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dc.contributor.authorZexing Cao
dc.contributor.author曹泽星
dc.contributor.authorZhaohui Zhou
dc.contributor.author周朝晖
dc.contributor.authorHuilin Wan
dc.contributor.author万惠霖
dc.contributor.authorQianer Zhang
dc.contributor.author张乾二
dc.date.accessioned2011-11-21T01:17:59Z
dc.date.available2011-11-21T01:17:59Z
dc.date.issued2005-02
dc.identifier.citationINTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY,2005,103(3):344-353zh_CN
dc.identifier.issn0020-7608
dc.identifier.urihttp://dx.doi.org/doi: 10.1002/qua.20492
dc.identifier.urihttps://dspace.xmu.edu.cn/handle/2288/11213
dc.description.abstractWe used density functional calculations to model dinitrogen reduction by a FeMo cofactor containing a central nitrogen atom and by a Mo-based catalyst. Plausible intermediates, reaction pathways, and relative energetics in the enzymatic and catalytic reduction of N-2 to ammonia at a single Mo center are explored. Calculations indicate that the binding of N-2, to the Mo atom and the subsequent multiple proton-electron transfer to dinitrogen and its protonated species involved in the conversion of N-2, are feasible energetically. In the reduction of N-2, the Mo atom experiences a cycled oxidation state from Mo(IV) to Mo(VI) by nitrogenase and from Mo(III) to Mo(VI) by the molybdenum catalyst, respectively, tuning the gradual reduction of N-2. Such a wide range of oxidation states exhibited by the Mo center is crucial for the gradual reduction process via successive proton-electron transfer. Present results suggest that the Mo atom in the N-centered FeMo cofactor is a likely alternative active site for dinitrogen binding and reduction under mild conditions once there is an empty site available at the Mo site. (c) 2005 Wiley Periodicals, Inc.zh_CN
dc.language.isoenzh_CN
dc.publisherJOHN WILEY & SONS INCzh_CN
dc.subjectdensity functional calculationszh_CN
dc.subjectnitrogenasezh_CN
dc.subjectFeMo cofactorzh_CN
dc.subjectmolybdenumzh_CN
dc.subjectnitrogen fixationzh_CN
dc.titleEnzymatic and catalytic reduction of dinitrogen to ammonia: Density functional theory characterization of alternative molybdenum active siteszh_CN
dc.typeArticlezh_CN


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