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

Author

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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
    Shanghai Jiao Tong University)

  • Qi Shao

    (Soochow University)

  • Yong Xu

    (Soochow University)

  • Xiaoqing Huang

    (Soochow University)

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.

Suggested Citation

  • Shuxing Bai & Fangfang Liu & Bolong Huang & Fan Li & Haiping Lin & Tong Wu & Mingzi Sun & Jianbo Wu & Qi Shao & Yong Xu & Xiaoqing Huang, 2020. "High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14742-x
    DOI: 10.1038/s41467-020-14742-x
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    Cited by:

    1. Yueshan Xu & Daoxiong Wu & Qinghua Zhang & Peng Rao & Peilin Deng & Mangen Tang & Jing Li & Yingjie Hua & Chongtai Wang & Shengkui Zhong & Chunman Jia & Zhongxin Liu & Yijun Shen & Lin Gu & Xinlong Ti, 2024. "Regulating Au coverage for the direct oxidation of methane to methanol," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Chongyang Tang & Cong Wei & Yanyan Fang & Bo Liu & Xianyin Song & Zenan Bian & Xuanwei Yin & Hongbo Wang & Zhaohui Liu & Gongming Wang & Xiangheng Xiao & Xiangfeng Duan, 2024. "Electrocatalytic hydrogenation of acetonitrile to ethylamine in acid," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Jiwon Kim & Jae Hyung Kim & Cheoulwoo Oh & Hyewon Yun & Eunchong Lee & Hyung-Suk Oh & Jong Hyeok Park & Yun Jeong Hwang, 2023. "Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Yang, Le & Lin, Hongju & Fang, Zhihao & Yang, Yanhui & Liu, Xiaohao & Ouyang, Gangfeng, 2023. "Recent advances on methane partial oxidation toward oxygenates under mild conditions," Renewable and Sustainable Energy Reviews, Elsevier, vol. 184(C).
    5. Zhang, Rui & He, Yuting & Luo, Yuehui & Lou, DanFeng & Zhu, Rui & Zhu, Can & Li, Quanxin, 2023. "Selective preparation of jet fuels from low carbon alcohols and ABE at atmospheric pressure," Energy, Elsevier, vol. 281(C).
    6. Xiao Sun & Xuanye Chen & Cong Fu & Qingbo Yu & Xu-Sheng Zheng & Fei Fang & Yuanxu Liu & Junfa Zhu & Wenhua Zhang & Weixin Huang, 2022. "Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates," Nature Communications, Nature, vol. 13(1), pages 1-12, December.

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