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Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Author

Listed:
  • Lei Luo

    (Northwest University)

  • Lei Fu

    (Northwest University)

  • Huifen Liu

    (Northwest University)

  • Youxun Xu

    (University College London)

  • Jialiang Xing

    (Northwest University)

  • Chun-Ran Chang

    (Xi’an Jiaotong University)

  • Dong-Yuan Yang

    (Xi’an Jiaotong University
    Shaanxi Yanchang Petroleum (Group) Corp. Ltd.)

  • Junwang Tang

    (University College London)

Abstract

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion and selectivity. Herein, under visible irradiation (420 nm), the synergy of palladium (Pd) atom cocatalyst and oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h−1 of C1 oxygenates, with a selectivity of primary products (CH3OH and CH3OOH) up to 82.5%. Mechanism investigation elucidates that such superior photocatalysis is induced by the dedicated function of Pd single atoms and oxygen vacancies on boosting hole and electron transfer, respectively. O2 is proven to be the only oxygen source for CH3OH production, while H2O acts as the promoter for efficient CH4 activation through ·OH production and facilitates product desorption as indicated by DFT modeling. This work thus provides new understandings on simultaneous regulation of both activity and selectivity by the synergy of single atom cocatalysts and oxygen vacancies.

Suggested Citation

  • Lei Luo & Lei Fu & Huifen Liu & Youxun Xu & Jialiang Xing & Chun-Ran Chang & Dong-Yuan Yang & Junwang Tang, 2022. "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30434-0
    DOI: 10.1038/s41467-022-30434-0
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    2. 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.
    3. Chengyang Feng & Shouwei Zuo & Miao Hu & Yuanfu Ren & Liwei Xia & Jun Luo & Chen Zou & Sibo Wang & Yihan Zhu & Magnus Rueping & Yu Han & Huabin Zhang, 2024. "Optimizing the reaction pathway of methane photo-oxidation over single copper sites," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
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    5. Wenqing Zhang & Dawei Xi & Yihong Chen & Aobo Chen & Yawen Jiang & Hengjie Liu & Zeyu Zhou & Hui Zhang & Zhi Liu & Ran Long & Yujie Xiong, 2023. "Light-driven flow synthesis of acetic acid from methane with chemical looping," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Yingying Fan & Yuheng Jiang & Haiting Lin & Jianan Li & Yuanjiang Xie & Anyi Chen & Siyang Li & Dongxue Han & Li Niu & Zhiyong Tang, 2024. "Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    7. 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.
    8. Youxun Xu & Chao Wang & Xiyi Li & Lunqiao Xiong & Tianyu Zhang & Liquan Zhang & Qinghua Zhang & Lin Gu & Yang Lan & Junwang Tang, 2024. "Efficient methane oxidation to formaldehyde via photon–phonon cascade catalysis," Nature Sustainability, Nature, vol. 7(9), pages 1171-1181, September.

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