Uncovering the reaction mechanism behind CoO as active phase for CO2 hydrogenation

被引:146
作者
ten Have, Iris C. [1 ]
Kromwijk, Josepha J. G. [1 ]
Monai, Matteo [1 ]
Ferri, Davide [2 ]
Sterk, Ellen B. [1 ]
Meirer, Florian [1 ]
Weckhuysen, Bert M. [1 ]
机构
[1] Univ Utrecht, Inorgan Chem & Catalysis Grp, Debye Inst Nanomat Sci, Univ Weg 99, NL-3584 CG Utrecht, Netherlands
[2] Paul Scherrer Inst, Forschungsstr 111, CH-5232 Villigen, Switzerland
关键词
FISCHER-TROPSCH SYNTHESIS; MODULATION EXCITATION SPECTROSCOPY; X-RAY-ABSORPTION; INFRARED-SPECTROSCOPY; CATALYSTS; CONVERSION; SUPPORT; HYDROCARBONS; METHANATION; ELECTROREDUCTION;
D O I
10.1038/s41467-022-27981-x
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C2+ hydrocarbons. The C2+ selectivity increases to 39% (yielding 104 mmol h(-1) g(cat)(-1) C2+ hydrocarbons) upon co-feeding CO and CO2 at a ratio of 1:2 at 250 degrees C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts. Catalytic conversion of CO2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a titania carrier produce more C2+ hydrocarbons than their metallic cobalt counterpart by following a different reaction mechanism.
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页数:11
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