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Shuxing Bai¹, Fangfang Liu², Bolong Huang³

¹College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China.

Nature Communications

|February 21, 2020

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 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.

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