Mechanistic study of water-gas shift reaction over copper/zinc-oxide/alumina catalyst in a reformed gas atmosphere: Influence of hydrogen on reaction rate

被引：14

作者：

Taniya, Keita ^{[1
,2
,3
]}

Horie, Yasuhiro ^{[1
]}

Fujita, Ryo ^{[1
]}

Ichihashi, Yuichi ^{[1
,2
,3
]}

Nishiyama, Satoru ^{[1
,2
]}

机构：

[1] Kobe Univ, Grad Sch Engn, Dept Chem Sci & Engn, Nada, Kobe 6578501, Japan

[2] Kobe Univ, Grad Sch Engn, Social Implementat Renewable Energy Res Ctr, Nada, Kobe 6578501, Japan

[3] Kobe Univ, Res Ctr Membrane & Film Technol, Nada, Kobe 6578501, Japan

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 330卷

关键词：

Water -gas shift reaction; Low-temperature shift; Competitive redox mechanism; Active site estimation; METHANOL SYNTHESIS; STRUCTURE-SENSITIVITY; CARBON-MONOXIDE; ADSORBED OXYGEN; CU(110) SURFACE; CU-ZNO; REDUCTION; KINETICS; CO;

D O I：

10.1016/j.apcatb.2023.122568

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：

Kinetic and pulse experiments were performed to elucidate the mechanism of the water-gas shift reaction (WGSR) under practical conditions. CO conversion was found to be significantly influenced by H2. The reaction was strongly suppressed at high H2 concentrations. A simple rate equation based on a competitive redox mechanism was derived. The H2O-induced oxidation of Cu0 to Cu+ was assumed to be the rate-determining step. H2 affected the CO conversion rate because it competitively reduced Cu+ to Cu0. In the proposed rate equation, the rate constant kf determines the rate of the catalytic cycle and the selectivity factor & kappa; may control the selectivity to CO conversion. CO-pulse experiments independently yielded the selectivity factor & kappa; (1.38), which was almost identical to that obtained from the kinetic analysis (1.39). The coincidence of these values strongly corroborates the proposed competitive redox mechanism.

引用

页数：11

共 30 条

[11] Kinetic and mechanistic studies of the water-gas shift reaction on Pt/TiO2 catalyst [J].