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

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 nar...

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Main Authors: Yasemen Kuddusi, Laura Piveteau, Mounir Mensi, Daniel C. Cano-Blanco, Andreas Züttel
Format: Article
Language:English
Published: Elsevier 2025-01-01
Series:Journal of CO2 Utilization
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Online Access:http://www.sciencedirect.com/science/article/pii/S2212982024003366
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author Yasemen Kuddusi
Laura Piveteau
Mounir Mensi
Daniel C. Cano-Blanco
Andreas Züttel
author_facet Yasemen Kuddusi
Laura Piveteau
Mounir Mensi
Daniel C. Cano-Blanco
Andreas Züttel
author_sort Yasemen Kuddusi
collection DOAJ
description 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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spelling doaj-art-d192acd2d174437fb6ea4716765f7b8f2025-01-13T04:18:50ZengElsevierJournal of CO2 Utilization2212-98392025-01-0191103001Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalystsYasemen Kuddusi0Laura Piveteau1Mounir Mensi2Daniel C. Cano-Blanco3Andreas Züttel4Laboratory of Materials for Renewable Energy (LMER), Institute of Chemical Sciences and Engineering (ISIC), Basic Science Faculty (SB), École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis, Rue de l’Industrie 17, 1951 Sion, Switzerland; Empa Materials Science & Technology, 8600 Dübendorf, Switzerland; Corresponding author at: Laboratory of Materials for Renewable Energy (LMER), Institute of Chemical Sciences and Engineering (ISIC), Basic Science Faculty (SB), École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis, Rue de l’Industrie 17, 1951 Sion, Switzerland.NMR Platform, Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), Rte Cantonale, 1015 Lausanne, SwitzerlandX-Ray Diffraction and Surface Analytics Platform (XRDSAP), Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis, Rue de l’Industrie 17, 1951 Sion, SwitzerlandPaul Scherrer Institute, PSI Center for Energy and Environmental Sciences, 5232 Villigen PSI, Switzerland; Institute for Chemical and Chemical Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, SwitzerlandLaboratory of Materials for Renewable Energy (LMER), Institute of Chemical Sciences and Engineering (ISIC), Basic Science Faculty (SB), École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis, Rue de l’Industrie 17, 1951 Sion, Switzerland; Empa Materials Science & Technology, 8600 Dübendorf, SwitzerlandDirect 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.http://www.sciencedirect.com/science/article/pii/S2212982024003366CO2 hydrogenationEthyleneLight olefinsGalliumIndiumBifunctional catalyst
spellingShingle Yasemen Kuddusi
Laura Piveteau
Mounir Mensi
Daniel C. Cano-Blanco
Andreas Züttel
Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
Journal of CO2 Utilization
CO2 hydrogenation
Ethylene
Light olefins
Gallium
Indium
Bifunctional catalyst
title Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
title_full Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
title_fullStr Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
title_full_unstemmed Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
title_short Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts
title_sort selective light olefin synthesis with high ethylene abundance via co2 hydrogenation over ga in 2o3 ssz 13 catalysts
topic CO2 hydrogenation
Ethylene
Light olefins
Gallium
Indium
Bifunctional catalyst
url http://www.sciencedirect.com/science/article/pii/S2212982024003366
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AT laurapiveteau selectivelightolefinsynthesiswithhighethyleneabundanceviaco2hydrogenationovergain2o3ssz13catalysts
AT mounirmensi selectivelightolefinsynthesiswithhighethyleneabundanceviaco2hydrogenationovergain2o3ssz13catalysts
AT danielccanoblanco selectivelightolefinsynthesiswithhighethyleneabundanceviaco2hydrogenationovergain2o3ssz13catalysts
AT andreaszuttel selectivelightolefinsynthesiswithhighethyleneabundanceviaco2hydrogenationovergain2o3ssz13catalysts