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DOI | 10.1126/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 |
ISSN | 0036-8075 |
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
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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 |
推荐引用方式 GB/T 7714 | 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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