脱氢
催化作用
水煤气变换反应
蒸汽重整
甲醇
化学
氢
制氢
离解(化学)
无机化学
吸附
反应机理
反应速率
选择性
光化学
物理化学
有机化学
作者
Luning Chen,Zhiyuan Qi,Xiaoyuan Peng,Jeng-Lung Chen,Chih‐Wen Pao,Xibo Zhang,Chaochao Dun,Melissa Young,David Prendergast,Jeffrey J. Urban,Jinghua Guo,Gábor A. Somorjai,Junfeng Su
摘要
We demonstrated how the special synergy between a noble metal single site and neighboring oxygen vacancies provides an “ensemble reaction pool” for high hydrogen generation efficiency and carbon dioxide (CO2) selectivity of a tandem reaction: methanol steam reforming. Specifically, the hydrogen generation rate over single site Ru1/CeO2 catalyst is up to 9360 mol H2 per mol Ru per hour (579 mLH2 gRu–1 s–1) with 99.5% CO2 selectivity. Reaction mechanism study showed that the integration of metal single site and O vacancies facilitated the tandem reaction, which consisted of methanol dehydrogenation, water dissociation, and the subsequent water gas shift (WGS) reaction. In addition, the strength of CO adsorption and the reaction activation energy difference between methanol dehydrogenation and WGS reaction play an important role in determining the activity and CO2 selectivity. Our study paves the way for the further rational design of single site catalysts at the atomic scale. Furthermore, the development of such highly efficient and selective hydrogen evolution systems promises to deliver highly desirable economic and ecological benefits.
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