次无机气溶胶来源解析

Source Apportionment of Ammonium in Atmospheric PM2.5 in the Pearl River Delta Based on Nitrogen Isotope

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基于多同位素的珠三角PM_2.5中二次无机气溶胶来源解析

Source Apportionment of Ammonium in Atmospheric PM_2.5 in the Pearl River Delta Based on Nitrogen Isotope