Reverse oxygen spillover triggered by CO adsorption on Sn-doped Pt/TiO2 for low-temperature CO oxidation

被引：101

作者：

Chen, Jianjun ^{[1
]}

Xiong, Shangchao ^{[2
]}

Liu, Haiyan ^{[1
]}

Shi, Jianqiang ^{[1
]}

Mi, Jinxing ^{[1
]}

Liu, Hao ^{[1
]}

Gong, Zhengjun

Oliviero, Laetitia ^{[3
]}

Mauge, Francoise ^{[3
]}

Li, Junhua ^{[1
]}

机构：

[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China

[2] Southwest Jiaotong Univ, Fac Geosci & Environm Engn, Chengdu 610031, Peoples R China

[3] Univ Caen, Lab Catalyse & Spectrochim, ENSI, CAEN,CNRS, 6 Bd Marechal Juin, F-14050 Caen, France

来源：

NATURE COMMUNICATIONS | 2023年 / 14卷 / 01期

基金：

中国博士后科学基金; 中国国家自然科学基金; 国家重点研发计划;

关键词：

METAL-SUPPORT INTERACTIONS; ELECTRONIC-STRUCTURE; SINGLE; CATALYST; ATOM; CLUSTERS; TIO2; SIZE; PERFORMANCE; REACTIVITY;

D O I：

10.1038/s41467-023-39226-6

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

The spillover of oxygen species is fundamentally important in redox reactions, but the spillover mechanism has been less understood compared to that of hydrogen spillover. Herein Sn is doped into TiO2 to activate low-temperature (<100 degrees C) reverse oxygen spillover in Pt/TiO2 catalyst, leading to CO oxidation activity much higher than that of most oxide-supported Pt catalysts. A combination of near-ambient-pressure X-ray photoelectron spectroscopy, in situ Raman/Infrared spectroscopies, and ab initiomolecular dynamics simulations reveal that the reverse oxygen spillover is triggered by CO adsorption at Pt2+ sites, followed by bond cleavage of Ti-O-Sn moieties nearby and the appearance of Pt4+ species. The O in the catalytically indispensable Pt-O species is energeticallymore favourable to be originated from Ti-O-Sn. This work clearly depicts the interfacial chemistry of reverse oxygen spillover that is triggered by COadsorption, and the understanding is helpful for the design of platinum/titania catalysts suitable for reactions of various reactants.

引用

页数：12

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