Yan Dongxu, Gao Yanxia, Qi Ming-Yu, Jia Hongpeng, Xu Yi-Jun
Xiamen Key Laboratory of Materials for Gaseous Pollutant Control, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
Precis Chem. 2023 Apr 12;1(5):299-308. doi: 10.1021/prechem.3c00023. eCollection 2023 Jul 24.
The dynamic evolution of active site coordination structure during a high-temperature reaction is critically significant but often difficult for the research of efficient single-atom catalysts (SACs). Herein, we for the first time report the in situ activation behaviors of the local coordination structure of Pt single atoms (Pt) during the high-temperature oxidation of light alkanes. The distinctly enhanced activity of the catalyst is attributed to the in situ evolved Pt-oxygen vacancy (Pt-OV) combination ensemble as an efficient and stable active site. Theoretical calculations reveal that the lattice oxygen adjacent to Pt and the H dissociated from CH constitute the lattice hydroxyl, which is the initial step in the formation of the Pt-OV combination. Pt and nearby unsaturated Mn can donate the charge back to O-O to promote the dissociation of O. This work provides molecular-level insight into the in situ reaction-induced evolution of a single-atom coordination environment for designing efficient SACs under harsh conditions.
在高温反应过程中，活性位点配位结构的动态演变至关重要，但对于高效单原子催化剂（SACs）的研究而言往往颇具难度。在此，我们首次报道了在轻质烷烃高温氧化过程中Pt单原子（Pt）局部配位结构的原位活化行为。催化剂活性的显著增强归因于原位演化形成的Pt-氧空位（Pt-OV）组合整体，它作为一种高效且稳定的活性位点。理论计算表明，与Pt相邻的晶格氧以及从CH解离出的H构成了晶格羟基，这是Pt-OV组合形成的初始步骤。Pt和附近的不饱和Mn能够将电荷回传给O-O以促进O的解离。这项工作为在苛刻条件下设计高效SACs时单原子配位环境的原位反应诱导演化提供了分子层面的见解。
