High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst.

Bai, Shuxing; Liu, Fangfang; Huang, Bolong; Li, Fan; Lin, Haiping; Wu, Tong; Sun, Mingzi; Wu, Jianbo et al. · Nat Commun · 2020

basic_science · Level V

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Abstract

Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH<sub>4</sub> to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C-H activation of CH<sub>4</sub>. 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<sub>2</sub>) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO<sub>2</sub> NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH<sub>3</sub>OH and CH<sub>3</sub>OOH) under mild conditions. Compared to Rh/CeO<sub>2</sub> nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO<sub>2</sub> nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g<sub>Rh</sub><sup>-1</sup> h<sup>-1</sup>), 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.