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 () and Xiaoqing Huang ()
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Shuxing Bai: Soochow University
Fangfang Liu: Soochow University
Bolong Huang: The Hong Kong Polytechnic University, Hung Hom
Fan Li: Shanghai Jiao Tong University
Haiping Lin: Soochow University
Tong Wu: The Hong Kong Polytechnic University, Hung Hom
Mingzi Sun: The Hong Kong Polytechnic University, Hung Hom
Jianbo Wu: Shanghai Jiao Tong University
Qi Shao: Soochow University
Yong Xu: Soochow University
Xiaoqing Huang: Soochow University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract 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 high-efficiency 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.

Date: 2020
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DOI: 10.1038/s41467-020-14742-x

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