催化作用
材料科学
空位缺陷
氧化物
纳米团簇
化学工程
纳米颗粒
无机化学
化学
光化学
纳米技术
结晶学
有机化学
工程类
冶金
作者
Tao Gan,Jingxiu Yang,David J. Morris,Xuefeng Chu,Peng Zhang,Wenxiang Zhang,Yongcun Zou,Wenfu Yan,Su‐Huai Wei,Gang Liu
标识
DOI:10.1038/s41467-021-22946-y
摘要
Abstract Activation of O 2 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 O 2 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 O 2 . 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.
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