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Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst
Direct conversion of CO(2) to a single specific hydrocarbon with high selectivity is extremely attractive but very challenging. Herein, by employing an InZrO(x)-Beta composite catalyst in the CO(2) hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10164185/ https://www.ncbi.nlm.nih.gov/pubmed/37149644 http://dx.doi.org/10.1038/s41467-023-38336-5 |
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author | Wang, Han Fan, Sheng Guo, Shujia Wang, Sen Qin, Zhangfeng Dong, Mei Zhu, Huaqing Fan, Weibin Wang, Jianguo |
author_facet | Wang, Han Fan, Sheng Guo, Shujia Wang, Sen Qin, Zhangfeng Dong, Mei Zhu, Huaqing Fan, Weibin Wang, Jianguo |
author_sort | Wang, Han |
collection | PubMed |
description | Direct conversion of CO(2) to a single specific hydrocarbon with high selectivity is extremely attractive but very challenging. Herein, by employing an InZrO(x)-Beta composite catalyst in the CO(2) hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °C and 3.0 MPa, at a CO(2) conversion of 20.4%. Various characterizations and DFT calculation reveal that the generation of methanol-related intermediates by CO(2) hydrogenation is closely related to the surface oxygen vacancies of InZrO(x), which can be tuned through modulating the preparation methods. In contrast, the three-dimensional 12-ring channels of H-Beta conduces to forming higher methylbenzenes and methylnaphthalenes containing isopropyl side-chain, which favors the transformation of methanol-related intermediates to butane through alkyl side-chain elimination and subsequent methylation and hydrogenation. Moreover, the catalytic stability of InZrO(x)-Beta in the CO(2) hydrogenation is considerably improved by a surface silica protection strategy which can effectively inhibit the indium migration. |
format | Online Article Text |
id | pubmed-10164185 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-101641852023-05-08 Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst Wang, Han Fan, Sheng Guo, Shujia Wang, Sen Qin, Zhangfeng Dong, Mei Zhu, Huaqing Fan, Weibin Wang, Jianguo Nat Commun Article Direct conversion of CO(2) to a single specific hydrocarbon with high selectivity is extremely attractive but very challenging. Herein, by employing an InZrO(x)-Beta composite catalyst in the CO(2) hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °C and 3.0 MPa, at a CO(2) conversion of 20.4%. Various characterizations and DFT calculation reveal that the generation of methanol-related intermediates by CO(2) hydrogenation is closely related to the surface oxygen vacancies of InZrO(x), which can be tuned through modulating the preparation methods. In contrast, the three-dimensional 12-ring channels of H-Beta conduces to forming higher methylbenzenes and methylnaphthalenes containing isopropyl side-chain, which favors the transformation of methanol-related intermediates to butane through alkyl side-chain elimination and subsequent methylation and hydrogenation. Moreover, the catalytic stability of InZrO(x)-Beta in the CO(2) hydrogenation is considerably improved by a surface silica protection strategy which can effectively inhibit the indium migration. Nature Publishing Group UK 2023-05-06 /pmc/articles/PMC10164185/ /pubmed/37149644 http://dx.doi.org/10.1038/s41467-023-38336-5 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Wang, Han Fan, Sheng Guo, Shujia Wang, Sen Qin, Zhangfeng Dong, Mei Zhu, Huaqing Fan, Weibin Wang, Jianguo Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title | Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title_full | Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title_fullStr | Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title_full_unstemmed | Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title_short | Selective conversion of CO(2) to isobutane-enriched C(4) alkanes over InZrO(x)-Beta composite catalyst |
title_sort | selective conversion of co(2) to isobutane-enriched c(4) alkanes over inzro(x)-beta composite catalyst |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10164185/ https://www.ncbi.nlm.nih.gov/pubmed/37149644 http://dx.doi.org/10.1038/s41467-023-38336-5 |
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