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Facet-dependent active sites of a single Cu2O particle photocatalyst for CO2 reduction to methanol

Author

Listed:
  • Yimin A. Wu

    (Center for Nanoscale Materials, Argonne National Laboratory
    University of Waterloo)

  • Ian McNulty

    (Center for Nanoscale Materials, Argonne National Laboratory)

  • Cong Liu

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Kah Chun Lau

    (Materials Science Division, Argonne National Laboratory
    California State University)

  • Qi Liu

    (City University of Hong Kong)

  • Arvydas P. Paulikas

    (Materials Science Division, Argonne National Laboratory)

  • Cheng-Jun Sun

    (Advanced Photon Source, Argonne National Laboratory)

  • Zhonghou Cai

    (Advanced Photon Source, Argonne National Laboratory)

  • Jeffrey R. Guest

    (Center for Nanoscale Materials, Argonne National Laboratory)

  • Yang Ren

    (Advanced Photon Source, Argonne National Laboratory)

  • Vojislav Stamenkovic

    (Materials Science Division, Argonne National Laboratory)

  • Larry A. Curtiss

    (Materials Science Division, Argonne National Laboratory)

  • Yuzi Liu

    (Center for Nanoscale Materials, Argonne National Laboratory)

  • Tijana Rajh

    (Center for Nanoscale Materials, Argonne National Laboratory)

Abstract

Atomic-level understanding of the active sites and transformation mechanisms under realistic working conditions is a prerequisite for rational design of high-performance photocatalysts. Here, by using correlated scanning fluorescence X-ray microscopy and environmental transmission electron microscopy at atmospheric pressure, in operando, we directly observe that the (110) facet of a single Cu2O photocatalyst particle is photocatalytically active for CO2 reduction to methanol while the (100) facet is inert. The oxidation state of the active sites changes from Cu(i) towards Cu(ii) due to CO2 and H2O co-adsorption and changes back to Cu(i) after CO2 conversion under visible light illumination. The Cu2O photocatalyst oxidizes water as it reduces CO2. Concomitantly, the crystal lattice expands due to CO2 adsorption then reverts after CO2 conversion. The internal quantum yield for unassisted wireless photocatalytic reduction of CO2 to methanol using Cu2O crystals is ~72%.

Suggested Citation

  • Yimin A. Wu & Ian McNulty & Cong Liu & Kah Chun Lau & Qi Liu & Arvydas P. Paulikas & Cheng-Jun Sun & Zhonghou Cai & Jeffrey R. Guest & Yang Ren & Vojislav Stamenkovic & Larry A. Curtiss & Yuzi Liu & T, 2019. "Facet-dependent active sites of a single Cu2O particle photocatalyst for CO2 reduction to methanol," Nature Energy, Nature, vol. 4(11), pages 957-968, November.
    • Handle: RePEc:nat:natene:v:4:y:2019:i:11:d:10.1038_s41560-019-0490-3
    DOI: 10.1038/s41560-019-0490-3
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    Cited by:

    1. Jingwen Ke & Jiankang Zhao & Mingfang Chi & Menglin Wang & Xiangdong Kong & Qixuan Chang & Weiran Zhou & Chengxuan Long & Jie Zeng & Zhigang Geng, 2022. "Facet-dependent electrooxidation of propylene into propylene oxide over Ag3PO4 crystals," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    2. Jijia Xie & Xiyi Li & Jian Guo & Lei Luo & Juan J. Delgado & Natalia Martsinovich & Junwang Tang, 2023. "Highly selective oxidation of benzene to phenol with air at room temperature promoted by water," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Guifeng Ma & Olga A. Syzgantseva & Yan Huang & Dragos Stoian & Jie Zhang & Shuliang Yang & Wen Luo & Mengying Jiang & Shumu Li & Chunjun Chen & Maria A. Syzgantseva & Sen Yan & Ningyu Chen & Li Peng &, 2023. "A hydrophobic Cu/Cu2O sheet catalyst for selective electroreduction of CO to ethanol," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Xiaodong Li & Li Li & Guangbo Chen & Xingyuan Chu & Xiaohui Liu & Chandrasekhar Naisa & Darius Pohl & Markus Löffler & Xinliang Feng, 2023. "Accessing parity-forbidden d-d transitions for photocatalytic CO2 reduction driven by infrared light," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Mingru Bai & Ting Wang & Zhenyu Xing & Haoju Huang & Xizheng Wu & Mohsen Adeli & Mao Wang & Xianglong Han & Ling Ye & Chong Cheng, 2024. "Electron-donable heterojunctions with synergetic Ru-Cu pair sites for biocatalytic microenvironment modulations in inflammatory mandible defects," Nature Communications, Nature, vol. 15(1), pages 1-22, December.
    6. Jie Zhou & Jie Li & Liang Kan & Lei Zhang & Qing Huang & Yong Yan & Yifa Chen & Jiang Liu & Shun-Li Li & Ya-Qian Lan, 2022. "Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Xinfeng Chen & Chengdong Peng & Wenyan Dan & Long Yu & Yinan Wu & Honghan Fei, 2022. "Bromo- and iodo-bridged building units in metal-organic frameworks for enhanced carrier transport and CO2 photoreduction by water vapor," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    8. Yuan-Sheng Xia & Meizhong Tang & Lei Zhang & Jiang Liu & Cheng Jiang & Guang-Kuo Gao & Long-Zhang Dong & Lan-Gui Xie & Ya-Qian Lan, 2022. "Tandem utilization of CO2 photoreduction products for the carbonylation of aryl iodides," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    9. Jie Ding & Zhiming Wei & Fuhua Li & Jincheng Zhang & Qiao Zhang & Jing Zhou & Weijue Wang & Yuhang Liu & Zhen Zhang & Xiaozhi Su & Runze Yang & Wei Liu & Chenliang Su & Hong Bin Yang & Yanqiang Huang , 2023. "Atomic high-spin cobalt(II) center for highly selective electrochemical CO reduction to CH3OH," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    10. Yangyang Zhang & Yanxu Chen & Xiaowen Wang & Yafei Feng & Zechuan Dai & Mingyu Cheng & Genqiang Zhang, 2024. "Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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