Identification of Active Sites in HCHO Oxidation over TiO2-Supported Pt Catalysts

被引：50

作者：

Chen, Muhua ^{[1
]}

Wang, Weizhen ^{[2
]}

Qiu, Yuping ^{[1
]}

Wen, He ^{[1
]}

Li, Guangyao ^{[1
]}

Yang, Zhiqing ^{[3
]}

Wang, Ping ^{[1
]}

机构：

[1] South China Univ Technol, Sch Mat Sci & Engn, Guangzhou 510641, Peoples R China

[2] Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China

[3] Ji Hua Lab, Foshan 528000, Peoples R China

来源：

ACS CATALYSIS | 2022年 / 12卷 / 09期

关键词：

cooperative catalysis; oxygen vacancy; metal/oxide interface; formaldehyde oxidation; catalytic mechanism; METAL-SUPPORT INTERACTIONS; WATER-GAS SHIFT; FORMALDEHYDE OXIDATION; CO OXIDATION; INTERFACE; TIO2; DECOMPOSITION; NANOPARTICLES; PERFORMANCE; ADSORPTION;

D O I：

10.1021/acscatal.2c01150

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The cooperative catalysis between noble metals and oxygen vacancies in reducible oxides plays an important role in many heterogeneous catalytic reactions, but definite identification of active sites remains challenging. Herein, we report an experimental identification of active sites in HCHO oxidation over TiO2-supported Pt catalysts by means of microscopic and spectroscopic techniques. Pt/TiO2, catalysts with tunable oxygen vacancy concentrations were designed and fabricated based on hydrogen spillover. A combination of aberration-corrected scanning transmission electron microscopy and electron energy loss spectroscopy allowed us to directly observe the spatial distribution of oxygen vacancies and probe its correlation with the catalytic activity. In situ diffuse reflectance infrared Fourier transform spectroscopy in combination with the online gas chromatography technique was employed to investigate the functionalities of Pt and oxygen vacancies in HCHO oxidation. Our study revealed that HCHO oxidation occurred at the Pt/TiO2-x interface via a cooperative mechanism: oxygen vacancies served as active sites for chemically absorbing HCHO molecules and the adjacent Pt site dissociatively activated O-2.

引用

页码：5565 / 5573

页数：9

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