Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis

Adrian Galilea; Xuan Gong; Mustafa Caglayan; Stefan-Adrian F. Nastase; Edy Abou-Hamad; Lieven Gevers; Luigi Cavallo; Abhishek Dutta Chowdhury; Jorge Gascon

doi:10.1038/s41467-021-26090-5

Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis

Adrian Galilea, Xuan Gong, Mustafa Caglayan, Stefan-Adrian F. Nastase, Edy Abou-Hamad, Lieven Gevers, Luigi Cavallo, Abhishek Dutta Chowdhury, Jorge Gascon

Research output: Contribution to journal › Article › peer-review

61 Scopus citations

Abstract

AbstractCascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for the one-step valorization of C1-feedstocks. The combination of metal-based catalysts and zeolites in the gas phase hydrogenation of CO2 leads to a large degree of product selectivity control, defined mainly by zeolites. However, a great deal of mechanistic understanding remains unclear: metal-based catalysts usually lead to complex product compositions that may result in unexpected zeolite reactivity. Here we present an in-depth multivariate analysis of the chemistry involved in eight different zeolite topologies when combined with a highly active Fe-based catalyst in the hydrogenation of CO2 to olefins, aromatics, and paraffins. Solid-state NMR spectroscopy and computational analysis demonstrate that the hybrid nature of the active zeolite catalyst and its preferred CO2-derived reaction intermediates (CO/ester/ketone/hydrocarbons, i.e., inorganic-organic supramolecular reactive centers), along with 10 MR-zeolite topology, act as descriptors governing the ultimate product selectivity.

Original language	English (US)
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-26090-5
State	Published - Oct 8 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-10-12
Acknowledgements: This project has received financial supports from the King Abdullah University of Science and Technology (Saudi Arabia), the start-up research grant from the Institute for Advanced Studies (IAS), Wuhan University (China), and the National Natural Science Foundation of China (NSFC) (Grant No. 22050410276 to A.D.C.). The authors also acknowledge Mr. Ye Yiru (IAS, Wuhan, China) and Dr. Serhii Vasylevskyi (KAUST, Saudi Arabia) for their support during figures’ preparation and Raman measurements, respectively. A.D.C. also conveys sincere thanks to Dr. Alessandra Lucini Paioni for her advice in this work.

ASJC Scopus subject areas

General Biochemistry, Genetics and Molecular Biology
General Chemistry
General Physics and Astronomy

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10.1038/s41467-021-26090-5

https://repository.kaust.edu.sa/bitstream/10754/672537/1/s41467-021-26090-5.pdf

Cite this

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title = "Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis",

abstract = "AbstractCascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for the one-step valorization of C1-feedstocks. The combination of metal-based catalysts and zeolites in the gas phase hydrogenation of CO2 leads to a large degree of product selectivity control, defined mainly by zeolites. However, a great deal of mechanistic understanding remains unclear: metal-based catalysts usually lead to complex product compositions that may result in unexpected zeolite reactivity. Here we present an in-depth multivariate analysis of the chemistry involved in eight different zeolite topologies when combined with a highly active Fe-based catalyst in the hydrogenation of CO2 to olefins, aromatics, and paraffins. Solid-state NMR spectroscopy and computational analysis demonstrate that the hybrid nature of the active zeolite catalyst and its preferred CO2-derived reaction intermediates (CO/ester/ketone/hydrocarbons, i.e., inorganic-organic supramolecular reactive centers), along with 10 MR-zeolite topology, act as descriptors governing the ultimate product selectivity.",

author = "Adrian Galilea and Xuan Gong and Mustafa Caglayan and Nastase, {Stefan-Adrian F.} and Edy Abou-Hamad and Lieven Gevers and Luigi Cavallo and Chowdhury, {Abhishek Dutta} and Jorge Gascon",

note = "KAUST Repository Item: Exported on 2021-10-12 Acknowledgements: This project has received financial supports from the King Abdullah University of Science and Technology (Saudi Arabia), the start-up research grant from the Institute for Advanced Studies (IAS), Wuhan University (China), and the National Natural Science Foundation of China (NSFC) (Grant No. 22050410276 to A.D.C.). The authors also acknowledge Mr. Ye Yiru (IAS, Wuhan, China) and Dr. Serhii Vasylevskyi (KAUST, Saudi Arabia) for their support during figures{\textquoteright} preparation and Raman measurements, respectively. A.D.C. also conveys sincere thanks to Dr. Alessandra Lucini Paioni for her advice in this work.",

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AU - Galilea, Adrian

AU - Gong, Xuan

AU - Caglayan, Mustafa

AU - Nastase, Stefan-Adrian F.

AU - Abou-Hamad, Edy

AU - Gevers, Lieven

AU - Cavallo, Luigi

AU - Chowdhury, Abhishek Dutta

AU - Gascon, Jorge

N1 - KAUST Repository Item: Exported on 2021-10-12 Acknowledgements: This project has received financial supports from the King Abdullah University of Science and Technology (Saudi Arabia), the start-up research grant from the Institute for Advanced Studies (IAS), Wuhan University (China), and the National Natural Science Foundation of China (NSFC) (Grant No. 22050410276 to A.D.C.). The authors also acknowledge Mr. Ye Yiru (IAS, Wuhan, China) and Dr. Serhii Vasylevskyi (KAUST, Saudi Arabia) for their support during figures’ preparation and Raman measurements, respectively. A.D.C. also conveys sincere thanks to Dr. Alessandra Lucini Paioni for her advice in this work.

PY - 2021/10/8

Y1 - 2021/10/8

N2 - AbstractCascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for the one-step valorization of C1-feedstocks. The combination of metal-based catalysts and zeolites in the gas phase hydrogenation of CO2 leads to a large degree of product selectivity control, defined mainly by zeolites. However, a great deal of mechanistic understanding remains unclear: metal-based catalysts usually lead to complex product compositions that may result in unexpected zeolite reactivity. Here we present an in-depth multivariate analysis of the chemistry involved in eight different zeolite topologies when combined with a highly active Fe-based catalyst in the hydrogenation of CO2 to olefins, aromatics, and paraffins. Solid-state NMR spectroscopy and computational analysis demonstrate that the hybrid nature of the active zeolite catalyst and its preferred CO2-derived reaction intermediates (CO/ester/ketone/hydrocarbons, i.e., inorganic-organic supramolecular reactive centers), along with 10 MR-zeolite topology, act as descriptors governing the ultimate product selectivity.

AB - AbstractCascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for the one-step valorization of C1-feedstocks. The combination of metal-based catalysts and zeolites in the gas phase hydrogenation of CO2 leads to a large degree of product selectivity control, defined mainly by zeolites. However, a great deal of mechanistic understanding remains unclear: metal-based catalysts usually lead to complex product compositions that may result in unexpected zeolite reactivity. Here we present an in-depth multivariate analysis of the chemistry involved in eight different zeolite topologies when combined with a highly active Fe-based catalyst in the hydrogenation of CO2 to olefins, aromatics, and paraffins. Solid-state NMR spectroscopy and computational analysis demonstrate that the hybrid nature of the active zeolite catalyst and its preferred CO2-derived reaction intermediates (CO/ester/ketone/hydrocarbons, i.e., inorganic-organic supramolecular reactive centers), along with 10 MR-zeolite topology, act as descriptors governing the ultimate product selectivity.

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SN - 2041-1723

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JO - Nature Communications

JF - Nature Communications

IS - 1

ER -

Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis

Abstract

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