Active Phase of FeOx/Pt Catalysts in Low-Temperature CO Oxidation and Preferential Oxidation of CO Reaction

被引:42
|
作者
Chen, Hao [1 ,2 ]
Liu, Yun [1 ,2 ]
Yang, Fan [1 ]
Wei, Mingming [1 ,2 ]
Zhao, Xinfie [1 ,2 ]
Ning, Yanxiao [1 ]
Liu, Qingfei [1 ,2 ]
Zhang, Yi [1 ,2 ]
Fu, Qiang [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Catalysis,CAS Ctr Excellence Nanosc, Zhongshan Rd 457, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2017年 / 121卷 / 19期
基金
中国国家自然科学基金;
关键词
SCANNING-TUNNELING-MICROSCOPY; FERROUS CENTERS; PT(111) SURFACE; OXIDE-FILMS; OXYGEN; INTERFACE; COVERAGE; NANOSTRUCTURES; VACUUM; SITES;
D O I
10.1021/acs.jpcc.7b01392
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 interface between metal and reducible oxide has attracted increasing interest in catalysis. The FeOx Pt interface has been a typical example, which showed remarkable activity for the preferential oxidation of CO (PROX) at low temperatures. However, model catalytic studies under vacuum conditions or in high-pressure O-rich environment at 450 K have reported two different active phases with iron in two different valence states, invoking a possible pressure gap. To identify the active phase for low-temperature CO oxidation and PROX, it is necessary to investigate the stability and activity of FeO/Pt(111) under the realistic reaction conditions. We thus conducted an in situ study on FeO/Pt(111) from ultrahigh vacuum to the atmospheric pressure of reactant gases. Our study shows FeO islands were easily, oxidized in 1 Torr O-2 to form the trilayer FeO2 islands. However, the presence of 2 Torr CO could prevent the oxidation of FeO islands and lead to CO oxidation at the FeO/Pt(111) interface. The FeO/Pt(111) surface exhibits an excellent activity for CO, production with an initial reaction rate measured to be similar to X 10(14) molecules-cm(-2)-s(-1) at 300 K. FeO islands supported on Pt(111) were further investigated in the PROX gas, i.e., the mixture of 98.5% H-2, 1% CO, and 0.5% O-2 at elevated pressures up to 1 bar. Our results thus bridged the pressure gap and identified the bilayer FeO islands on Pt(111) as the active phase for PROX under the realistic reaction conditions.
引用
收藏
页码:10398 / 10405
页数:8
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