High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
Shuxing Bai1,6, Fangfang Liu2,6, Bolong Huang3,6, Fan Li4, Haiping Lin2, Tong Wu3, Mingzi Sun3, Jianbo Wu4,5*（邬剑波）, Qi Shao1, Yong Xu2*（徐勇）& Xiaoqing Huang1*（黄小青）
1College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu 215123, China
2Institute of Functional Nano&Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu 215123, China
3Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China
4State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
5Center of Hydrogen Science, Shanghai Jiao Tong University, Shanghai 200240, China
6These authors contributed equally: Shuxing Bai, Fangfang Liu, Bolong Huang
NATURE COMMUNICATIONS，(2020)11:954
Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH4 to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH4. The quest for highefficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO2) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO2 NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH3OH and CH3OOH) under mild conditions. Compared to Rh/CeO2 nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO2 nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol gRh−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.
链接：https://www.nature.com/articles/s41467-020-14742-x.pdf
