Regulating Catalytic Performance for CO Hydrogenation to Higher Oxygenates through Strong Metal–Support Interaction

作者：Ruyang Wang, Jing Yang, Peiyu Ma, Heng Cao, Zhentao Ma, Yide Zhu, Hao Lou, Zhandong Wang, Lei Luo, Jun Bao · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.5c02880 · 被引用次数：5 · 研究领域：Catalytic Processes in Materials Science、Catalysts for Methane Reforming、Nanomaterials for catalytic reactions

Optimizing the CO hydrogenation to higher oxygenates (C 2+ -Oxy) is both an intriguing opportunity and significant challenges. The strong metal–support interaction (SMSI) provides a promising avenue to regulate catalytic performance of CO hydrogenation, as it facilitates the encapsulation of nanoparticles and the modulation of active sites. In this study, we proved that Rh/MnO 2 exhibited SMSI subsequent to H 2 reduction. The coverage of MnO x suboxides on the surface of Rh particles was regulated by the reduction temperature, which in turn affected the quantity of consecutive Rh sites and the Rh + /Rh 0 ratio. This modulation contributed to an improvement in both the catalytic activity and selectivity for C 2+ -Oxy. Based on synchrotron-based vacuum ultraviolet photoionization mass spectrometry results, the presence of ketene (CH 2 CO) indicated that the initial carbon–carbon coupling might occur between the adsorbed *CH 2 and *CO. Subsequently, two different C 2 oxygenated intermediates were constructed, and the dominant one was also regulated by the MnO x coating, thereby adjusting the ratio of aldehyde and alcohol products. This study expands upon the catalyst system of SMSI and offers a significant contribution to understanding of the reaction mechanism involved in the C 2+ -Oxy synthesis.