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DOI10.1126/science.1238663
Dinitrogen cleavage and hydrogenation by a trinuclear titanium polyhydride complex
Shima T.; Hu S.; Luo G.; Kang X.; Luo Y.; Hou Z.
发表日期2013
ISSN0036-8075
起始页码1549
结束页码1552
卷号340期号:6140
英文摘要Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By 1H and 15N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N2) reduction proceeds sequentially through scission of a N2 molecule bonded to three Ti atoms in a μ-η1:η2:η2- end-on-side-on fashion to give a μ2-N/μ3-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ2-N nitrido unit.
英文关键词dinitrogen; hydrogen; nitrogen; titanium; trinuclear titanium polyhydride complex; unclassified drug; ammonia; chemical bonding; complexation; nitrogen; reaction kinetics; redox conditions; temperature effect; article; atom; chemical bond; environmental temperature; hydrogenation; nitrogen nuclear magnetic resonance; pressure; priority journal; proton nuclear magnetic resonance; X ray crystallography
语种英语
来源期刊Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/245467
作者单位Advanced Catalysis Research Group, RIKEN, Center for Sustainable Resource Science, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan; Organometallic Chemistry Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan; State Key Laboratory of Fine Chemicals and School of Pharmaceutical Science and Technology, Dalian University of Technology, Dalian 116024, China
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Shima T.,Hu S.,Luo G.,et al. Dinitrogen cleavage and hydrogenation by a trinuclear titanium polyhydride complex[J],2013,340(6140).
APA Shima T.,Hu S.,Luo G.,Kang X.,Luo Y.,&Hou Z..(2013).Dinitrogen cleavage and hydrogenation by a trinuclear titanium polyhydride complex.Science,340(6140).
MLA Shima T.,et al."Dinitrogen cleavage and hydrogenation by a trinuclear titanium polyhydride complex".Science 340.6140(2013).
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