Nitrogen isotope fractionations among gaseous and aqueous NH4+ NH3, N-2, and metal-ammine complexes: Theoretical calculations and applications

doi:10.1016/j.gca.2020.12.010

CORC > 力学研究所 > 中国科学院力学研究所 > 高温气体动力学国家重点实验室

	Nitrogen isotope fractionations among gaseous and aqueous NH4+ NH3, N-2, and metal-ammine complexes: Theoretical calculations and applications
	Li, Long 2; He YY(何雨旸)3; Zhang, Zhe 2; Liu, Yun 1,4,5
刊名	GEOCHIMICA ET COSMOCHIMICA ACTA
	2021-02-15
卷号	295 页码:80-97
关键词	Nitrogen isotope fractionation Ammonium Metal-ammine complex Ammonia degassing Hydrothermal fluid
ISSN号	0016-7037
DOI	10.1016/j.gca.2020.12.010
通讯作者	Li, Long(long4@ualberta.ca)
英文摘要	Ammonium (NH4+), ammonia (NH3) and N-2 are key nitrogen species in geological nitrogen recycling. NH3 has also been proposed to play an important role in mobilizing base metals in the form of metal-ammine complexes in hydrothermal fluids. The nitrogen isotope fractionation factors among these nitrogen species in aqueous and gaseous phases are essential parameters to trace source signatures and geochemical properties in geological processes. However, the nitrogen isotope fractionation factors for metal-ammine complexes are largely absent, and the few existing nitrogen isotope fractionation factors for the aqueous NH4+ - aqueous NH3 pair show large discrepancy between experimental results and theoretical calculations. In this study, we employed the density functional theory to systematically calculate the nitrogen isotope fractionation factors among the nitrogen species that may occur in a hydrothermal system, i.e., gaseous N-2, gaseous and aqueous NH4+ and NH3, and ammine complexes of Co, Zn, Cu, Cd, Ag, Au, and Pt. Based on these new results, the large nitrogen isotope fractionations for the aqueous NH4+ - aqueous NH3 pair observed in previous experimental studies can be well explained by a combined effect of an equilibrium isotope fractionation between aqueous NH4+ and aqueous NH3 and a kinetic isotope fractionation during NH3 degassing from the solution. This suggests that the nitrogen isotopic behavior during NH3 degassing in natural hydrothermal system can be more complicated than previous thought. A numeric model is thus established here to quantify the combined isotopic effect on partial NH3 degassing. Using the new results of metal-ammine complexes, we also tested the hypothesis that nitrogen mobilization could be controlled by copper-ammine complex based on the copper concentration-delta N-1(5) relationship previously observed in meta-gabbros. (C) 2020 Elsevier Ltd. All rights reserved.
分类号	一类
资助项目	NSERC-Discovery Grant ; China Postdoctoral Science Foundation[2019M660811] ; Chinese NSF[41530210]
WOS研究方向	Geochemistry & Geophysics
语种	英语
WOS记录号	WOS:000614115300005
资助机构	NSERC-Discovery Grant ; China Postdoctoral Science Foundation ; Chinese NSF
其他责任者	Li, Long
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/86061]
专题	力学研究所_高温气体动力学国家重点实验室
作者单位	1.Chengdu Univ Technol, Coll Earth Sci, Int Ctr Planetary Sci, Chengdu 610059, Peoples R China 2.Univ Alberta, Dept Earth & Atmospher Sci, Edmonton, AB T6G 2E3, Canada; 3.Chinese Acad Sci, Inst Mech, Beijing 100190, Peoples R China; 4.Chinese Acad Sci, Inst Geochem, State Key Lab Ore Deposit Geochem, Guiyang 550081, Peoples R China; 5.Chinese Acad Sci, Ctr Excellence Comparat Planetol, Hefei 230001, Peoples R China;
推荐引用方式 GB/T 7714	Li, Long,He YY,Zhang, Zhe,et al. Nitrogen isotope fractionations among gaseous and aqueous NH4+ NH3, N-2, and metal-ammine complexes: Theoretical calculations and applications[J]. GEOCHIMICA ET COSMOCHIMICA ACTA,2021,295:80-97.
APA	Li, Long,何雨旸,Zhang, Zhe,&Liu, Yun.(2021).Nitrogen isotope fractionations among gaseous and aqueous NH4+ NH3, N-2, and metal-ammine complexes: Theoretical calculations and applications.GEOCHIMICA ET COSMOCHIMICA ACTA,295,80-97.
MLA	Li, Long,et al."Nitrogen isotope fractionations among gaseous and aqueous NH4+ NH3, N-2, and metal-ammine complexes: Theoretical calculations and applications".GEOCHIMICA ET COSMOCHIMICA ACTA 295(2021):80-97.