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.
机构:
East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Tian, Pengfei
Ding, Doudou
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East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Ding, Doudou
Sun, Yang
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机构:
East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Sun, Yang
Xuan, Fuzhen
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机构:
East China Univ Sci & Technol, Key Lab Pressure Syst & Safety, Minist Educ, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Xuan, Fuzhen
Xu, Xingyan
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East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Xu, Xingyan
Xu, Jing
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机构:
East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Xu, Jing
Han, Yi-Fan
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机构:
East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Henan, Peoples R ChinaEast China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China