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首页> 外文会议>NATO Advanced Study Institute on Sustainable Strategies for the Upgrading of Natural Gas: Fundamentals, Challenges, and Opportunities; 20030706-18; Vilamoura(PT) >SURFACE ORGANOMETALLIC CHEMISTRY OF TANTALUM: APPLICATION TO THE METATHESIS OF ALKANES CATALYZED BY A TANTALUM HYDRIDE SUPPORTED ON SILICA
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SURFACE ORGANOMETALLIC CHEMISTRY OF TANTALUM: APPLICATION TO THE METATHESIS OF ALKANES CATALYZED BY A TANTALUM HYDRIDE SUPPORTED ON SILICA

机译：钽的表面有机化学：在氧化硅负载的氢化钽催化的链烷烃的复分解中的应用

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摘要

In the course of this short review, we have described the formation of various silica-supported tantalum complexes and presented some interesting catalytic properties of these surface species particularly, the tantalum hydride. This hydride was formed after reaction of the tris(neopentyl)neopentylidene tantalum complex 1 with the hydroxyl groups present on silica, then treatment of the obtained alkyl-alkylidene surface species 2a and 2b under hydrogen at 150℃. The tantalum hydride (≡SiO)_2Ta-H 3 can evolve further at 500℃ under hydrogen into the tri(siloxy) species (≡SiO)_3Ta 5, All these surface species were fully characterized by numerous physico-chemical methods. The highly unsaturated tantalum hydride shows interesting properties in the stoichiometric C-H bond activation of cycloalkanes and methane but above all, it revealed itself as a catalyst precursor for the new reaction of alkane metathesis which leads to the transformation of an alkane into its higher and lower homologues. The alkyl-alkylidene surface complexes 2a and 2b also proved to be catalytic precursors for the alkane metathesis affording the initial stoichiometric liberation of cross-metathesis products which opens the route to the investigation of catalytic cross-metathesis processes.
机译：在这篇简短的评论中，我们描述了各种二氧化硅负载的钽配合物的形成，并介绍了这些表面物质特别是氢化钽的一些有趣的催化性能。该氢化物是在三（新戊基）新戊基亚烷基钽配合物1与二氧化硅上存在的羟基反应后，然后在150℃，氢气下处理得到的烷基-亚烷基表面物质2a和2b而形成的。氢化钽（≡SiO）_2Ta-H 3可以在500℃下于氢气中进一步析出为三（甲硅烷氧基）物种（≡SiO）_3Ta 5，所有这些表面物种都已通过多种物理化学方法充分表征。高度不饱和的氢化钽在环烷烃和甲烷的化学计量CH键活化中显示出有趣的特性，但最重要的是，它显示出自己是烷烃复分解新反应的催化剂前体，该反应导致烷烃转化为其高低同系物。 。烷基-亚烷基表面配合物2a和2b也被证明是烷烃复分解反应的催化前体，提供了交叉复分解产物的最初的化学计量解放，这为研究催化交叉复分解过程开辟了道路。

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