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Density Functional Theory Calculations of Equilibrium Mo Isotope Fractionation Factors among MoOxS4-x2- Species in the Aqueous Phase by the ONIOM Method

文献类型：期刊论文

作者He, Yuyang1,2; Gao, Caihong5; Wei, Wei4; Liu, Yun3,5
刊名ACS EARTH AND SPACE CHEMISTRY
出版日期2023-01-19
卷号7期号:1页码:142-155
ISSN号2472-3452
关键词paleoredox proxy ab initio molecular dynamics implicit solvent model dispersion correction water-droplet periodical boundary condition
DOI10.1021/acsearthspacechem.2c00268
通讯作者He, Yuyang(yhe@mail.iggcas.ac.cn)
英文摘要Molybdenum (Mo) is a redox-sensitive metal element. Its isotope composition (delta Mo-98) has the potential to reconstruct oceanic oxygenation extent in deep time. To accurately reconstruct the bulk delta Mo-98 value of ancient seawater from sediment records, it is necessary to clarify the Mo isotope fractionation mechanism during the transformation among thiomolybdates (MoOxS4-x2-, x = 0 similar to 4) in marine environments. For aqueous systems, predicting the equilibrium isotope fractionation factors theoretically needs careful treatment of solvent effects. The commonly used water-droplet or periodical boundary condition methods are not only troublesome but also time-consuming. We test the efficiency of the two-layer own N-layer integrated molecular orbital molecular mechanics (ONIOM) method in predicting the reduced partition function ratios (beta factors) of the MoOxS42- species in aqueous phases. Compared to other methods, the ONIOM method can produce beta factors with the same accuracy and considerably fewer computational resources. The predicted beta factors are in the order MoO4(aq)2- > MoO3S(aq)2- > MoO2S2(aq)2- > MoOS3(aq)2- > MoS4(aq)2-, which are in line with previous laboratory experiments and field observations. The new results provide the basic data for reconstructing delta Mo-98 values in suboxic, ferruginous, and weakly euxinic sediments.
WOS关键词INITIO MOLECULAR-DYNAMICS ; EFFECTIVE CORE POTENTIALS ; CARBONATE MINERALS ; EUXINIC SEDIMENTS ; GAUSSIAN-ORBITALS ; MODERN BLACK ; MOLYBDENUM ; OXYGEN ; ADSORPTION ; MECHANISM
资助项目National Science Foundation of China (NSFC)[4217030170] ; National Science Foundation of China (NSFC)[42150202] ; NSFC[41903019] ; NSFC[42130114] ; CAS[XDB41000000] ; NSFC project[41902025] ; Civil Aerospace Technologies of China National Space Administration[D020203]
WOS研究方向Chemistry ; Geochemistry & Geophysics
语种英语
WOS记录号WOS:001111265000004
资助机构National Science Foundation of China (NSFC) ; NSFC ; CAS ; NSFC project ; Civil Aerospace Technologies of China National Space Administration
源URL[http://dspace.imech.ac.cn/handle/311007/93622]  
专题力学研究所_高温气体动力学国家重点实验室
通讯作者He, Yuyang
作者单位1.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China
2.Chinese Acad Sci, Inst Geol & Geophys, Key Lab Earth & Planetary Phys, Beijing 100029, Peoples R China
3.Chengdu Univ Technol, Coll Earth Sci, Int Ctr Planetary Sci, Chengdu 610059, Sichuan, Peoples R China
4.Univ Sci & Technol China, Sch Earth & Space Sci, CAS Key Lab Crust Mantle Mat & Environm, Hefei 230026, Anhui, Peoples R China
5.Chinese Acad Sci, Inst Geochem, State Key Lab Ore Deposit Geochem, Guiyang 550081, Guizhou, Peoples R China
推荐引用方式
GB/T 7714		 He, Yuyang,Gao, Caihong,Wei, Wei,et al. Density Functional Theory Calculations of Equilibrium Mo Isotope Fractionation Factors among MoOxS4-x2- Species in the Aqueous Phase by the ONIOM Method[J]. ACS EARTH AND SPACE CHEMISTRY,2023,7(1):142-155.
APA He, Yuyang,Gao, Caihong,Wei, Wei,&Liu, Yun.(2023).Density Functional Theory Calculations of Equilibrium Mo Isotope Fractionation Factors among MoOxS4-x2- Species in the Aqueous Phase by the ONIOM Method.ACS EARTH AND SPACE CHEMISTRY,7(1),142-155.
MLA He, Yuyang,et al."Density Functional Theory Calculations of Equilibrium Mo Isotope Fractionation Factors among MoOxS4-x2- Species in the Aqueous Phase by the ONIOM Method".ACS EARTH AND SPACE CHEMISTRY 7.1(2023):142-155.

入库方式： OAI收割

来源：力学研究所

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