贵金属在甲烷活化与转化中呈现出优良的反应性。研究气态条件下贵金属物种与甲烷的反应,可以从分子水平上揭示凝聚相贵金属催化体系的活性位点与基元反应机理,为理性设计和改进催化剂提供理论基础。本文综述了贵金属原子、离子、团簇、氢化物、卤化物、氧化物、甲基配合物以及掺杂团簇活化、转化甲烷取得的新进展,并针对不同贵金属体系的甲烷活化机理展开讨论。
Noble metals have been identified to exhibit excellent performance in methane chemistry. Gas phase study of chemical reactions between noble metal species and methane permits to uncover the active sites and elementary reaction mechanisms involved in condensed-phase catalytic reactions at a strictly molecular level. In this review,we summarize the recent progress in activation and transformation of methane by noble metal species including single atoms, atomic ions, cluster ions, hydrides, halides, oxides, metal-methyl complexes, and heteronuclear clusters. The mechanistic difference of methane activation by different noble metal systems is also discussed in detail.