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二氧化硅负载的氢化钽([三键]SiO)2Ta-H催化甲烷非氧化偶联生成乙烷和氢气的反应

Non-oxidative coupling reaction of methane to ethane and hydrogen catalyzed by the silica-supported tantalum hydride: ([triple bond]SiO)2Ta-H.

作者信息

Soulivong Daravong, Norsic Sébastien, Taoufik Mostafa, Copéret Christophe, Thivolle-Cazat Jean, Chakka Sudhakar, Basset Jean-Marie

机构信息

Laboratoire de Chimie Organométallique de Surface, UMR CNRS, ESCPE UCB 5265, 43 blvd du 11 Novembre 1918, F-69616 Villeurbanne Cedex, France.

出版信息

J Am Chem Soc. 2008 Apr 16;130(15):5044-5. doi: 10.1021/ja800863x. Epub 2008 Mar 26.

DOI:10.1021/ja800863x
PMID:18366170
Abstract

Silica-supported tantalum hydride, (SiO)2Ta-H (1), proves to be the first single-site catalyst for the direct non-oxidative coupling transformation of methane into ethane and hydrogen at moderate temperatures, with a high selectivity (>98%). The reaction likely involves the tantalum-methyl-methylidene species as a key intermediate, where the methyl ligand can migrate onto the tantalum-methylidene affording the tantalum-ethyl.

摘要

二氧化硅负载的氢化钽,(SiO)₂Ta-H (1),被证明是第一种能够在中等温度下将甲烷直接非氧化偶联转化为乙烷和氢气的单中心催化剂,具有高选择性(>98%)。该反应可能涉及钽-甲基-亚甲基物种作为关键中间体,其中甲基配体可以迁移到钽-亚甲基上,生成钽-乙基。

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