In situ FTIR spectroscopic study of the CO2 methanation mechanism on Ni/Ce0.5Zr0.5O2

被引：218

作者：

Pan, Qiushi ^{[1
,2
]}

Peng, Jiaxi ^{[1
]}

Wang, Sheng ^{[1
]}

Wang, Shudong ^{[1
]}

机构：

[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

CATALYSIS SCIENCE & TECHNOLOGY | 2014年 / 4卷 / 02期

基金：

中国国家自然科学基金; 国家高技术研究发展计划(863计划);

关键词：

TRANSFORM INFRARED-SPECTROSCOPY; WATER-GAS SHIFT; CARBON-DIOXIDE; LOW-TEMPERATURE; AMORPHOUS PRECURSORS; FORMIC-ACID; CATALYSTS; SURFACE; HYDROGENATION; ADSORPTION;

D O I：

10.1039/c3cy00868a

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：

CO2 adsorption and methanation on a Ni/Ce0.5Zr0.5O2 catalyst has been investigated using in situ FTIR spectroscopy. CO2 adsorption and methanation experiments were conducted on both components of the support and the catalyst to identify the adsorption species and any intermediate species. It was proposed that CO2 prefers to adsorb on surface oxygen sites adjacent to Ce(III) compared with those adjacent to Ce(IV)/Zr or surface hydroxyl sites. Five adsorption species were revealed for CO2 adsorption on Ni/Ce0.5Zr0.5O2 and monodentate carbonates formed on Ce(III) are easier to be hydrogenated than those on Ce(IV). Formate species were found to be the main intermediate species during the reaction and Ce(III) sites were proposed to be active sites for their hydrogenation. The adsorption and hydrogenation of formic acid were also conducted to confirm the identification of the intermediate species during the reaction. -CH2OH species were detected for the first time and found to be the further intermediates in the reaction.

引用

页码：502 / 509

页数：8

共 39 条

[21] SPECTROSCOPIC IDENTIFICATION OF ADSORBED SPECIES DERIVED FROM ADSORPTION AND DECOMPOSITION OF FORMIC-ACID, METHANOL, AND FORMALDEHYDE ON CERIUM OXIDE [J].