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Electronic asymmetry of lattice oxygen sites in ZnO promotes the photocatalytic oxidative coupling of methane

Author

Listed:
  • Mengyao Sun

    (China University of Petroleum
    Shenyang Normal University)

  • Yanjun Chen

    (China University of Petroleum
    Shenyang Normal University)

  • Xiaoqiang Fan

    (Shenyang Normal University)

  • Dong Li

    (China University of Petroleum
    Shenyang Normal University)

  • Jiaxin Song

    (China University of Petroleum
    Shenyang Normal University)

  • Ke Yu

    (China University of Petroleum
    Shenyang Normal University)

  • Zhen Zhao

    (China University of Petroleum
    Shenyang Normal University)

Abstract

Photocatalytic oxidative coupling of methane with oxygen is promising to obtain valuable muti-carbon products, yet suffering low reactivity. Here, we apply cerium modifications on zinc oxide-supported gold catalysts based on the electronic asymmetry design of lattice oxygen to improve the coupling activity. The methane conversion rate exceeds 16000 μmol g−1 h−1 with muti-carbon selectivity of 94.9% and catalytic durability of 3 days, and it can increase to 34000 μmol g−1 h−1 under more thermal assistance, with a turnover frequency of 507 h−1 for ethane and an apparent quantum efficiency of 33.7% at 350 nm. According to systematic characterizations and theoretical analysis, cerium dopants not only can boost the formation of reactive oxygen species but also intervene in the vivacity of lattice oxygen by manipulating metal-oxygen bond strength, thereby leading to favorable methyl desorption to form ethane and quick water release. This work provides insight into the rational design of efficient photocatalysts for aerobic methane-to-ethane conversion.

Suggested Citation

  • Mengyao Sun & Yanjun Chen & Xiaoqiang Fan & Dong Li & Jiaxin Song & Ke Yu & Zhen Zhao, 2024. "Electronic asymmetry of lattice oxygen sites in ZnO promotes the photocatalytic oxidative coupling of methane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54226-w
    DOI: 10.1038/s41467-024-54226-w
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    1. Wenqing Zhang & Cenfeng Fu & Jingxiang Low & Delong Duan & Jun Ma & Wenbin Jiang & Yihong Chen & Hengjie Liu & Zeming Qi & Ran Long & Yingfang Yao & Xiaobao Li & Hui Zhang & Zhi Liu & Jinlong Yang & Z, 2022. "High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Xiang Yu & Vincent Waele & Axel Löfberg & Vitaly Ordomsky & Andrei Y. Khodakov, 2019. "Selective photocatalytic conversion of methane into carbon monoxide over zinc-heteropolyacid-titania nanocomposites," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    3. Xiang Yu & Vladimir L. Zholobenko & Simona Moldovan & Di Hu & Dan Wu & Vitaly V. Ordomsky & Andrei Y. Khodakov, 2020. "Stoichiometric methane conversion to ethane using photochemical looping at ambient temperature," Nature Energy, Nature, vol. 5(7), pages 511-519, July.
    4. Xuxing Chen & Yunpeng Li & Xiaoyang Pan & David Cortie & Xintang Huang & Zhiguo Yi, 2016. "Photocatalytic oxidation of methane over silver decorated zinc oxide nanocatalysts," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
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