High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
Shuxing Bai1,6, Fangfang Liu2,6, Bolong Huang 3,6, Fan Li4, Haiping Lin 2, Tong Wu3, Mingzi Sun 3, Jianbo Wu 4,5*（邬剑波）, Qi Shao1 , Yong Xu 2* （徐勇）& Xiaoqing Huang1*（黄小青）
1 College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu 215123, China
2 Institute 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
4 State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
5 Center of Hydrogen Science, Shanghai Jiao Tong University, Shanghai 200240, China
6 These 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