上海市亚微米颗粒物中有机胺的浓度与组成特征

doi:10.16258/j.cnki.1674-5906.2022.10.010

生态环境学报 ›› 2022, Vol. 31 ›› Issue (10): 2019-2027.DOI: 10.16258/j.cnki.1674-5906.2022.10.010

上海市亚微米颗粒物中有机胺的浓度与组成特征

陈浩(), 张玉莹, 钟妍, 张世伟, 陈俊伟, 冯加良^*()

上海大学环境与化学工程学院，上海 200444

收稿日期:2020-04-15 出版日期:2022-10-18 发布日期:2022-12-09
通讯作者: ^*E-mail: fengjialiang@shu.edu.cn
作者简介:陈浩（1994年生），男，硕士研究生，研究方向为气溶胶化学。E-mail: 964099816@qq.com
基金资助:
国家自然科学基金项目(41877373);国家自然科学基金项目(41473088)

Concentration and Composition of Organic Amines in PM₁ in Shanghai

CHEN Hao(), ZHANG Yuying, ZHONG Yan, ZHANG Shiwei, CHEN Junwei, FENG Jialiang^*()

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P. R. China

Received:2020-04-15 Online:2022-10-18 Published:2022-12-09

摘要/Abstract

摘要：

有机胺是大气细颗粒中一类重要的碱性含氮有机物，可能在大气新粒子生成和二次有机气溶胶形成过程中起着重要作用，但我们对大气细颗粒物中有机胺浓度和组成的了解还很缺乏。为了解上海市亚微米颗粒物（PM₁）中有机胺的浓度、组成及潜在来源，在上海大学宝山校区于2017年6月—2018年5月采集了65个PM₁样品，采用苯磺酰氯（BSC）衍生化和气相色谱-质谱联用仪（GC-MS）检测方法定量分析了甲胺（MA）、二甲胺（DMA）、乙胺（EA）、二乙胺（DEA）、丙胺（PA）和丁胺（BA）6种低分子脂肪胺的浓度，并通过相关性分析、主成分分析及气团后向轨迹分析探讨了有机胺的潜在来源。结果表明，采样期间上海PM₁中6种有机胺总质量浓度为4.60—132.98 ng·m^-3，年平均质量浓度为46.49 ng·m^-3；甲胺、二甲胺、乙胺和二乙胺是主要的有机胺单体，占6种有机胺总浓度的97%，其中甲胺的年均占比为51.3%。PM₁中有机胺总浓度呈现较明显的季节性变化：夏季>秋季>春季≈冬季；MA在有机胺总浓度中的占比夏季最高、冬季最低，而DMA和DEA的相对贡献冬季最高、夏天最低。有机胺总浓度与SO₄^2-浓度之间在不同季节均存在显著正相关关系，而与NO₃^-之间仅在冬季和夏季显著相关，说明有机胺可能主要与硫酸根结合。有机胺单体之间的相关性分析以及结合主要水溶性组分的主成分分析表明这些有机胺单体可能来自相似的排放源，但不同单体浓度的季节变化不同，说明不同季节有机胺的来源有一定的差别，二次生成及生物质燃烧可能不是上海PM₁中有机胺的主要来源。后向轨迹聚类分析显示，有机胺主要受本地排放源的影响，外来传输以及海洋源可能有一定的影响，但不是主要的来源。研究结果能为大气细颗粒物环境影响评价提供重要的基础数据。

关键词: PM₁, 有机胺, GC-MS, 上海

Abstract:

Organic amines are an important group of alkaline nitrogen-containing compounds in the atmospheric fine particles, which may play an important role in the formation of new particles and secondary organic aerosols. However, data on the concentration and composition of organic amines in the atmospheric fine particles is still very limited. In order to understand the compositional characteristics and potential sources of organic amines in the sub-micron particles (PM₁) in Shanghai, 65 PM₁ samples were collected at the Baoshan campus of Shanghai University from June 2017 to May 2018. Six low molecular weight aliphatic amines including methylamine (MA), dimethylamine (DMA), ethylamine (EA), diethylamine (DEA), propylamine (PA) and butylamine (BA) were measured using a gas chromatography-mass spectrometer (GC-MS) after derivatization with benzenesulfonyl chloride (BSC). Correlation analysis, principal component analysis (PCA) and air parcel backward trajectory analysis were used to investigate the potential sources of amines. Results showed that the total concentration of six organic amines (Ʃamines) in PM₁ in Shanghai was 4.60-132.98 ng·m^-3, with an annual average of 46.49 ng·m^-3. Methylamine, dimethylamine, ethylamine and diethylamine were the main individual amines, accounting for 97% of the Ʃamines annually, among which methylamine alone accounted for 51%. The concentration of Ʃamines showed a distinct seasonal trend of summer>autumn>spring≈winter. The contribution of MA to Ʃamines was the highest in summer and the lowest in winter, whereas for DMA and DEA it was the highest in winter and the lowest in summer. Significant correlations were found in all seasons between Ʃamines and sulfate, but the significant correlation between Ʃamines and nitrate was only found in winter and summer, suggesting that amines might mainly combine with sulfate. The correlation analysis between the individual amines combined with the PCA analysis of amines and the main water-soluble components showed that different individual amines might come from similar emission sources, but the emission sources of amines in different seasons would be different to some extent, and secondary formation and biomass burning might not be the main sources of amines in PM₁ in Shanghai. Cluster analysis of the backward trajectories of air parcels arriving in Shanghai showed that the concentration of the organic amines in PM₁ in Shanghai was mainly affected by local emissions, and long distance transport and marine emissions were not the main sources. The results could provide important data for the environmental impact assessment of the atmospheric fine particles.

Key words: PM₁, organic amines, GC-MS, Shanghai

中图分类号:

X131.1
X51

陈浩, 张玉莹, 钟妍, 张世伟, 陈俊伟, 冯加良. 上海市亚微米颗粒物中有机胺的浓度与组成特征[J]. 生态环境学报, 2022, 31(10): 2019-2027.

CHEN Hao, ZHANG Yuying, ZHONG Yan, ZHANG Shiwei, CHEN Junwei, FENG Jialiang. Concentration and Composition of Organic Amines in PM₁ in Shanghai[J]. Ecology and Environment, 2022, 31(10): 2019-2027.

图/表 10

参考文献 44

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季节 Season	有机胺质量浓度 ∑ρ(amines)/ (ng·m^-3)	PM₁质量浓度 ρ(PM₁)/ (μg·m^-3)	有机胺/PM₁ ∑ρ(amines)/ ρ(PM₁)
春季 Spring (n=17)	40.57±27.55	26.07±10.76	0.16%
夏季 Summer (n=18)	53.81±38.44	22.01±9.06	0.24%
秋季 Autumn (n=18)	45.79±24.07	22.19±9.06	0.21%
冬季 Winte r(n=12)	40.65±22.54	44.09±18.40	0.09%

季节 Season	有机胺质量浓度 ∑ρ(amines)/ (ng·m^-3)	PM₁质量浓度 ρ(PM₁)/ (μg·m^-3)	有机胺/PM₁ ∑ρ(amines)/ ρ(PM₁)
春季 Spring (n=17)	40.57±27.55	26.07±10.76	0.16%
夏季 Summer (n=18)	53.81±38.44	22.01±9.06	0.24%
秋季 Autumn (n=18)	45.79±24.07	22.19±9.06	0.21%
冬季 Winte r(n=12)	40.65±22.54	44.09±18.40	0.09%

有机胺 ρ(Amine)	春季 Spring (n=17)	夏季 Summer (n=18)	秋季 Autumn (n=18)	冬季 Winter (n=12)	全年 Annual (n=65)	夏季/冬季 Summer/Winter
甲胺 ρ(MA)	21.52±16.36	31.28±25.03	22.65±14.21	14.34±6.31	22.45±18.54	2.2
二甲胺 ρ(DMA)	9.51±7.32	7.87±4.81	9.98±5.57	10.12±3.94	9.37±5.74	0.8
乙胺 ρ(EA)	2.67±1.90	5.26±3.93	3.99±2.27	3.46±1.84	3.85±2.88	1.5
二乙胺 ρ(DEA)	5.84±3.18	7.71±5.08	7.82±3.86	6.31±3.25	6.92±4.09	1.2
丙胺 ρ(PA)	0.15±0.13	0.20±0.13	0.21±0.09	0.22±0.11	0.20±0.16	0.9
丁胺 ρ(BA)	0.89±0.72	1.47±1.08	1.13±0.83	0.56±0.41	1.01±0.89	2.6

有机胺 ρ(Amine)	春季 Spring (n=17)	夏季 Summer (n=18)	秋季 Autumn (n=18)	冬季 Winter (n=12)	全年 Annual (n=65)	夏季/冬季 Summer/Winter
甲胺 ρ(MA)	21.52±16.36	31.28±25.03	22.65±14.21	14.34±6.31	22.45±18.54	2.2
二甲胺 ρ(DMA)	9.51±7.32	7.87±4.81	9.98±5.57	10.12±3.94	9.37±5.74	0.8
乙胺 ρ(EA)	2.67±1.90	5.26±3.93	3.99±2.27	3.46±1.84	3.85±2.88	1.5
二乙胺 ρ(DEA)	5.84±3.18	7.71±5.08	7.82±3.86	6.31±3.25	6.92±4.09	1.2
丙胺 ρ(PA)	0.15±0.13	0.20±0.13	0.21±0.09	0.22±0.11	0.20±0.16	0.9
丁胺 ρ(BA)	0.89±0.72	1.47±1.08	1.13±0.83	0.56±0.41	1.01±0.89	2.6

有机胺 Amine	甲胺 MA	二甲胺 DMA	乙胺 EA	二乙胺 DEA
甲胺 MA	1
二甲胺 DMA	0.690^**	1
乙胺 EA	0.840^**	0.671^**	1
二乙胺 DEA	0.677^**	0.652^**	0.772^**	1

上海市亚微米颗粒物中有机胺的浓度与组成特征

Concentration and Composition of Organic Amines in PM₁ in Shanghai

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采样地点 Sampling site	日期 Date	颗粒物粒径 Particle size	有机胺质量浓度 ρ(Amine)/(ng·m^-3)						分析方法Analysis method	参考文献 Reference
采样地点 Sampling site	日期 Date	颗粒物粒径 Particle size	甲胺MA	二甲胺 DMA	乙胺 EA	二乙胺 DEA	丙胺 PA	丁胺BA	分析方法Analysis method	参考文献 Reference
上海 Shanghai	Jun, 2017-May, 2018	PM₁	22.45	9.37	3.85	6.92	0.20	1.55	GC-MS	This study
上海 Shanghai	Jul, 2013-Aug, 2013	PM₁	7.7	13.4	9.7	—	—	—	IC	2016
上海 Shanghai	Jul, 2013-Aug, 2013	PM_2.5	3.89	—	0.26	—	0.11	0.39	HPLC	2016
广州 Guangzhou	Sep, 2014-Oct, 2014	PM₃	50.4	17.7	3.95	4.78	0.59	3.04	GC-MS	2017b
广州 Guangzhou	Oct, 2016-Nov, 2017	PM_2.5	56.1	45.5	—	9.17	—	—	GC-MS	2018
南京 Nanjing	Nov, 2017-Dec, 2018	PM_2.5	13.1	20.2	6.3	—	—	—	IC	2020
扬州 Yangzhou	Nov, 2015-Apr, 2016	PM_2.5	5.7	7.9	20.3	—	—	—	HPLC	2017
扬州 Yangzhou	Apr, 2016-Nov, 2016	PM_2.5	1.42	3.62	12.6	—	—	—	HPLC	2020
北京 Beijing	Jan, 2013-Feb, 2013	PM_2.5	31.0	4.3	14.8	2.1	—	—	HPLC	2016
西安 Xi’an	Jan, 2013-Feb, 2013	PM_2.5	24.7	3.8	12.6	2.0	—	—	HPLC	2016
厦门 Xiamen	Jan, 2013-Feb, 2013	PM_2.5	10.2	1.7	15.3	0.9	—	—	HPLC	2016
中国香港 Hong Kong, China	Jan, 2013-Feb, 2013	PM_2.5	12.1	1.5	4.5	0.9	—	—	HPLC	2016
黄海和渤海 The Yellow Sea and Bohai Sea of China	May, 2012	PM_1.1	—	121.7	—	—	—	—	IC	2015
中国东海 The East Sea of China	Aug, 2015	PM₁₀	—	41.9	—	—	—	—	IC	2016
土耳其 Turkey	Oct, 2006-Apr, 2007	PM_2.5	3.42	3.73	3.28	3.46	4.32	5.45	HPLC	2008
韩国 Korea	Mar, 2001-Apr, 2001		13.5	—	3.1	—	—	—	HPLC	2004
美国 USA	Jul, 2005-Aug, 2005	PM_2.5	—	31.0	—	—	—	—	IC	2007
美国 USA	Jul, 2012-Jul, 2013	PM₁	—	14.5	—	—	—	—	IC	2015

有机胺 Amine	季节 Season	硝酸根质量浓度c(NO₃^-)	硫酸根质量浓度 c(SO₄^2-)
总有机胺 ∑c(Amine)	春季 Spring(n=17)	0.269	0.586^*
	夏季 Summer(n=18)	0.510^*	0.547^*
	秋季 Autumn(n=18)	0.213	0.521^*
	冬季 Winter(n=12)	0.770^**	0.890^**

组分 Components	因子1 Factor 1	因子2 Factor 2	因子3 Factor 3	因子4 Factor 4
水溶性有机氮 WSON	0.614	0.315	-0.134	0.249
甲胺 MA	0.008	0.943	-0.049	0.065
二甲胺 DMA	0.451	0.732	0.092	-0.238
乙胺 EA	0.101	0.922	0.089	0.026
二乙胺DEA	0.252	0.806	0.073	0.059
氯离子 Cl^-	0.657	-0.157	0.533	0.005
硝酸根离子 NO₃^-	0.851	0.051	0.370	-0.139
硫酸根离子 SO₄^2-	0.663	0.423	0.071	0.307
钠离子 Na⁺	0.038	0.000	0.127	0.945
铵根离子 NH₄⁺	0.894	0.264	0.168	-0.099
钾离子 K⁺	0.752	0.148	0.390	0.063
钙离子 Ca²⁺	0.267	-0.102	0.864	0.025
镁离子 Mg²⁺	0.005	-0.043	0.800	0.015
方差百分比% of variance	25%	23%	22%	8%

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上海市亚微米颗粒物中有机胺的浓度与组成特征

Concentration and Composition of Organic Amines in PM1 in Shanghai

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Concentration and Composition of Organic Amines in PM₁ in Shanghai