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In situ Raman spectroscopic study of nitrogen speciation in aqueous fluids under pressure
Chen, Qi1; Zhang, Zhigang2,3; Wang, Zhongping4; Li, Wan-Cai1; Gao, Xiao-Ying1; Ni, Huaiwei1
2019-02-20
发表期刊CHEMICAL GEOLOGY
ISSN0009-2541
卷号506页码:51-57
摘要Nitrogen speciation in aqueous fluids is important for understanding the partitioning of N between fluid and coexisting melt or mineral phases and the storage and recycling of nitrogen in Earth's interior. Previously N speciation in aqueous fluids has only been investigated using the approach of quenched fluid inclusions or thermodynamic modeling. Here we present the results from in situ Raman spectroscopic measurements of N speciation in aqueous fluids held in hydrothermal diamond anvil cell, at P-T conditions up to above 800 degrees C and 2 GPa. We identify the presence of N in aqueous fluids as N-2 and NH3 (replaced by NH4+ at low pH) with N-2 being the favored species toward higher temperature. The fugacity equilibrium constant for reaction N-2 + 3 H2O = 2 NH3 + 3/2 O-2 is determined to be lnK(f) =-16.15-23,489/T with T being temperature in Kelvin. Our equilibrium constant is significantly lower than that from quenched fluid inclusions, but is in good agreement with that calculated from the Deep Earth Water (DEW) model. We suggest that the thermodynamic stability of N-2 relative to NH3 in aqueous fluids has been underestimated by quench experiments. Because N is stored in silicate minerals and melts mainly as NH4+, the bulk partition coefficient of N between fluid and mineral or melt should be greater than previously thought if one assumes a fixed partition coefficient for trivalent N. For subduction zones this means that a higher fraction of N is recycled by slab-derived fluids, and concomitantly less N is carried by subducting slabs to Earth's deeper interior.
关键词Nitrogen Aqueous fluids Speciation Oxygen fugacity Raman
DOI10.1016/j.chemgeo.2018.12.016
资助者Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China
关键词[WOS]UPPER-MANTLE ; AMMONIUM ; WATER ; INCLUSIONS ; VOLATILE ; BEHAVIOR ; STATE ; EARTH ; MICAS ; PH
语种英语
资助项目Strategic Priority Research Program (B) of the Chinese Academy of Sciences[XDB18000000] ; National Natural Science Foundation of China[41825004] ; National Natural Science Foundation of China[41590622] ; National Natural Science Foundation of China[41721002] ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China[WK2080000102]
资助者Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; Strategic Priority Research Program (B) of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; 111 Project of Ministry of Education, China ; 111 Project of Ministry of Education, China ; Fundamental Research Funds for the Central Universities of China ; Fundamental Research Funds for the Central Universities of China
WOS研究方向Geochemistry & Geophysics
WOS类目Geochemistry & Geophysics
WOS记录号WOS:000456708100005
出版者ELSEVIER SCIENCE BV
引用统计
文献类型期刊论文
条目标识符http://ir.iggcas.ac.cn/handle/132A11/90223
专题地球与行星物理院重点实验室
通讯作者Li, Wan-Cai; Ni, Huaiwei
作者单位1.Univ Sci & Technol China, Sch Earth & Space Sci, CAS Key Lab Crust Mantle Mat & Environm, Hefei 230026, Anhui, Peoples R China
2.Chinese Acad Sci, Inst Geol & Geophys, Key Lab Earth & Planetary Phys, Beijing 100029, Peoples R China
3.Univ Chinese Acad Sci, Coll Earth & Planetary Sci, Beijing 100049, Peoples R China
4.Univ Sci & Technol China, Phys Expt Teaching Ctr, Hefei 230026, Anhui, Peoples R China
推荐引用方式
GB/T 7714
Chen, Qi,Zhang, Zhigang,Wang, Zhongping,et al. In situ Raman spectroscopic study of nitrogen speciation in aqueous fluids under pressure[J]. CHEMICAL GEOLOGY,2019,506:51-57.
APA Chen, Qi,Zhang, Zhigang,Wang, Zhongping,Li, Wan-Cai,Gao, Xiao-Ying,&Ni, Huaiwei.(2019).In situ Raman spectroscopic study of nitrogen speciation in aqueous fluids under pressure.CHEMICAL GEOLOGY,506,51-57.
MLA Chen, Qi,et al."In situ Raman spectroscopic study of nitrogen speciation in aqueous fluids under pressure".CHEMICAL GEOLOGY 506(2019):51-57.
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