Reversible deactivation of a Au/Ce0.62Zr0.38O2 catalyst in CO oxidation: A systematic study of CO2-triggered carbonate inhibition

被引：42

作者：

del Rio, Eloy ^{[1
]}

Collins, Sebastian E. ^{[2
]}

Aguirre, Alejo ^{[2
]}

Chen, Xiaowei ^{[1
]}

Jose Delgado, Juan ^{[1
]}

Juan Calvino, Jose ^{[1
]}

Bernal, Serafin ^{[1
]}

机构：

[1] Univ Cadiz, Fac Ciencias, Dept Ciencia Mat Ingn Met & Quim Inorgan, E-11510 Puerto Real, Cadiz, Spain

[2] UNL, CONICET, Inst Desarrollo Tecnol Ind Quim, RA-3450 Guemes, Argentina

来源：

JOURNAL OF CATALYSIS | 2014年 / 316卷

关键词：

Gold catalyst; CO oxidation; Deactivation; Carbonate species; CO2; poisoning; Mass spectrometry isotopic analysis; Time-resolved infrared spectroscopy; DRIFT; Modulation excitation spectroscopy (MES); Reaction mechanism; CATALYTICALLY ACTIVE GOLD; GAS SHIFT REACTION; VIBRATIONAL SPECTROSCOPY; AU/FE2O3; CATALYSTS; ZIRCONIA CATALYSTS; AU/TIO2; CATALYST; TEMPERATURE; FTIR; ADSORPTION; NANOPARTICLES;

D O I：

10.1016/j.jcat.2014.05.016

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：

Highly active supported gold catalysts frequently undergo substantial decrease in activity due to deactivation. The aim of this paper is to investigate a reversible inhibition phenomenon of the CO oxidation in an Au/Ce0.62Zr0.38O2 (Au/CZ) catalyst. The results of a systematic study of CO oxidation conditions (CO, O-2, and CO2) are discussed. By identifying CO2 as an Au/CZ poison using isotopic transient analysis ((CO)-C-13/(CO2)-C-12), we also investigate the origin of inhibition activity by transient and modulated infrared spectroscopy in DRIFT mode. Results demonstrate that carbonate species are formed by reaction of CO2 with reactive lattice oxygen at the metal-support interphase, which in turn inhibits the replenishment of the vacancies by molecular oxygen. A microkinetic model that accounts for the reaction mechanism and inhibition by CO2 is proposed. (C) 2014 Elsevier Inc. All rights reserved.

引用

页码：210 / 218

页数：9

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