Electron donation of non-oxide supports boosts O2 activation on nano-platinum catalysts

Tao Gan, Jingxiu Yang (), David Morris, Xuefeng Chu, Peng Zhang, Wenxiang Zhang (), Yongcun Zou, Wenfu Yan, Su-Huai Wei and Gang Liu ()
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Tao Gan: Jilin University
Jingxiu Yang: Jilin Jianzhu University
David Morris: Dalhousie University
Xuefeng Chu: Jilin Jianzhu University
Peng Zhang: Dalhousie University
Wenxiang Zhang: Jilin University
Yongcun Zou: Jilin University
Wenfu Yan: Jilin University
Su-Huai Wei: Beijing Computational Science Research Center
Gang Liu: Jilin University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Activation of O2 is a critical step in heterogeneous catalytic oxidation. Here, the concept of increased electron donors induced by nitrogen vacancy is adopted to propose an efficient strategy to develop highly active and stable catalysts for molecular O2 activation. Carbon nitride with nitrogen vacancies is prepared to serve as a support as well as electron sink to construct a synergistic catalyst with Pt nanoparticles. Extensive characterizations combined with the first-principles calculations reveal that nitrogen vacancies with excess electrons could effectively stabilize metallic Pt nanoparticles by strong p-d coupling. The Pt atoms and the dangling carbon atoms surround the vacancy can synergistically donate electrons to the antibonding orbital of the adsorbed O2. This synergistic catalyst shows great enhancement of catalytic performance and durability in toluene oxidation. The introduction of electron-rich non-oxide substrate is an innovative strategy to develop active Pt-based oxidation catalysts, which could be conceivably extended to a variety of metal-based catalysts for catalytic oxidation.

Date: 2021
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DOI: 10.1038/s41467-021-22946-y

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