甲烷
电离能
星团(航天器)
催化作用
反应性(心理学)
兴奋剂
氢
化学
电离
氢原子
Atom(片上系统)
物理化学
氧气
分析化学(期刊)
材料科学
有机化学
群(周期表)
离子
程序设计语言
替代医学
嵌入式系统
病理
医学
光电子学
计算机科学
作者
Bowei Yuan,Shiya Tang,Shaodong Zhou
标识
DOI:10.1002/chem.202201136
摘要
Abstract The size and doping effects in methane activation by Ti−Si−O clusters have been explored by using a combination of gas‐phase experiments and quantum chemical calculations. All [Ti m Si n O 2( m + n ) ] .+ ( m + n =2, 3, 8, 10, 12, 14) clusters can extract a hydrogen from methane. The associated energies and structures have been revealed in detail. Moreover, the doping and size effects have been discussed involving generalized Kohn‐Sham energy decomposition analysis, natural population analysis, Wiberg bond indexes (WBI), molecular polarity index (MPI) and ionization potential (IP). It suggested that Ti−Si−O clusters with a low Ti : Si ratio is beneficial to adsorbing methane and inclination to the hydrogen atom transfer (HAT) process, while the clusters with a high Ti : Si ratio favors the generation of a terminal oxygen radical and results in high reactivity and turnover frequency. On the other hand, a cluster size of m + n =12 is recommended considering both the ionization potential and the turnover frequency of the reaction. Hopefully, these finding will be instructive for the design of high‐performance Ti−Si−O catalyst toward methane conversion.
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