Simultaneous measurements of gas- and aerosol-phase water-soluble organic nitrogen in the winter urban atmosphere of Chengdu, China

IF 5.7 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
Kaitao Chen,Zheng Li,Rui Li,Luyao Chen,Rongjie Li,Binyu Xiao,Shaojun Lv,Can Wu,Rui Li,Junke Zhang,Gehui Wang
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Abstract

Partitioning gaseous water-soluble organic nitrogen (WSON) to the aerosol phase is a major formation pathway of atmospheric secondary organic aerosols (SOA). However, the factors influencing this WSON partitioning process remain unclear. We conducted simultaneous wintertime measurements of WSON in both gas and aerosol phases at an urban site in Chengdu (CD), located in the Sichuan Basin (SCB), China, to investigate the concentration, gas-particle partitioning processes, and driven factors of WSON. The average concentration of particulate WSON (2.3±1.4µgNm-3) was about twice that of gaseous WSON (1.2±0.9µgNm-3) and increased significantly as PM 2.5 increased. In winter, WSON readily partitions into the particle phase (FWSON=0.70±0.14), partitioning into the organic phase under warm, dry conditions and into aerosol liquid water under cold, humid conditions, with higher F WSON in the latter. Amines (methylamine, MA; dimethylamine, DMA) were predominantly present in the gas phase but exhibited enhanced partitioning into the particle phase during the PM 2.5 polluted periods. Amines preferentially partitioned into aerosol liquid water throughout the entire campaign, stably existing as amine-sulfate or amine-nitrate salts in PM 2.5 . The influence of aerosol liquid water content (ALWC) on the partitioning behavior of both WSON and amines was substantially greater than that of temperature ( T ), relative humidity (RH), and aerosol acidity (pH), as further confirmed by thermodynamic modeling with S-curve analysis. Furthermore, NH 4 NO 3 was identified as the primary contributor to ALWC, suggesting that controlling NO x and NH 3 emissions is crucial for reducing ALWC and subsequent WSON formation.
成都冬季城市大气中气相和气溶胶相水溶性有机氮的同时测量
气态水溶性有机氮(WSON)向气溶胶相的分配是大气次生有机气溶胶(SOA)的主要形成途径。然而,影响WSON划分过程的因素尚不清楚。我们在中国四川盆地成都(CD)的一个城市站点同时进行了冬季气相和气溶胶相的WSON测量,以研究WSON的浓度、气-颗粒分配过程和驱动因素。颗粒物WSON的平均浓度(2.3±1.4µgNm-3)约为气态WSON(1.2±0.9µgNm-3)的2倍,且随PM 2.5的升高而显著升高。在冬季,WSON容易分裂为颗粒相(FWSON=0.70±0.14),在温暖干燥条件下分裂为有机相,在寒冷潮湿条件下分裂为气溶胶液态水,后者的WSON较高。胺类(甲胺,MA,二甲胺,DMA)主要存在于气相,但在PM 2.5污染期间表现出向颗粒相的增强分配。在整个战役中,胺优先分配到气溶胶液态水中,稳定地以硫酸胺或硝酸胺盐的形式存在于PM 2.5中。气溶胶液态水含量(ALWC)对WSON和胺类物质分配行为的影响明显大于温度(T)、相对湿度(RH)和气溶胶酸度(pH),这一点在s曲线分析的热力学模型中得到了进一步证实。此外,nh4no3被确定为ALWC的主要贡献者,这表明控制nox和nh3的排放对于减少ALWC和随后的WSON形成至关重要。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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