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Component characteristics and formation mechanism of carbonyl compounds in the atmosphere during a typical pollution period in Jinan urban area |
YAN Huai-zhong1,2, WANG Jie1, SHI Jing-hua2, CAO Yan-yan2, YOU Xi-hua2, WEI Xiao-feng1, LIU Shi-jie3, ZHANG Gui-qin1 |
1. School of Municipal and Environmental Engineering, Shandong Jianzhu University, Jinan 250101, China; 2. Shandong Provincial Eco-Environment Monitoring Center, Jinan 250101, China; 3. Resources and Environment Innovation Institute, Shandong Jianzhu University, Jinan 250101, China |
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Abstract Carbonyl compounds in the atmosphere at two different urban sites (Jianda and Chuangyeyuan) of Jinan were synchronously collected using 2,4-dinitrophenylhydrazine sampling tubes during a typical summer ozone pollution period (from June 14 to 22, 2022) and quantified using high-performance liquid chromatography. The photochemical reactions of major carbonyls were simulated with the Observation-based model (OBM) to identify the secondary formation pathways and critical precursors of these carbonyl compounds. The total concentration of carbonyl compounds was (19.78±9.83)×10-9 of which formaldehyde, acetaldehyde, and acetone accounted for 36.75%, 21.39% and 14.64%, respectively. The formaldehyde concentration showed "double peak" characteristics at noon and night in Jianda and had a peak change in morning and evening in Chuangyeyuan, exhibiting relatively higher concentrations at night and minimal concentrations around noontime. The concentration ratios of formaldehyde to acetaldehyde (C1/C2) of the two urban sites were 1.97 and 1.47, respectively. The concentration ratios of acetaldehyde to propionaldehyde (C2/C3) of the two sites were 9.27 and 8.76, respectively. The maximum formation rate was simulated to be 6.17×10-9h-1 for formaldehyde, 1.67×10-9h-1 for acetaldehyde, and 0.66×10-9h-1 for acetone; and the alkoxy radical (RO)+O2 reaction was the main secondary formation pathway. We also observed that alkene had an important effect on the secondary formation of formaldehyde and acetaldehyde in the atmosphere; and ethylene, isoprene, and propylene were important precursors of formaldehyde, while propylene and 2-butylene served as precursors of acetaldehyde. Obviously, effectively controlling artificial alkene emissions from industries will help mitigate the secondary formation of major carbonyl compounds in the atmosphere.
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Received: 26 June 2023
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|
|
|
|
[1] |
Atkinson R.Atmospheric chemistry of VOCs and NOx [J].Atmospheric Environment, 1998,34(12-14):2063-2101.
|
[2] |
李元昭,李少华,张成龙,等.北京市大兴区夏季大气中醛酮类化合物的污染水平、来源及影响[J].环境化学, 2021,40(7):1999-2015.Li Y Z, Li S H, Zhang C L, et al.The pollution levels, sources and impact of atmospheric carbonyls in summer of Daxing District, Beijing [J].Environmental Chemistry, 2021,40(7):1999-2015.
|
[3] |
Qian X, Shen H, Chen Z.Characterizing summer and winter carbonyl compounds in Beijing atmosphere [J].Atmospheric Environment, 2019,214:116845.
|
[4] |
Altemose B, Gong J, Zhu T, et al.Aldehydes in relation to air pollution sources:A case study around the Beijing Olympics [J].Atmospheric Environment, 2015,109:61-69.
|
[5] |
王伯光,刘灿,吕万明,等.广州大气挥发性醛酮类化合物的污染特征及来源研究[J].环境科学, 2009,30(3):631-636.Wang B G, Liu C, Lv W M, et al.Character of volatile carbonyl compounds and source in Guangzhou ambient air [J].Environmental Science, 2009,30(3):631-636.
|
[6] |
谢顺涛,巨天珍,葛建团,等.基于卫星遥感中国甲醛的时空分布及影响因子[J].中国环境科学, 2018,38(5):1677-1684.Xie S T, Ju T Z, Ge J T, et al.Spatial and temporal distribution and related factors analysis of formaldehyde in China, based on satellite remote sensing [J].China Environmental Science, 2018,38(5):1677-1684.
|
[7] |
咸龙,葛建团,徐敏,等.珠江三角洲对流层HCHO柱浓度遥感监测及影响因子[J].中国环境科学, 2018,38(9):3221-3231.Xian L, Ge J T, Xu M, et al.Remote sensing monitoring of tropospheric HCHO column concentration and influential factors over pearl river delta China [J].China Environmental Science, 2018,38(9):3221-3231.
|
[8] |
程婧晨,崔彤,何万清,等.北京市典型餐饮企业油烟中醛酮类化合物污染特征[J].环境科学, 2015,36(8):2743-2749.Cheng Q C, Cui T, He W Q, et al.Pollution characteristics of aldehydes and ketones compounds in the exhaust of Beijing typical restaurants [J].Environmental Science, 2015,36(8):2743-2749.
|
[9] |
彭华.城市大气环境中醛酮类化合物污染状况及变化规律[J].环境监测管理与技术, 2011,23(1):39-41.Peng H.Research on aldehydes and ketones pollutions in urban air [J].The Administration and Technique of Environmental Monitoring, 2011,23(1):39-41.
|
[10] |
黄娟,冯艳丽,傅家谟,等.植物排放的羰基化合物及其与大气的交换[J].生态环境, 2008,17(1):428-433.Huang J, Feng Y L, Fu J M, et al.The researches of carbonyl compounds in the atmosphere and its exchange between plants and the atmosphere [J].Ecology and Environment, 2008,17(1):428-433.
|
[11] |
Cheng Y, Lee S C, Huang Y, et al.Diurnal and seasonal trends of carbonyl compounds in roadside, urban, and suburban environment of Hong Kong [J].Atmospheric Environment, 2014,89:43-51.
|
[12] |
林宜玲,洪有为,纪晓婷,等.沿海城市秋季大气甲醛污染来源及其环境影响[J].中国环境科学, 2023,43(1):52-60.Lin Y L, Hong Y W, Ji X T, et al.Pollution characteristics of atmospheric formaldehyde (HCHO) and its environmental effects in autumn in a coastal city [J].China Environmental Science, 2023,43(1):52-60.
|
[13] |
黄海滨,成海容,胡柯,等.武汉市夏季典型光化学污染过程中二羰基化合物的污染特征及来源[J].中国环境科学, 2023,43(10):5114-5122.Huang H B, Cheng H R, Hu K, et al.Characteristics and sources of dicarbonyl compounds during summer photochemical pollution episodes in Wuhan [J].China Environmental Science, 2023,43(10):5114-5122.
|
[14] |
Wang J, Chen S, Qiu X, et al.Pollution characteristics of atmospheric carbonyl compounds in a large city of Northern China [J].Journal of Chemistry, 2022,vol.2022:1-13.
|
[15] |
冯旸,刘锐源,刘雷璐,等.广州典型印刷企业VOCs排放特征及环境影响和健康风险评价[J].中国环境科学, 2020,40(9):3791-3800.Feng Y, Liu R Y, Liu L L, et al.VOCs emission characteristics, environmental impact and health risk assessment of typical printing enterprises in Guangzhou [J].China Environmental Science, 2020, 40(9):3791-3800.
|
[16] |
Xue L, Wang T, Wang X, et al.On the use of an explicit chemical mechanism to dissect peroxy acetyl nitrate formation [J].Environmental Pollution, 2014,195:39-47.
|
[17] |
丁萌萌,周健楠,常淼,等.北京大气中醛酮化合物污染特征与来源分析[J].环境科学研究, 2023,36(6):1095-1106.Ding M M, Zhou J N, Chang M, et al.Pollution characterization and source analyses of carbonyls in the ambient air in Beijing [J].Research of Environmental Sciences, 2023,36(6):1095-1106.
|
[18] |
黄禹,陈曦,王迎红,等.华北区域大气中羰基化合物体积分数水平及化学反应活性[J].环境科学, 2021,42(10):4602-4610.Huang Y, Chen X, Wang Y H, et al.Concentration and reactivityof carbonyl compounds in the atmosphere of North China [J].Environmental Science, 2021,42(10):4602-4610.
|
[19] |
陈丰,段玉森,冯艳丽,等.上海地区2017年夏季大气中羰基化合物的空间分布特征[J].上海大学学报, 2021,27(1):86-96.Chen F, Duan Y S, Feng Y L, et al.Spatial distribution of atmospheric carbonyl compounds in the Summer of 2017, Shanghai Area [J].Journal of Shanghai University, 2021,27(1):86-96.
|
[20] |
Chen T S, Zheng P G, Zhang Y N, et al.Characteristics and formation mechanisms of atmospheric carbonyls in an oilfield region of northern China [J].Atmospheric Environment, 2022,vol.274:118958.
|
[21] |
Liu Y, Yuan B, Li X, et al.Impact of pollution controls in Beijing on atmospheric oxygenated volatile organic compounds (OVOCs) during the 2008 Olympic Games:observation and modeling implications [J].Atmospheric Chemistry and Physics, 2015,15(6):3045-3062.
|
[22] |
张崇旭.京津冀污染传输通道大气醛酮化合物的污染特征、来源及反应活性研究[D].济南:山东建筑大学, 2019.Zhang C X.Pollution characteristics, sources and reactivity of atmospheric carbonyl compounds in the Beijing-Tianjin-Hebei air pollution transmission channel area [D].Jinan:Shangdong Jianzhu University, 2019.
|
[23] |
Rao Z, Chen Z, Liang H, et al.Carbonyl compounds over urban Beijing:Concentrations on haze and non-haze days and effects on radical chemistry [J].Atmospheric Environment, 2016,124:207-216.
|
[24] |
Yang X, Xue L, Wang T, et al.Observations and explicit modeling of summertime carbonyl formation in Beijing:Identification of key precursor species and their impact on atmospheric oxidation chemistry [J].Journal of Geophysical Research:Atmospheres, 2018,123(2):1426-1440.
|
[25] |
Yang X, Zhang G, Sun Y, et al.Explicit modeling of background HCHO formation in southern China [J].Atmospheric Research, 2020, 240:104941.
|
[26] |
孙晓艳,赵敏,申恒青,等.济南市城区夏季臭氧污染过程及来源分析[J].环境科学, 2022,43(2):686-695.Sun X Y, Zhao M, Shen H Q, et al.Ozone Formation and Key VOCs of a Continuous Summertime O3 Pollution Event in Ji'nan [J].Environmental Science, 2022,43(2):686-695.
|
[27] |
钱韵,吴健生,谭羲,等.长三角对流层甲醛柱浓度时空变化及驱动因素[J].中国环境科学, 2021,41(11):4973-4981.Qian Y, Wu J S, Tan X, et al.Spatiotemporal variation of tropospheric formaldehyde concentration and its driving factors in Yangtze River [J].China Environmental Science, 2021,41(11):4973-4981.
|
[28] |
Chen T, Xue L, Zheng P, et al.Volatile organic compounds and ozone air pollution in an oil production region in northern China [J].Atmospheric Chemistry and Physics, 2020,20(11):7069-7086.
|
[29] |
HJ 683-2014环境空气醛、酮类化合物的测定高效液相色谱法[S].HJ 683-2014 Ambient air-Determination of aldehyde and ketone compounds-High performance liquid chromatography [S].
|
[30] |
张鑫,李红,张成龙,等.环境空气中醛酮类化合物检测方法优化与初步应用[J].环境科学研究, 2019,32(5):821-829.Zhang X, Li H, Zhang C L, et al.Optimization and preliminary application of the detection method of carbonyl compounds in the ambient air [J].Research of Environmental Sciences, 2019,32(5):821-829.
|
[31] |
司利国,邢冠华,王超,等.高效液相色谱法测定环境空气醛酮类化合物[J].环境化学, 2019,38(10):2222-2228.Si L G, Xing G H, Wang C, et al.Determination of aldehydes and ketones in ambient air using adsorbent cartridge followed by high performance liquid chromatography [J].Environmental Chemistry, 2019,38(10):2222-2228.
|
[32] |
黄敏,马飞攀,张济龙,等.环境中醛酮类羰基化合物分析方法研究进展[J].四川环境, 2023,42(1):300-305.Huang M, Ma F P, Zhang J L, et al.Research progress of the environmental monitoring analytical methods of aldehydes and ketones carbonyl compounds [J].Sichuan Environment, 2023,42(1):300-305.
|
[33] |
张英南,薛丽坤,陈天舒,等.基于观测的模型(OBM)的发展历程及其在我国大气化学研究中的应用与展望[J].环境科学研究, 2022, 35(3):621-632.Zhang Y N, Xue L K, Chen T S, et al.Development History of Observation-Based Model (OBM) and Its Application and Prospect in Atmospheric Chemistry Studies in China [J].Research of Environmental Sciences, 2022,35(3):621-632.
|
[34] |
Saunders S M, Jenkin M E, Derwent R G, et al.Protocol for the development of the Master Chemical Mechanism, MCM v3(Part A):tropospheric degradation of non-aromatic volatile organic compounds [J].Atmospheric Chemistry and Physics, 2003,3(1):161-180.
|
[35] |
Xue L K, Wang T, Guo H, et al.Sources and photochemistry of volatile organic compounds in the remote atmosphere of western China:results from the Mt.Waliguan Observatory [J].Atmospheric Chemistry and Physics, 2013,13(17):8551-8567.
|
[36] |
吴琳,薛丽坤,王文兴.基于观测的臭氧污染研究方法[J].地球环境学报, 2017,8(6):479-491.Wu L, Xue L K, Wang X W.Review on the observation-based methods for ozone air pollution research [J].Journal of Earth Environment, 2017,8(6):479-491.
|
[37] |
Yang Z, Cheng H R, Wang Z W, et al.Chemical characteristics of atmospheric carbonyl compounds and source identification of formaldehyde in Wuhan, Central China [J].Atmospheric Research, 2019,228:95-106.
|
[38] |
李世杰.淄博市大气羰基化合物的污染特征、来源及臭氧生成敏感性分析[D].北京:中国环境科学研究院, 2021.Li S J.Characteristics, sources of carbonyl compounds and analysis of ozone formation sensitivity in Zibo city [D].Bei Jing:Chinese Research Academy of Environmental Sciences, 2021.
|
[39] |
李明芳,马小杰.临沂市夏季大气中醛酮类化合物的污染状况研究[J].四川环境, 2022,41(5):97-103.Li M F, Ma X J.Study on the pollution status of ambient aldehydes and ketones in Linyi city in summer [J].Sichuan Environment, 2022, 41(5):97-103.
|
[40] |
郑玄,蒋朝晖,翟海晴,等.长沙市大气中醛酮类化合物浓度变化特征[J].中国环境监测, 2019,35(3):93-99.Zheng X, Jiang Z H, Zhai H Q, et al.Variation characteristics of atmospheric carbonyl compounds in Changsha [J].Environmental Monitoring in China, 2019,35(3):93-99.
|
[41] |
周雪明,谭吉华,项萍,等.佛山市冬夏季羰基化合物污染特征[J].中国环境科学, 2017,37(3):844-850.Zhou X M, Tan J H, Xiang P, et al.Chemical characteristics of atmospheric carbonyls in winter and summer in Foshan City [J].China Environmental Science, 2017,37(3):844-850.
|
[42] |
王楚涵,张鑫,吴鸣,等.沈阳市郊区环境空气中醛酮类化合物的污染特征与来源分析[J].环境科学研究, 2020,33(12):2771-2784.Wang C H, Zhang X, Wu M, et al, Pollution Characterization and Source Analyses of Carbonyls in the Ambient Air in a Suburban Area of Shenyang [J].Research of Environmental Sciences, 2020,33(12):2771-2784.
|
[43] |
梁文萍.石化企业典型区域VOCs污染特征及来源解析[J].现代化工, 2019,39(9):5-10.Liang W P.Pollution characteristics and source of VOCs in typical areas of petrochemical enterprises [J].Modern Chemical Industry, 2019,39(9):5-10.
|
[44] |
马磊,孟凡伟.石化企业VOCs重点排放源排放特征及物质清单的研究[J].当代化工, 2019,48(12):2750-2753.Ma L, Meng F W.Study on emission characteristics and material list of VOCs key emission sources in petrochemical enterprises [J].Contemporary Chemical Industry, 2019,48(12):2750-2753.
|
[45] |
王成辉,陈军辉,韩丽,等.成都市城区大气VOCs季节污染特征及来源解析[J].环境科学, 2020,41(9):3951-3960.Wang C H, Chen J H, Han L, et al.Seasonal pollution characteristics and analysis of the sources of atmospheric VOCs in Chengdu urban area [J].Environmental Science, 2020,41(9):3951-3960.
|
[46] |
吴飞,庞小兵,卢钰,等.杭州及绍兴大气中羰基化合物的污染特征、来源及影响[J].环境化学, 2023,42(6):1825-1835.Wu F, Pang X B, Lu Y, et al.The pollution levels, sources and impact of carbonyls in Hangzhou and Shaoxing atmosphere [J].Environmental Chemistry, 2023,42(6):1825-1835.
|
[47] |
景盛翱.上海市典型区域大气羰基化合物水平研究[J].环境污染与防治, 2017,39(7):713-716.Jing S A.Study on the level of ambient carbonly compounds in typical regions of Shanghai [J].Environmental Pollution & Control, 2017, 39(7):713-716.
|
[48] |
畅云霞,李凡修,陈炫.太原市冬、夏季醛酮化合物污染特征及来源分析[J].中国环境监测, 2022,38(2):37-45.Chang Y X, Li F X, Chen X.Pollution characteristics and sources of aldehydes and ketones in winter and summer in Taiyuan [J].Environmental Monitoring in China, 2022,38(2):37-45.
|
[49] |
霍瑞娜,王文红,刘敏,等.濮阳市夏季环境空气中醛酮类化合物污染特征及臭氧生成潜势分析[J].广东化工, 2020,47(20):71-72.Huo R N, Wang W H, Liu M, et al.Study on the pollution characteristics and ozone formation potential of carbonyl compounds in the ambient air of Puyang in summer [J].Guangdong Chemical Industry, 2020,47(20):71-72.
|
[50] |
蒋朝晖,王玉娇,郑玄,等.张家界森林大气中醛酮类化合物浓度变化特征[J].环境科学研究, 2016,29(9):1272-1278.Jiang Z H, Wang Y J, Zheng X, et al.Variation characteristics of atmospheric carbonyl compounds in Zhangjiajie Forest [J].Research of Environmental Sciences, 2016,29(9):1272-1278.
|
[51] |
胡崑,王鸣,王红丽,等.基于PMF和源示踪物比例法的大气羰基化合物来源解析:以南京市观测为例[J].环境科学, 2021,42(1):45-54.Hu K, Wang M, Wang H L,et al.Source apportionment of ambient carbonyl compounds based on a PMF and source tracer ratio method:A case based on observations in Nanjing [J].Environmental Science, 2021,42(1):45-54.
|
[52] |
韩恒霄,夏士勇,罗遥,等.深圳市大气甲醛四季污染特征及来源解析[J].中国环境科学, 2023,43(8):3867-3876.Han H X, Xia S Y, Luo Y, et al.Four seasons pollution characteristics and source analysis of atmospheric formaldehyde in Shenzhen [J].China Environmental Science, 2023,43(8):3867-3876.
|
[53] |
冯艳丽,陈颖军,文晟,等.广州东站室内停车场空气中羰基化合物调查[J].环境污染与防治, 2006,28(11):863-875.Feng Y L, Chen Y J, Wen S, et al.A survery of carbonyl compounds in the indoor parking lot in the east rail way station of Guangzhou [J].Environmental Pollution and control, 2006,28(11):863-875.
|
[54] |
廖彤,林玉君,季文浩,等.珠江三角洲光化学活跃期甲醛及其前体物的源解析研究[J].中国环境科学, 2022,42(12):5533-5541.Liao T, Lin Y J, Ji W H, et al.Research on the sources of formaldehyde and its precursors during the active period of atmospheric photochemistry in the Pearl River Delta [J].China Environmental Science, 2022,42(12):5533-5541.
|
[55] |
杨帆,闫雨龙,戈云飞,等.晋城市冬季环境空气中挥发性有机物的污染特征及来源解析[J].环境科学, 2018,39(9):4042-4050.Yang F, Yan Y L, Ge Y F, et al.Characteristics and source apportionment of ambient volatile organic compounds in winter in Jincheng [J].Environmental Science, 2018,39(9):4042-4050.
|
[56] |
张玉欣,安俊琳,王俊秀,等.南京工业区挥发性有机物来源解析及其对臭氧贡献评估[J].环境科学, 2018,39(2):502-510.Zhang Y X, An J L, Wang J X, et al.Source analysis of volatile organic compounds in the Nanjing industrial area and evaluation of their contribution to ozone [J].Environmental Science, 2018,39(2):502-510.
|
[57] |
叶露,邰菁菁,俞华明.汽车工业区大气挥发性有机物(VOCs)变化特征及来源解析[J].环境科学, 2021,42(2):624-633.Ye L, Tai Q Q, Yu H M.Characteristics and Source Apportionment of Volatile Organic Compounds(VOCs) in the Automobile Industrial Park of Shanghai [J].Environmental Science, 2021,42(2):624-633.
|
[58] |
卢立栋,王浩,李媛媛.关中地区典型煤化工行业VOCs排放系数与特征研究[J].煤化工, 2022,50(4):15-20.Lu L D, Wang H, Li Y Y.Study on VOCs emission factor and characteristics of typical coal chemical industry in Guanzhong area [J].Coal Chemical Industry, 2022,50(4):15-20.
|
[59] |
徐晨曦,陈军辉,韩丽,等.四川省典型行业挥发性有机物源成分谱[J].环境科学, 2020,41(7):3031-3041.Xu C X, Chen J H, Han L, et al.Source composition spectrum of volatile organic compounds in typical industries in Sichuan [J].Environmental Science, 2020,41(7):3031-3041.
|
|
|
|