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

Cascade 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 CO 2 leads...

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Published inNature communications Vol. 12; no. 1; pp. 5914 - 13
Main Authors Ramirez, Adrian, Gong, Xuan, Caglayan, Mustafa, Nastase, Stefan-Adrian F., Abou-Hamad, Edy, Gevers, Lieven, Cavallo, Luigi, Dutta Chowdhury, Abhishek, Gascon, Jorge
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 08.10.2021
Nature Publishing Group
Nature Portfolio
Subjects
140/131
140/133
639/638/298
639/638/77/887
Alkenes
Aromatic compounds
Carbon dioxide
Catalysis
Catalysts
Computer applications
Humanities and Social Sciences
Hydrocarbons
Hydrogenation
Intermediates
Magnetic resonance spectroscopy
multidisciplinary
Multivariate analysis
NMR
NMR spectroscopy
Nuclear magnetic resonance
Paraffins
Reaction mechanisms
Science
Science (multidisciplinary)
Selectivity
Topology
Vapor phases
Zeolites
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Abstract Cascade 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 CO 2 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 CO 2 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 CO 2 -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. The reaction mechanism of carbon dioxide to high-value hydrocarbons over metal-zeolite bifunctional catalysts remains ambiguous. Here, the authors demonstrate that active zeolite catalysts’ topology and hybrid nature are descriptors; regulating the reaction mechanism and ultimate product selectivity.
AbstractList The reaction mechanism of carbon dioxide to high-value hydrocarbons over metal-zeolite bifunctional catalysts remains ambiguous. Here, the authors demonstrate that active zeolite catalysts’ topology and hybrid nature are descriptors; regulating the reaction mechanism and ultimate product selectivity.
Cascade 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.Cascade 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.
Cascade 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.The reaction mechanism of carbon dioxide to high-value hydrocarbons over metal-zeolite bifunctional catalysts remains ambiguous. Here, the authors demonstrate that active zeolite catalysts’ topology and hybrid nature are descriptors; regulating the reaction mechanism and ultimate product selectivity.
Cascade 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 CO 2 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 CO 2 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 CO 2 -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.
Cascade 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 CO 2 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 CO 2 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 CO 2 -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. The reaction mechanism of carbon dioxide to high-value hydrocarbons over metal-zeolite bifunctional catalysts remains ambiguous. Here, the authors demonstrate that active zeolite catalysts’ topology and hybrid nature are descriptors; regulating the reaction mechanism and ultimate product selectivity.
ArticleNumber 5914
Author Gong, Xuan
Cavallo, Luigi
Ramirez, Adrian
Gascon, Jorge
Abou-Hamad, Edy
Caglayan, Mustafa
Dutta Chowdhury, Abhishek
Nastase, Stefan-Adrian F.
Gevers, Lieven
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Snippet Cascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for...
The reaction mechanism of carbon dioxide to high-value hydrocarbons over metal-zeolite bifunctional catalysts remains ambiguous. Here, the authors demonstrate...
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StartPage 5914
SubjectTerms 140/131
140/133
639/638/298
639/638/77/887
Alkenes
Aromatic compounds
Carbon dioxide
Catalysis
Catalysts
Computer applications
Humanities and Social Sciences
Hydrocarbons
Hydrogenation
Intermediates
Magnetic resonance spectroscopy
multidisciplinary
Multivariate analysis
NMR
NMR spectroscopy
Nuclear magnetic resonance
Paraffins
Reaction mechanisms
Science
Science (multidisciplinary)
Selectivity
Topology
Vapor phases
Zeolites
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Title Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis
URI https://link.springer.com/article/10.1038/s41467-021-26090-5
https://www.proquest.com/docview/2580181962
https://www.proquest.com/docview/2580700119
https://pubmed.ncbi.nlm.nih.gov/PMC8501036
https://doaj.org/article/3d5c0f86e073499f885508bf2d550f02
Volume 12
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