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Surface frustrated Lewis pairs in titanium nitride enable gas phase heterogeneous CO2 photocatalysis

Author

Listed:
  • Yunjie Zou

    (Tongji University)

  • Chengliang Mao

    (80 Saint George Street)

  • Mingkai Xu

    (Tongji University)

  • Chao Xing

    (Tongji University)

  • Ruizhao Wang

    (Tongji University)

  • Geoffrey A. Ozin

    (80 Saint George Street)

  • Lan Ling

    (Tongji University)

Abstract

Gas-phase heterogeneous catalytic CO2 hydrogenation to commodity chemicals and fuels via surface frustrated Lewis pairs is a growing focus of scientific and technological interest. Traditional gas-phase heterogeneous surface frustrated Lewis pair catalysts primarily involve metal oxide-hydroxides (MOH•••M). An avenue to improve the process performance metrics lies in replacing the Lewis base MOH with a stronger alternative; an intriguing example being the amine MNH2 in metal nitrides. This study establishes a proof-of-concept that an amine-type photoactive surface frustrated Lewis pair (MNH2•••M) can be constructed in titanium nitride (TiNxOy) when integrated with a nanoscale platinum spillover co-catalyst. This surface frustrated Lewis pair, comprising Ti-NH2 as the Lewis base and low-valent Ti as the Lewis acid, facilitates the gas-phase light-assisted heterogeneous reverse water-gas shift reaction. The reaction proceeds via a surface-active carbamate intermediate, Ti-(H2N-COO)-Ti, whereby the synergism of Lewis acidic and Lewis basic sites endows it with superior performance indicators compared to TiNxOy alone, as well as conventional platinum supported metal oxides.

Suggested Citation

  • Yunjie Zou & Chengliang Mao & Mingkai Xu & Chao Xing & Ruizhao Wang & Geoffrey A. Ozin & Lan Ling, 2024. "Surface frustrated Lewis pairs in titanium nitride enable gas phase heterogeneous CO2 photocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54951-2
    DOI: 10.1038/s41467-024-54951-2
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