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Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces
The conversion of CO(2) into fuels and chemicals is an attractive option for mitigating CO(2) emissions. Controlling the selectivity of this process is beneficial to produce desirable liquid fuels, but C–C coupling is a limiting step in the reaction that requires high pressures. Here, we propose a s...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8851537/ https://www.ncbi.nlm.nih.gov/pubmed/35135880 http://dx.doi.org/10.1073/pnas.2114768119 |
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author | Zhou, Chengshuang Asundi, Arun S. Goodman, Emmett D. Hong, Jiyun Werghi, Baraa Hoffman, Adam S. Nathan, Sindhu S. Bent, Stacey F. Bare, Simon R. Cargnello, Matteo |
author_facet | Zhou, Chengshuang Asundi, Arun S. Goodman, Emmett D. Hong, Jiyun Werghi, Baraa Hoffman, Adam S. Nathan, Sindhu S. Bent, Stacey F. Bare, Simon R. Cargnello, Matteo |
author_sort | Zhou, Chengshuang |
collection | PubMed |
description | The conversion of CO(2) into fuels and chemicals is an attractive option for mitigating CO(2) emissions. Controlling the selectivity of this process is beneficial to produce desirable liquid fuels, but C–C coupling is a limiting step in the reaction that requires high pressures. Here, we propose a strategy to favor C–C coupling on a supported Ru/TiO(2) catalyst by encapsulating it within the polymer layers of an imine-based porous organic polymer that controls its selectivity. Such polymer confinement modifies the CO(2) hydrogenation behavior of the Ru surface, significantly enhancing the C(2+) production turnover frequency by 10-fold. We demonstrate that the polymer layers affect the adsorption of reactants and intermediates while being stable under the demanding reaction conditions. Our findings highlight the promising opportunity of using polymer/metal interfaces for the rational engineering of active sites and as a general tool for controlling selective transformations in supported catalyst systems. |
format | Online Article Text |
id | pubmed-8851537 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-88515372022-08-08 Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces Zhou, Chengshuang Asundi, Arun S. Goodman, Emmett D. Hong, Jiyun Werghi, Baraa Hoffman, Adam S. Nathan, Sindhu S. Bent, Stacey F. Bare, Simon R. Cargnello, Matteo Proc Natl Acad Sci U S A Physical Sciences The conversion of CO(2) into fuels and chemicals is an attractive option for mitigating CO(2) emissions. Controlling the selectivity of this process is beneficial to produce desirable liquid fuels, but C–C coupling is a limiting step in the reaction that requires high pressures. Here, we propose a strategy to favor C–C coupling on a supported Ru/TiO(2) catalyst by encapsulating it within the polymer layers of an imine-based porous organic polymer that controls its selectivity. Such polymer confinement modifies the CO(2) hydrogenation behavior of the Ru surface, significantly enhancing the C(2+) production turnover frequency by 10-fold. We demonstrate that the polymer layers affect the adsorption of reactants and intermediates while being stable under the demanding reaction conditions. Our findings highlight the promising opportunity of using polymer/metal interfaces for the rational engineering of active sites and as a general tool for controlling selective transformations in supported catalyst systems. National Academy of Sciences 2022-02-08 2022-02-15 /pmc/articles/PMC8851537/ /pubmed/35135880 http://dx.doi.org/10.1073/pnas.2114768119 Text en Copyright © 2022 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) . |
spellingShingle | Physical Sciences Zhou, Chengshuang Asundi, Arun S. Goodman, Emmett D. Hong, Jiyun Werghi, Baraa Hoffman, Adam S. Nathan, Sindhu S. Bent, Stacey F. Bare, Simon R. Cargnello, Matteo Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title | Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title_full | Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title_fullStr | Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title_full_unstemmed | Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title_short | Steering CO(2) hydrogenation toward C–C coupling to hydrocarbons using porous organic polymer/metal interfaces |
title_sort | steering co(2) hydrogenation toward c–c coupling to hydrocarbons using porous organic polymer/metal interfaces |
topic | Physical Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8851537/ https://www.ncbi.nlm.nih.gov/pubmed/35135880 http://dx.doi.org/10.1073/pnas.2114768119 |
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