化学
催化作用
格式化
无机化学
路易斯酸
傅里叶变换红外光谱
甲烷
烷氧基
非阻塞I/O
吸附
烷基
光化学
有机化学
化学工程
工程类
作者
Yimeng Lyu,Rui Xu,Olivia C. Williams,Ziyuan Wang,Carsten Sievers
标识
DOI:10.1016/j.jcat.2021.10.004
摘要
Methane activation over NiO/Ce0.82Zr0.18O2 catalysts synthesized by combustion synthesis is studied by in-situ IR spectroscopy and correlated to the properties and oxygen speciation of the catalyst. Through XRD, H2-TPR, and pyridine adsorption followed by FTIR spectroscopy, the reducibility and Lewis acidity of the catalysts are assessed. In-situ FTIR spectroscopy is used to monitor the methane activation on catalyst surfaces. Complex IR features of methane-derived surface species are observed and are attributed to the formation of surface alkyl/alkoxy, aldehyde, formate/carbonate, and aromatic species. A data analysis algorithm is developed to evaluate the evolution of different surface species over time. The formation of formate and carbonate species is driven by adsorbed surface oxygen, while less reactive oxygen species associated with NiO allow for the production of aromatics and alkoxy intermediates. By tuning the reducibility and Lewis acidity of the catalyst, the selectivity to alkoxy intermediates can be improved.
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