Insights into the Mechanism of Methanol Steam Reforming Tandem Reaction over CeO 2 Supported Single-Site Catalysts

作者：Luning Chen, Zhiyuan Qi, Xinxing Peng, Jeng‐Lung Chen, Chih‐Wen Pao, Xibo Zhang, Chaochao Dun, Melissa Young, David Prendergast, Jeffrey J. Urban, Jinghua Guo, Gábor A. Somorjai, Ji Su · 发表于：Journal of the American Chemical Society · 年份：2021 · DOI：10.1021/jacs.1c03895 · 被引用次数：179 · 研究领域：Catalytic Processes in Materials Science、Catalysts for Methane Reforming、Electrocatalysts for Energy Conversion

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 (CO 2 ) selectivity of a tandem reaction: methanol steam reforming. Specifically, the hydrogen generation rate over single site Ru 1 /CeO 2 catalyst is up to 9360 mol H 2 per mol Ru per hour (579 mL H2 g Ru –1 s –1 ) with 99.5% CO 2 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 CO 2 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.