Effect of Zn addition on the direct synthesis of hydrogen peroxide over supported palladium catalysts

被引:71
作者
Wang, Suli [1 ]
Gao, Kaige [1 ]
Li, Wei [1 ]
Zhang, Jinli [1 ,2 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
[2] Shihezi Univ, Sch Chem & Chem Engn, Key Lab Green Proc Chem Engn Xinjiang Bingtuan, Shihezi 832000, Xinjiang, Peoples R China
基金
中国国家自然科学基金;
关键词
PdZn catalysts; Direct synthesis of hydrogen peroxide; Geometric change; Electronic effect; PDZN ALLOY FORMATION; DIRECT OXIDATION; AU CATALYSTS; SELECTIVITY ENHANCERS; BIMETALLIC CATALYSTS; PD/AL2O3; CATALYSTS; AMBIENT CONDITIONS; DIMETHYL ETHER; CO ADSORPTION; ACTIVE-SITES;
D O I
10.1016/j.apcata.2016.10.023
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
Alumina-supported Pd-Zn bimetallic catalysts were prepared and evaluated for direct synthesis of hydrogen peroxide. The effect of Zn on the catalytic performance was studied via characterizations by transmission electron microscopy (TEM), temperature-programmed reduction (TPR), X-ray photoelectron energy spectroscopy (XPS), temperature-programmed desorption of H-2/O-2 (H-2-/O-2-TPD), CO chemisorption and diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption (CO DRIFTS). H2O2 productivity of up to 25431 mol kg(pd)(-1) h(-1) was observed with the optimal bimetallic catalyst 1Pd5Zn, much higher than that over the monometallic catalyst 1Pd (8533 mol kg(Pd)(-1) h(-1)). This increase may be attributed to the geometric change caused by the Zn additive and the electronic interactions between Pd and Zn. The addition of Zn increases the isolated Pd sites (the primary active sites for H2O2 formation), which can promote H2O2 selectivity. PdZn catalysts show a higher Pd dispersion and incremental Pd content than monometallic Pd owing to electronic interactions between Pd and Zn, which result in increased H2O2 productivity. However, a high Pd dispersion and incremental Pd content can increase the H2O2 hydrogenation rate, negatively affecting the H2O2 selectivity. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:89 / 95
页数:7
相关论文
共 65 条
[1]   Effect of Zn addition on the water-gas shift reaction over supported palladium catalysts [J].
Bollmann, Luis ;
Ratts, Joshua L. ;
Joshi, Ajay M. ;
Williams, W. Damion ;
Pazmino, Jorge ;
Joshi, Yogesh V. ;
Miller, Jeffrey T. ;
Kropf, A. Jeremy ;
Delgass, W. Nicholas ;
Ribeiro, Fabio H. .
JOURNAL OF CATALYSIS, 2008, 257 (01) :43-54
[2]   Hydrogen peroxide synthesis: An outlook beyond the anthraquinone process [J].
Campos-Martin, Jose M. ;
Blanco-Brieva, Gema ;
Fierro, Jose L. G. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (42) :6962-6984
[3]   Modifying structure-sensitive reactions by addition of Zn to Pd [J].
Childers, David J. ;
Schweitzer, Neil M. ;
Shahari, Seyed Mehdi Kamali ;
Rioux, Robert M. ;
Miller, Jeffrey T. ;
Meyer, Randall J. .
JOURNAL OF CATALYSIS, 2014, 318 :75-84
[4]   A mechanistic study of H2O2 and H2O formation from H2 and O2 catalyzed by palladium in an aqueous medium [J].
Chinta, S ;
Lunsford, JH .
JOURNAL OF CATALYSIS, 2004, 225 (01) :249-255
[5]   Direct oxidation of H2 to H2O2 over Pd-based catalysts:: Influence of oxidation state, support and metal additives [J].
Choudhary, V. R. ;
Samanta, C. ;
Choudhary, T. V. .
APPLIED CATALYSIS A-GENERAL, 2006, 308 :128-133
[6]   Stability of bimetallic Pd-Zn catalysts for the steam reforming of methanol [J].
Conant, Travis ;
Karim, Ayman M. ;
Lebarbier, Vanessa ;
Wang, Yong ;
Girgsdies, Frank ;
Schloegl, Robert ;
Datye, Abhaya .
JOURNAL OF CATALYSIS, 2008, 257 (01) :64-70
[7]   Catalysts for direct H2O2 synthesis taking advantage of the high H2 activating ability of Pt: kinetic characteristics of Pt catalysts and new additives for improving H2O2 selectivity [J].
Deguchi, T. ;
Yamano, H. ;
Takenouchi, S. ;
Iwamoto, M. .
CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (12) :4232-4242
[8]   Direct synthesis of hydrogen peroxide from H2 and O2 using supported Au-Pd catalysts [J].
Edwards, Jennifer K. ;
Carley, Albert F. ;
Herzing, Andrew A. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
FARADAY DISCUSSIONS, 2008, 138 :225-239
[9]   Advances in the direct synthesis of hydrogen peroxide from hydrogen and oxygen [J].
Edwards, Jennifer K. ;
Freakley, Simon J. ;
Lewis, Richard J. ;
Pritchard, James C. ;
Hutchings, Graham J. .
CATALYSIS TODAY, 2015, 248 :3-9
[10]   Strategies for Designing Supported Gold-Palladium Bimetallic Catalysts for the Direct Synthesis of Hydrogen Peroxide [J].
Edwards, Jennifer K. ;
Freakley, Simon J. ;
Carley, Albert F. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
ACCOUNTS OF CHEMICAL RESEARCH, 2014, 47 (03) :845-854