甲烷活化机理研究进展

对近年来CH4活化机理方面的研究做了综述。在甲烷氧化偶联(OCM)反应中,催化剂表面上究竟何种氧负离子(O2-(超氧)、O22-(过氧)、表面晶格氧O2-)是参与活化CH4的活性氧物种仍然是一个存在争议的问题。在不同金属表面上CH4的直接活化模式被认为有两种,一种是形变模式,另一种是伸缩模式。在通过中间体途径活化CH4的研究中,发现“三中心两电子”脱氢反应和与有机金属阳离子络合物的络合交换反应是两种在温和条件下活化CH4的很有前景的活化方式。

Development of the study on methane activation mechanism

Development of the study on methane activation mechanism in recent years have been reviewed in this article. Which oxygen- anion (O2- , O22- or O2- ) on the oxide surface is the active specie in methane activation during oxidative coupling of methane (OCM)reaction is still an argumentative topic. It is believed that there are two modes in direct activating of methane on metal surface, one is deformation mode of CH4 and the other is C- H stretch mode. In the study of methane activation in way of precursor - mediated process, "three - center two -electron" dehydrogenation reaction and σ - bonded ligand exchange reaction in the system of CH4 + organometal-lic cationic complexes are shown to be promising systems for CH4 activation under mild conditions.