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Engineered disorder in CO2 photocatalysis

Author

Listed:
  • Zhao Li

    (Soochow University
    University of Toronto
    Soochow University)

  • Chengliang Mao

    (University of Toronto)

  • Qijun Pei

    (Chinese Academy of Sciences)

  • Paul N. Duchesne

    (Queen’s University)

  • Teng He

    (Chinese Academy of Sciences)

  • Meikun Xia

    (University of Toronto)

  • Jintao Wang

    (Chinese Academy of Sciences)

  • Lu Wang

    (The Chinese University of Hong Kong, Shenzhen)

  • Rui Song

    (Soochow University
    University of Toronto
    Soochow University)

  • Feysal M. Ali

    (University of Toronto)

  • Débora Motta Meira

    (Argonne National Laboratory
    Canadian Light Source Inc.)

  • Qingjie Ge

    (Chinese Academy of Sciences)

  • Kulbir Kaur Ghuman

    (Matériaux et Télécommunications)

  • Le He

    (Soochow University
    Soochow University)

  • Xiaohong Zhang

    (Soochow University
    Soochow University)

  • Geoffrey A. Ozin

    (University of Toronto)

Abstract

Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sodium and TiO2 forms a core-shell c-TiO2@a-TiO2-x(OH)y heterostructure, comprised of HO-Ti-[O]-Ti surface frustrated Lewis pairs (SFLPs) embedded in an amorphous shell surrounding a crystalline core, which enables a new genre of chemical reactivity. Specifically, these SFLPs heterolytically dissociate dihydrogen at room temperature to form charge-balancing protonated hydroxyl groups and hydrides at unsaturated titanium surface sites, which display high reactivity towards CO2 reduction. This crystalline-amorphous heterostructure also boosts light absorption, charge carrier separation and transfer to SFLPs, while prolonged carrier lifetimes and photothermal heat generation further enhance reactivity. The collective results of this study motivate a general approach for catalytically generating sustainable chemicals and fuels through engineered disorder in heterogeneous CO2 photocatalysts.

Suggested Citation

  • Zhao Li & Chengliang Mao & Qijun Pei & Paul N. Duchesne & Teng He & Meikun Xia & Jintao Wang & Lu Wang & Rui Song & Feysal M. Ali & Débora Motta Meira & Qingjie Ge & Kulbir Kaur Ghuman & Le He & Xiaoh, 2022. "Engineered disorder in CO2 photocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34798-1
    DOI: 10.1038/s41467-022-34798-1
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    References listed on IDEAS

    as
    1. James M. Ball & Annamaria Petrozza, 2016. "Defects in perovskite-halides and their effects in solar cells," Nature Energy, Nature, vol. 1(11), pages 1-13, November.
    2. Landong Li & Junqing Yan & Tuo Wang & Zhi-Jian Zhao & Jian Zhang & Jinlong Gong & Naijia Guan, 2015. "Sub-10 nm rutile titanium dioxide nanoparticles for efficient visible-light-driven photocatalytic hydrogen production," Nature Communications, Nature, vol. 6(1), pages 1-10, May.
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