Tuned selectivity and enhanced activity of CO2 methanation over Ru catalysts by modified metal-carbonate interfaces

• 作者: Qiaojuan Wang Yating Gao Chantsalmaa Tumurbaatar Tungalagtamir Bold Fei Wei Yihu Dai Yanhui Yang
• 来源期刊: 能源化学
• 年，卷（期）: 2022,（1）
• 页码范围: 38-46
• 页数: 9页
• 语种: 英文

摘要

Carbonate-modified metal-support interfaces allow Ru/MnCO3 catalyst to exhibit over 99％ selectivity,great specific activity and long-term anti-CO poisoning stability in atmospheric CO2 methanation.As a contrast,Ru/MnO catalyst with metal-oxide interfaces prefers reverse water-gas shift rather than metha-nation route,along with a remarkably lower activity and a less than 15％ CH4 selectivity.The carbonate-modified interfaces are found to stabilize the Ru species and activate CO2 and H2 molecules.Ru-CO* spe-cies are identified as the reaction intermediates steadily formed from CO2 dissociation,which show mod-erate adsorption strength and high reactivity in further hydrogenation to CH4.Furthermore,carbonates of Ru/MnCO3 are found to be consumed by hydrogenation to form CH4 and replenished by exchange with CO2,which are in a dynamic equilibrium during the reaction.Modification with surface carbonates is proved as an efficient strategy to endow metal-support interfaces of Ru-based catalysts with unique cat-alytic functions for selective CO2 hydrogenation.