珠三角典型地区气态氨分布及其对PM<sub>2.5</sub>贡献

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摘要为探讨珠三角典型地区气态氮(NH₃)对细颗粒物(PM_2.5)的贡献,于2022年6月~2023年5月,在珠三角地区四个代表性城市选择了三个城市站点和一个郊区站点开展了NH₃的在线监测,并同步收集了水溶性离子、HNO₃、PM_2.5以及气象参数等资料.此基础上分析了NH₃的浓度水平特征和日变化特征,进一步评估了NH₃对PM_2.5的潜在贡献.结果表明,公园前(GYQ)、梅华(MH)、东城(DC)和鹤山花果山(HGS)的NH₃年均值分别为(5.74±3.00),(4.70±2.41),(5.09±2.26)和(4.17±1.95)μg/m³,除GYQ外,其余三站点NH₃季节变化均表现出秋季>春季>夏季>冬季的趋势.NH₃浓度日变化规律与温度相近,与相对湿度相反.经由修正的气体比率(AdjGR)评估,四个站点均处于富氨的条件下.随着PM_2.5污染浓度的上升,AdjGR逐渐下降,同时氨转化率(NHR)逐渐升高.除此之外,四个站点NHR > 0.5的情况均主要发生在温度<25℃和相对湿度<70%的气象条件下.

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	黄国锋
	肖林海
	陈梓杰
	张涛
	钟庄敏
	方晓丹
	廖彤
	陈多宏

关键词 ：气态氨, 细颗粒物, 气体比率, 二次无机气溶胶, 气粒转化

Abstract：To investigate the contribution of NH₃ to fine particulate matter (PM_2.5) in typical areas of the Pearl River Delta in Southern China, three urban sites (GYQ, MH, and DC) and one suburban site (HGS) in the Pearl River Delta were selected to carry out online monitoring of NH₃. Water-soluble inorganic ion, nitric acid (HNO₃), PM_2.5 and meteorological parameters were collected simultaneously. The characteristics of concentration level and diurnal variation of NH₃ were analyzed. The potential contribution of NH₃ to PM_2.5 was further evaluated. The observed results showed that the annual average of NH₃ at GYQ, MH, DC and HGS were (5.74±3.0), (4.70±2.41), (5.09۬.26) and (4.17±1.95) μg/m³ respectively. Except for GYQ, the seasonal variation of NH₃ in other sites showed an increasing trend of autumn > spring > summer > winter. The diurnal variation of NH₃ concentration is similar to that of temperature, and opposite to that of relative humidity. According to the adjusted gas ratio (AdjGR), all sites exhibited high levels of NH₃. With the increase of PM_2.5 pollution concentration, AdjGR gradually decreased, while the ammonium-to-total ratio of NH₃ (NHR) gradually increased. In addition, the NHR > 0.5 of the four sites mainly occurred under the meteorological conditions of temperature < 25℃ and relative humidity < 70%.

Key words： atmospheric ammonia fine particulate matter adjusted gas ratio secondary inorganic aerosol gas-to-particle conversion

收稿日期: 2024-02-26

PACS:

X513

基金资助:国家重点研发计划重点专项(2022YFC3701101);国家自然科学基金重点项目(42230602);广东省科技计划项目(科技创新平台类) (2019B121201002)

通讯作者: 张涛,正高级工程师,gdeemc_zt@139.com;陈多宏,正高级工程师,chenduohong@139.com E-mail: gdeemc_zt@139.com;chenduohong@139.com

作者简介: 黄国锋(1974-),男,广东新会人,华南农业大学博士研究生,主要从事生态环境监测与管理研究.发表论文10余篇.49399439@qq.com.

引用本文:

黄国锋, 肖林海, 陈梓杰, 张涛, 钟庄敏, 方晓丹, 廖彤, 陈多宏. 珠三角典型地区气态氨分布及其对PM_2.5贡献[J]. 中国环境科学, 2024, 44(9): 4796-4804. HUANG Guo-feng, XIAO Lin-hai, CHEN Zi-jie, ZHANG Tao, HONG Zhuang-min, FANG Xiao-dan, LIAO Tong, CHEN Duo-hong. Atmospheric ammonia distribution and contribution to PM_2.5 in typical areas of Pearl River Delta. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(9): 4796-4804.

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[1] 方华,莫江明.活性氮增加:一个威胁环境的问题[J]. 生态环境, 2006,15(1):164-168. Fang H, Mo J M. Reactive nitrogen increasing: A threat to our environment [J]. Ecology and Environment, 2006,15(1):164-168.
[2] 赵晨旭,徐鹏,廖雅君,等.气态活性氮排放的环境影响研究进展[J]. 环境污染与防治, 2017,39(5):569-573. Zhao C X, Xu P, Liao J Y, et al. Research progress on environment impact of gaseous reactive nitrogen emission [J]. Environmental Pollution & Control, 2017,39(5):569-573.
[3] Wang F, Wang W C, Wang Z Y, et al. Drivers of PM_2.5-O₃co-pollution: from the perspective of reactive nitrogen conversion pathways in atmospheric nitrogen cycling [J]. Science Bulletin, 2022,67(18):1833-1836.
[4] Xu R T, Tian H Q, Pan S F, et al. Global ammonia emissions from synthetic nitrogen fertilizer applications in agricultural systems: Empirical and process-based estimates and uncertainty [J]. Global Change Biology, 2019,25(1):314-326.
[5] Xu J, Chen J, Zhao N, et al. Importance of gas-particle partitioning of ammonia in haze formation in the rural agricultural environment [J]. Atmospheric Chemistry and Physics, 2020,20(12):7259-7269.
[6] Yin S S, Huang Z J, Zheng J Y, et al. Characteristics of inorganic aerosol formation over ammonia-poor and ammonia-rich areas in the Pearl River Delta region, China [J]. Atmospheric Environment, 2018,177:120-31.
[7] Yue D L, Hu M, Wu Z J, et al. Variation of particle number size distributions and chemical compositions at the urban and downwind regional sites in the Pearl River Delta during summertime pollution episodes [J]. Atmospheric Chemistry and Physics, 2010,10(19):9431-9439.
[8] Dai W, Gao J Q, Cao G, et al. Chemical composition and source identification of PM_2.5 in the suburb of Shenzhen, China [J]. Atmospheric Research, 2013,122:391-400.
[9] Huang R J, Zhang Y L, Bozzetti C, et al. High secondary aerosol contribution to particulate pollution during haze events in China [J]. Nature, 2014,514(7521):218-222.
[10] Liu M X, Huang X, Song Y, et al. Ammonia emission control in China would mitigate haze pollution and nitrogen deposition, but worsen acid rain [J]. Proceedings of the National Academy of Sciences, 2019,116(16):7760-7765.
[11] Liu Z H, Zhou M, Chen Y F, et al. The nonlinear response of fine particulate matter pollution to ammonia emission reductions in North China [J]. Environmental Research Letters, 2021,16(3):034014.
[12] Zhai S X, Jacob D J, Wang X, et al. Control of particulate nitrate air pollution in China [J]. Nature Geoscience, 2021,14(6):389-395.
[13] Gu B J, Zhang L, Van Dingenen R, et al. Abating ammonia is more cost-effective than nitrogen oxides for mitigating PM_2.5 air pollution [J]. Science, 2021,374(6568):758-762.
[14] 杨显玉,吕雅琼,邵平,等.四川盆地大气氨与氮氧化物排放对细颗粒物污染的影响及减排潜力[J]. 中国环境科学, 2022,42(8):3502-3511. Yang X Y, Lv Y Q, Shao P, et al. Impacts of ammonia and nitrogen oxides emissions on fine particle matter pollution and mitigation potential over the Sichuan Basin [J]. China Environmental Science, 2022,42(8):3502-3511.
[15] 薛文博,许艳玲,唐晓龙,等.中国氨排放对PM_2.5污染的影响[J]. 中国环境科学, 2016,36(12):3531-3539. Xue W B, Xu Y L, Tang X L, et al. Impacts of ammonia emission on PM_2.5 pollution in China [J]. China Environmental Science, 2016,36(12):3531-3539.
[16] Liu L, Xu W, Lu X, et al. Exploring global changes in agricultural ammonia emissions and their contribution to nitrogen deposition since 1980[J]. Proceedings of the National Academy of Sciences, 2022, 119(14):e2121998119.
[17] Yu G R, Jia Y L, HE N P, et al. Stabilization of atmospheric nitrogen deposition in China over the past decade [J]. Nature Geoscience, 2019,12(6):424-429.
[18] Bhattarai N, Wang S X, Xu Q C, et al. Sources of gaseous NH₃ in urban Beijing from parallel sampling of NH₃ and NH₄⁺, their nitrogen isotope measurement and modeling [J]. Science of the Total Environment, 2020,747:141361.
[19] Chang Y H, Zou Z, Zhang Y L, et al. Assessing contributions of agricultural and nonagricultural emissions to atmospheric ammonia in a Chinese megacity [J]. Environmental Science & Technology, 2019, 53(4):1822-1833.
[20] Pan Y P, Tian S L, Liu D W, et al. Fossil fuel combustion-related emissions dominate atmospheric ammonia sources during severe haze episodes: evidence from ¹⁵N-stable isotope in size-resolved aerosol ammonium [J]. Environmental Science & Technology, 2016,50(15):8049-8056.
[21] Zhou C L, Zhou H, Holsen T M, et al. Ambient ammonia concentrations across New York state [J]. Journal of Geophysical Research: Atmospheres, 2019,124(14):8287-8302.
[22] 张子俊.珠三角PM_2.5浓度率先进入“1字头” [N]. 南方日报, 2023-01-10(A06). Zhao Z J. The concentration of PM_2.5 in the Pearl River Delta is the first to enter the "prefix" [N]. Nanfang Daily, 2023-01-10(A06).
[23] 黄春桃,林锦眉,张馨予.2016~2020年珠三角地区PM_2.5时空变化特征分析[J]. 山东化工, 2021,50(15):263-265,269. Huang C T, Lin J M, Zhang X Y. Analysis of the characteristics of the temporal and spatial changes of PM_2.5 in the Pearl River Delta from 2016 to 2020[J]. Shandong Chemical Industry, 2021,50(15):263-265,269.
[24] 刘湘雪,蒲维维,马志强,等.北京地区大气氨时空变化特征[J]. 中国环境科学, 2021,41(8):3473-3483. Liu X X, Pu W W, Ma Z Q, et al. Study on the temporal and spatial variation of atmospheric ammonia in Beijing [J]. China Environmental Science, 2021,41(8):3473-3483.
[25] 邵生成,常运华,曹芳,等.南京城市大气氨-铵的高频演化及其气粒转化机制[J]. 环境科学, 2019,40(10):4355-4363. Shao S C, Chang Y H, Cao F, et al. High-frequency evolution of urban atmospheric ammonia and ammonium and its gas-to-particle conversion mechanism in Nanjing City [J]. Environmental Science, 2019,40(10):4355-4363.
[26] 余益军,庄旻,王振,等.富氨对常州PM_2.5理化性质与二次反应的影响[J/OL]. 环境科学:1-13[2023-12-06]. DOI:10.13227/j.hjkx.202309100. Yu Y J, Zhuang M, Wang Z, et al. Role of ammonia in aerosol liquid water, pH, and secondary inorganic aerosols formation at an ammonia-rich city in Changzhou [J/OL]. Environmental Science: 1-13[2023-12-06]. DOI:10.13227/j.hjkx.202309100.
[27] 周斌,王雪,段玉森,等.北京秋冬季大气氨观测研究[J]. 环境科学学报, 2022,42(9):384-391. Zhou B, Wang X, Duan Y S, et al. The observation of atmospheric ammonia in Beijing during autumn and winter [J]. Acta Scientiae Circumstantiae, 2022,42(9):384-391.
[28] HJ 1328-2023环境空气颗粒物(PM_2.5)中水溶性离子连续自动监测技术规范[S]. HJ 1328-2023 Technical specifications for continuous automated monitoring of water-soluble ions in ambient air particulate matter (PM_2.5) [S].
[29] HJ 817-2018环境空气颗粒物(PM₁₀和PM_2.5)连续自动监测系统运行和质控技术规范[S]. HJ 817-2018 Technical specifications for operation and quality control of ambient air quality automated monitoring system for particulate matter (PM₁₀ and PM_2.5) [S].
[30] Hu G Y, Zhang Y M, Sun J Y, et al. Variability, formation and acidity of water-soluble ions in PM_2.5 in Beijing based on the semi-continuous observations [J]. Atmospheric Research, 2014,145-146:1-11.
[31] Pinder R W, Dennis R L, Bhave P V. Observable indicators of the sensitivity of PM_2.5 nitrate to emission reductions—Part I: Derivation of the adjusted gas ratio and applicability at regulatory-relevant time scales [J]. Atmospheric Environment, 2008,42(6):1275-1286.
[32] 宋晓聪,杜帅,沈鹏,等.中国农业氨排放和PM_2.5空间分布特征分析[J]. 生态经济, 2023,39(10):200-207. Song X C, Du S, Shen P, et al. Analysis on the spatial distribution of agricultural ammonia emissions and PM_2.5 in China [J]. Ecological Economy, 2023,39(10):200-207.
[33] 邹忠,常运华.基于隧道法的机动车对上海城市大气环境中氨的源排放贡献研究[J]. 环境监控与预警, 2018,10(1):6-9. Zou Z, Chang Y H. Study on the contribution of vehicles to ammonia emission of shanghai atmospheric environment based on tunnel method [J]. Environmental Monitoring and Forewarning, 2018,10(1):6-9.
[34] Huang X J, Zhang J K, Zhang W, et al. Atmospheric ammonia and its effect on PM_2.5 pollution in urban Chengdu, Sichuan Basin, China [J]. Environmental Pollution, 2021,291:118195.
[35] Pan Y P, Tian S L, Zhao Y H, et al. Identifying ammonia hotspots in China using a national observation network [J]. Environmental Science & Technology, 2018,52(7):3926-3934.
[36] Zhang X, Zhang K, Liu H P, et al. Pollution sources of atmospheric fine particles and secondary aerosol characteristics in Beijing [J]. Journal of Environmental Sciences, 2020,95:91-98.
[37] Lonati G, Cernuschi S. Temporal and spatial variability of atmospheric ammonia in the Lombardy region (Northern Italy) [J]. Atmospheric Pollution Research, 2020,11(12):2154-2163.
[38] 岳玎利,钟流举,张涛,等.珠三角地区大气PM_2.5理化特性季节规律与成因[J]. 环境污染与防治, 2015,37(4):1-6,12. Yue D L, Zhong L J, Zhang T, et al. Causes, physical and chemical properties of atmospheric PM_2.5in Pearl River Delta during four season [J]. Environmental Pollution & Control, 2015,37(4):1-6,12.
[39] Edgerton E S, Saylor R D, Hartsell B E. Ammonia and ammonium measurements from the southeastern United States [J]. Atmospheric Environment, 2007,41(16):3339-3351.
[40] Zbieranowski A L, Aherne J. Ambient concentrations of atmospheric ammonia, nitrogen dioxide and nitric acid across a rural–urban– agricultural transect in southern Ontario, Canada [J]. Atmospheric Environment, 2012,62:481-491.
[41] Park J, Kim E, Oh S, et al. Contributions of ammonia to high concentrations of PM_2.5 in an urban area [J]. Atmosphere, 2021, 12(1676-1690).
[42] 姚星灿,康汉青,杜亚宁,等.基于二次无机气溶胶研究南京冬春季霾污染过程的形成特征和来源解析[J]. 环境化学, 2023,42(12):4151-4160. Yao X C, Kang H Q, Du Y N, et al. Formation characteristics and source analysis of haze pollution process during winter and spring in Nanjing based on secondary inorganic aerosol [J]. Environmental Chemistry, 2023,42(12):4151-4160.
[43] Hu M, Wu Z J, Slanina J, et al. Acidic gases, ammonia and water-soluble ions in PM_2.5 at a coastal site in the Pearl River Delta, China [J]. Atmospheric Environment, 2008,42(25):6310-6320.
[44] Zhao M J, Wang S X, Tan J H, et al. Variation of urban atmospheric ammonia pollution and its relation with PM_2.5 chemical property in winter of Beijing, China [J]. Aerosol and Air Quality Research, 2016, 16(6):1378-1389.
[45] Ianniello A, Spataro F, Esposito G, et al. Occurrence of gas phase ammonia in the area of Beijing (China) [J]. Atmospheric Chemistry and Physics, 2010,10(19):9487-9503.
[46] Wang S S, Nan J L, Shi C Z, et al. Atmospheric ammonia and its impacts on regional air quality over the megacity of Shanghai, China [J]. Scientific Reports, 2015,5:15842.
[47] Baek B H, Aneja V P, Tong Q S. Chemical coupling between ammonia, acid gases, and fine particles [J]. Environmental Pollution, 2004,129(1):89-98.
[48] ISBN 978-92-4-003422-8. WHO global air quality guidelines: particulate matter (PM_2.5 and PM₁₀), ozone, nitrogen dioxide, sulfur dioxide and carbon monoxide [S].
[49] Zhang R Y, Wang G H, Guo S, et al. Formation of urban fine particulate matter [J]. Chemical Reviews, 2015,115(10):3803-3855.
[50] Seinfeld J H and Pandis S N. Atmospheric chemistry and physics: From air pollution to climate change, Third Edition [M]. John Wiley & Sons Inc, 2016.