Indium Oxide as a Superior Catalyst for Methanol Synthesis by CO2 Hydrogenation

被引:940
|
作者
Martin, Oliver [1 ]
Martin, Antonio J. [1 ]
Mondelli, Cecilia [1 ]
Mitchell, Sharon [1 ]
Segawa, Takuya F. [2 ]
Hauert, Roland [3 ]
Drouilly, Charlotte [4 ]
Curulla-Ferre, Daniel [4 ]
Perez-Ramirez, Javier [1 ]
机构
[1] ETH, Dept Chem & Appl Biosci, Inst Chem & Bioengn, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
[2] ETH, Dept Chem & Appl Biosci, Phys Chem Lab, Vladimir Prelog Weg 2, CH-8093 Zurich, Switzerland
[3] Swiss Fed Labs Mat Sci & Technol, Empa, Uberlandstr 129, CH-8600 Dubendorf, Switzerland
[4] Total Res & Technol Feluy, Zone Ind Feluy C, B-7181 Seneffe, Belgium
关键词
CO2; hydrogenation; indium oxide; methanol synthesis; oxygen vacancies; zirconium oxide; WATER-GAS SHIFT; REFORMING ACTIVITY; IN2O3; ADSORPTION; RESONANCE; KINETICS; SITE; DFT; ZNO;
D O I
10.1002/anie.201600943
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Methanol synthesis by CO2 hydrogenation is attractive in view of avoiding the environmental implications associated with the production of the traditional syngas feedstock and mitigating global warming. However, there still is a lack of efficient catalysts for such alternative processes. Herein, we unveil the high activity, 100% selectivity, and remarkable stability for 1000 h on stream of In2O3 supported on ZrO2 under industrially relevant conditions. This strongly contrasts to the benchmark Cu-ZnO-Al2O3 catalyst, which is unselective and experiences rapid deactivation. In-depth characterization of the In2O3-based materials points towards a mechanism rooted in the creation and annihilation of oxygen vacancies as active sites, whose amount can be modulated in situ by co-feeding CO and boosted through electronic interactions with the zirconia carrier. These results constitute a promising basis for the design of a prospective technology for sustainable methanol production.
引用
收藏
页码:6261 / 6265
页数:5
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