High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
Shuxing Bai, Fangfang Liu, Bolong Huang, Fan Li, Haiping Lin, Tong Wu, Mingzi Sun, Jianbo Wu, Qi Shao, Yong Xu, Xiaoqing Huang
Abstract
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.