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Water enables mild oxidation of methane to methanol on gold single-atom catalysts

Author

Listed:
  • Laihao Luo

    (University of Science and Technology of China)

  • Jie Luo

    (University of Science and Technology of China)

  • Hongliang Li

    (University of Science and Technology of China)

  • Fangning Ren

    (University of Science and Technology of China)

  • Yifei Zhang

    (University of Science and Technology of China)

  • Andong Liu

    (University of Science and Technology of China)

  • Wei-Xue Li

    (University of Science and Technology of China)

  • Jie Zeng

    (University of Science and Technology of China)

Abstract

As a 100% atom-economy process, direct oxidation of methane into methanol remains as a grand challenge due to the dilemma between activation of methane and over-oxidation of methanol. Here, we report that water enabled mild oxidation of methane into methanol with >99% selectivity over Au single atoms on black phosphorus (Au1/BP) nanosheets under light irradiation. The mass activity of Au1/BP nanosheets reached 113.5 μmol gcatal−1 in water pressured with 33 bar of mixed gas (CH4:O2 = 10:1) at 90 °C under light irradiation (1.2 W), while the activation energy was 43.4 kJ mol−1. Mechanistic studies revealed that water assisted the activation of O2 to generate reactive hydroxyl groups and •OH radicals under light irradiation. Hydroxyl groups reacted with methane at Au single atoms to form water and CH3* species, followed by oxidation of CH3* via •OH radicals into methanol. Considering the recycling of water during the whole process, we can also regard water as a catalyst.

Suggested Citation

  • Laihao Luo & Jie Luo & Hongliang Li & Fangning Ren & Yifei Zhang & Andong Liu & Wei-Xue Li & Jie Zeng, 2021. "Water enables mild oxidation of methane to methanol on gold single-atom catalysts," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21482-z
    DOI: 10.1038/s41467-021-21482-z
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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. Jingyi Yang & Yike Huang & Haifeng Qi & Chaobin Zeng & Qike Jiang & Yitao Cui & Yang Su & Xiaorui Du & Xiaoli Pan & Xiaoyan Liu & Weizhen Li & Botao Qiao & Aiqin Wang & Tao Zhang, 2022. "Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration," Nature Communications, Nature, vol. 13(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. Peng Rao & Yijie Deng & Wenjun Fan & Junming Luo & Peilin Deng & Jing Li & Yijun Shen & Xinlong Tian, 2022. "Movable type printing method to synthesize high-entropy single-atom catalysts," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    5. Pengfei Xie & Jing Ding & Zihao Yao & Tiancheng Pu & Peng Zhang & Zhennan Huang & Canhui Wang & Junlei Zhang & Noah Zecher-Freeman & Han Zong & Dashui Yuan & Shengwei Deng & Reza Shahbazian-Yassar & C, 2022. "Oxo dicopper anchored on carbon nitride for selective oxidation of methane," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    6. Lei Luo & Xiaoyu Han & Keran Wang & Youxun Xu & Lunqiao Xiong & Jiani Ma & Zhengxiao Guo & Junwang Tang, 2023. "Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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