Effect of Reaction Conditions on the Direct Synthesis of Hydrogen Peroxide with a AuPd/TiO2 Catalyst in a Flow Reactor

被引:90
作者
Freakley, Simon J. [1 ]
Piccinini, Marco [1 ]
Edwards, Jennifer K. [1 ]
Ntainjua, Edwin N. [1 ]
Moulijn, Jacob A. [1 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff CF10 3AT, S Glam, Wales
基金
英国工程与自然科学研究理事会;
关键词
hydrogen peroxide; flow reactor; kinetics; gold; palladium catalyst; GOLD-PALLADIUM CATALYSTS; DIRECT OXIDATION; H-2; H2O2; O-2; PD; HALIDE; PERFORMANCES; REDUCTION; KINETICS;
D O I
10.1021/cs400004y
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 direct synthesis of hydrogen peroxide (H2O2) represents a potential alternative to the currently industrially used anthraquinone process, and Au-Pd catalysts have been identified as effective catalysts. To obtain a direct process, a detailed understanding of the reaction conditions in a continuous flow system is needed. In this study, we use a flow reactor to study reaction conditions independently, including total gas flow rate, catalyst mass, reaction pressure, solvent flow rate, and H-2/O-2 molar ratio. The study was carried out without the addition of any halide or acid additives often used to suppress the sequential hydrogenation and decomposition reactions that allowed the kinetics of these reactions to be studied along with the synthesis reaction. A global kinetic model describing the net and gross synthesis rate is proposed, and on the basis of this model, we propose that the decomposition reaction suppresses the production of H2O2 to a greater extent than hydrogenation and that catalyst design studies should aim at blocking or generating catalysts without O-O dissociation sites.
引用
收藏
页码:487 / 501
页数:15
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