DOI: 10.1016/j.atmosenv.2020.117563
论文题名: Source and formation of fine particulate nitrate in South China: Constrained by isotopic modeling and online trace gas analysis
作者: Su T. ; Li J. ; Tian C. ; Zong Z. ; Chen D. ; Zhang G.
刊名: Atmospheric Environment
ISSN: 1352-2310
出版年: 2020
卷: 231 语种: 英语
英文关键词: Bayesian networks
; Coal combustion
; Free radicals
; Gases
; Intelligent systems
; Monte Carlo methods
; Nitrogen oxides
; Phase interfaces
; Environmental parameter
; Equilibrium fractionations
; Fine particulate matter (PM2.5)
; Gas-phase reactions
; On-line trace gas analysis
; Potential source contribution function
; Relative contribution
; Thermodynamic effect
; Trace analysis
; carbon monoxide
; coal
; dinitrogen pentoxide
; hydroxyl radical
; nitrate
; nitrogen
; nitrogen 15
; nitrogen dioxide
; nitrogen oxide
; oxygen
; oxygen 18
; sulfur dioxide
; Bayesian analysis
; combustion
; concentration (composition)
; fractionation
; hydrolysis
; isotopic composition
; nitrate
; nitrogen isotope
; oxidation
; oxygen isotope
; particle size
; thermodynamics
; aerosol
; Article
; autumn
; Bayes theorem
; chemical analysis
; chemical composition
; China
; combustion
; concentration (parameter)
; environmental parameters
; fractionation
; gas analysis
; hydrolysis
; isotope analysis
; Monte Carlo method
; particulate matter
; priority journal
; reaction analysis
; seasonal variation
; spring
; summer
; thermodynamics
; winter
; China
; Guangdong
学科: Isotope
; Nitrate
; Pearl River Delta
; Source apportionment
中文摘要: NOx is an important precursor of fine particulate matter (PM2.5) and O3 and its oxidation product NO3− may be the main driver of PM2.5. In this study, 76 daily fine particle samples were collected from a site in South China, and the characteristics of NO3− were studied using an improved Bayesian mixing model based on δ15N–δ18O compositions and online trace gas analysis. NO3− concentrations ranged from 0.60 to 21.7 μg/m3, accounting for 6.0 ± 3.3% of total PM2.5 on average. δ15N–NO3− values varied from −3.6 to 15.4‰ (average: 7.5 ± 3.3‰). Driven by changes in chemical pathways and environmental parameters, including equilibrium fractionation and thermodynamic effects, δ15N–NO3- values were lowest in spring and highest in winter. δ18O–NO3- values varied from 21.0 to 90.1‰ (average: 62.4 ± 14.0‰). In spring, the lowest δ18O–NO3- values were observed due to high proportions originating from ·HO2 and ·OH reaction pathways, as well as changes in other parameters. In winter, the highest δ18O–NO3- values were observed due to cold and dry weather, along with the lowest proportion from the ·OH pathway. Moreover, the trace gases CO, O3, NOx, SO2, and N2O5 were measured seasonally to determine the main drivers of seasonality in δ15N–δ18O composition. Monte Carlo simulation was used to estimate the relative contributions of the gas-phase reactions of NO2 and ·OH radicals and the hydrolysis of N2O5. The results showed that the ·OH generation pathway was predominant throughout the year, with relative contributions of 72 ± 18%, 76 ± 16%, 63 ± 17% and 39 ± 15% in spring, summer, fall and winter, respectively. Coal combustion (50.1 ± 13.8%) was the predominant source of NO3− identified using the Bayesian model, and originated from central and southern Guangdong Province, as indicated by potential source contribution function analysis. © 2020 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/160773
Appears in Collections: 气候变化与战略
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作者单位: State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, 510640, China; Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai, 264003, China; Guangdong Environmental Monitoring Center, Guangzhou, 510308, China; University of Chinese Academy of Sciences, Beijing, 100049, China
Recommended Citation:
Su T.,Li J.,Tian C.,et al. Source and formation of fine particulate nitrate in South China: Constrained by isotopic modeling and online trace gas analysis[J]. Atmospheric Environment,2020-01-01,231