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

Yunjie Zou, Chengliang Mao, Mingkai Xu, Chao Xing, Ruizhao Wang, Geoffrey A. Ozin () and Lan Ling ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-54951-2

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