Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts

被引:1
|
作者
Kuddusi, Yasemen [1 ,2 ]
Piveteau, Laura [3 ]
Mensi, Mounir [4 ]
Cano-Blanco, Daniel C. [5 ,6 ]
Zuttel, Andreas [1 ,2 ]
机构
[1] Ecole Polytech Fed Lausanne EPFL Valais Wallis, Inst Chem Sci & Engn ISIC, Basic Sci Fac SB, Lab Mat Renewable Energy LMER, Rue Ind 17, CH-1951 Sion, Switzerland
[2] Empa Mat Sci & Technol, CH-8600 Dubendorf, Switzerland
[3] Ecole Polytech Fed Lausanne EPFL, Inst Chem Sci & Engn ISIC, NMR Platform, CH-1015 Lausanne, Switzerland
[4] Ecole Polytech Fed Lausanne EPFL Valais Wallis, Inst Chem Sci & Engn ISIC, X Ray Diffract & Surface Analyt Platform XRDSAP, Energypolis, Rue Ind 17, CH-1951 Sion, Switzerland
[5] Paul Scherrer Inst, PSI Ctr Energy & Environm Sci, CH-5232 Villigen, Switzerland
[6] Ecole Polytech Fed Lausanne EPFL, Inst Chem & Chem Engn, CH-1015 Lausanne, Switzerland
关键词
CO; 2; hydrogenation; Ethylene; Light olefins; Gallium; Indium; Bifunctional catalyst; CARBON-DIOXIDE; PROPANE DEHYDROGENATION; METHANOL SYNTHESIS; OXIDE; CONVERSION; HYDROCARBONS; ACTIVATION; REDUCTION; PROPENE; TRENDS;
D O I
10.1016/j.jcou.2024.103001
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct light olefin synthesis from CO2 hydrogenation is a new pathway to decarbonize the chemical industry. Inspired by the promising catalytic activity of Ga2O3-based catalysts in alkane dehydrogenation, this study reveals that optimizing Ga content in the GaxIn2-xO3/SSZ-13 catalytic system can narrow the product distribution toward light olefins. The optimized catalyst exhibits light olefin and C2H4 selectivity up to 84 % and 45.9 %, respectively, amongst C2+ hydrocarbons with a maximum olefin/paraffin ratio of 6.4 and a CO2 conversion of 14.8 % at 20 bar and 653 K. In particular, a sevenfold increase in C2H4 space-time yield compared to pure metal oxides on SSZ-13 was observed, along with the gradual suppression of C3H8 formation. Herein, we established a catalyst structure-performance relationship as a function of chemical composition. As such, CO and paraffin formation rates can be suppressed, and light olefin formation rates can be enhanced. Therefore, the change in light olefin STY upon gallium incorporation could be ascribed to modulations in the structural and electronic properties, as well as alterations in the surface adsorption and acidic strengths. The findings presented here provide a strategy to tune CO2 hydrogenation product distributions toward specific target products.
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页数:11
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