High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst

作者：Shuxing Bai, Fangfang Liu, Bolong Huang, Fan Li, Haiping Lin, Tong Wu, Mingzi Sun, Jianbo Wu, Qi Shao, Yong Xu, Xiaoqing Huang · 发表于：Nature Communications · 年份：2020 · DOI：10.1038/s41467-020-14742-x · 被引用次数：294 · 研究领域：Catalytic Processes in Materials Science、Advanced Photocatalysis Techniques、Catalysis and Oxidation Reactions

Abstract Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH 4 to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH 4 . The quest for high-efficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO 2 ) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO 2 NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH 3 OH and CH 3 OOH) under mild conditions. Compared to Rh/CeO 2 nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO 2 nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g Rh −1 h −1 ), which largely outperforms that of the reported catalysts in the same class. This work demonstrates a highly efficient DMC process and promotes the research on Rh single-atom catalysts in heterogeneous catalysis.