Insight into active sites of Pd-Au/TiO2 catalysts in hydrogen peroxide synthesis directly from H2 and O2

被引:124
作者
Ouyang, Like [1 ]
Da, Guo-jin [1 ]
Tian, Peng-fei [1 ]
Chen, Tian-yuan [1 ]
Liang, Guo-da [1 ]
Xu, Jing [1 ]
Han, Yi-Fan [1 ]
机构
[1] E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
基金
美国国家科学基金会;
关键词
Pd-Au nanoalloy; H2O2; synthesis; hydrogenation; Active sites; Interface; Characterization; MOLECULARLY CHEMISORBED OXYGEN; NEAR-ATMOSPHERIC PRESSURES; SUPPORTED PD CATALYSTS; CO OXIDATION; SUBSURFACE OXYGEN; ULTRAHIGH-VACUUM; GOLD; H2O2; AU; SURFACE;
D O I
10.1016/j.jcat.2013.11.008
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
H2O2 synthesis directly from H-2 and O-2 and side reactions in this system over a variety of Pd-Au/TiO2 catalysts have been studied systemically. The effects of Pd/Au ratio on H2O2 synthesis and subsequent H2O2 hydrogenation were investigated. The catalysts were characterized using multiple techniques including transmission electron microscopy (TEM), in situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption (CO-DRIFTS), X-rays photoelectron spectroscopy (XPS), and temperature-programmed desorption of H-2/O-2 (H-2-/O-2-TPD). By detailed analysis of these spectroscopies and the kinetics of this reaction, new insights into various active sites of Pd upon alloying with Au were elaborated. Pd monomer surrounded by Au atoms could be the primary active site for H2O2 formation. In addition, Pd ensembles were assumed to be more active for H2O2 hydrogenation than monomeric Pd sites; the over-oxidation of H-2 to H2O likely occurred at the interface between Au and TiO2. (C) 2013 Elsevier Inc. All rights reserved.
引用
收藏
页码:129 / 136
页数:8
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