气候变化领域集成服务门户(CCPortal): Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning

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DOI	10.5194/acp-19-12221-2019
	Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning
	Chang Y.; Zhang Y.-L.; Li J.; Tian C.; Song L.; Zhai X.; Zhang W.; Huang T.; Lin Y.-C.; Zhu C.; Fang Y.; Lehmann M.F.; Chen J.
发表日期	2019
ISSN	16807316
起始页码	12221
结束页码	12234
卷号	19 期号:19
英文摘要	Predicting tropospheric cloud formation and subsequent nutrient deposition relies on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloud water. However, this challenge is difficult to address quantitatively based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH+4 ) and nitrate (NO-3), play a particularly important role in tropospheric cloud formation. While dry and wet (mainly rainfall) deposition of NH+4 and NO-3 are regularly assessed, cloud water deposition is often underappreciated. Here we collected cloud water samples at the summit of Mt. Tai (1545m above sea level) in eastern China during a long-lasting biomass burning (BB) event and simultaneously measured for the first time the isotopic compositions (mean ±1σ/ of cloud water nitrogen species (δ15N-NH+4 = -6.53%±4.96 %, δ15N-NO-3 =-2.35%±2.00 %, δ18O-NO-3 = 57.80%±4.23 %), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloud water NH+4 (32.9%±4.6 %) and NO-3 (28.2%±2.7 %) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly developed computational quantum chemistry module. Despite an overall reduction in total anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ15N-NO-3 values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ18O-NO-3 values imply that the reaction of OH with NO2 is the dominant pathway of NO-3 formation (57%±11 %), yet the contribution of heterogeneous hydrolysis of dinitrogen pentoxide was almost as important (43%±11 %). Although the limited sample set used here results in a relatively large uncertainty with regards to the origin of cloud-associated nitrogen deposition, the high concentrations of inorganic nitrogen imply that clouds represent an important source of nitrogen, especially for nitrogen-limited ecosystems in remote areas. Further simultaneous and long-term sampling of aerosol, rainfall, and cloud water is vital for understanding the anthropogenic influence on nitrogen deposition in the study region. © 2019 Author(s).
语种	英语
scopus关键词	anthropogenic source; atmospheric chemistry; atmospheric deposition; biomass burning; chemical property; cloud water; concentration (composition); emission inventory; isotopic composition; nitrogen; China; Shandong; Tai Shan
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144118
作者单位	KLME and CIC-FEMD, Yale-NUIST Center on Atmospheric Environment, Nanjing University of Information Science and Technology, Nanjing, 210044, China; Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai, 200433, China; Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai, 264003, China; CAS Key Laboratory of Forest Ecology and Management, Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang, 110016, China; Aquatic and Isotope Biogeochemistry, Department of Environmental Sciences, University of Basel, Basel, 4056, Switzerland
推荐引用方式 GB/T 7714	Chang Y.,Zhang Y.-L.,Li J.,et al. Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning[J],2019,19(19).
APA	Chang Y..,Zhang Y.-L..,Li J..,Tian C..,Song L..,...&Chen J..(2019).Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning.Atmospheric Chemistry and Physics,19(19).
MLA	Chang Y.,et al."Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning".Atmospheric Chemistry and Physics 19.19(2019).