Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst
Abstract Direct conversion of CO2 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 CO2 hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under...
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Nature Portfolio
2023-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38336-5 |
| _version_ | 1797832050160435200 |
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| author | Han Wang Sheng Fan Shujia Guo Sen Wang Zhangfeng Qin Mei Dong Huaqing Zhu Weibin Fan Jianguo Wang |
| author_facet | Han Wang Sheng Fan Shujia Guo Sen Wang Zhangfeng Qin Mei Dong Huaqing Zhu Weibin Fan Jianguo Wang |
| author_sort | Han Wang |
| collection | DOAJ |
| description | Abstract Direct conversion of CO2 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 CO2 hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °C and 3.0 MPa, at a CO2 conversion of 20.4%. Various characterizations and DFT calculation reveal that the generation of methanol-related intermediates by CO2 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 CO2 hydrogenation is considerably improved by a surface silica protection strategy which can effectively inhibit the indium migration. |
| first_indexed | 2024-04-09T14:01:32Z |
| format | Article |
| id | doaj.art-d0a4d069f5da4c889b51a880a9d779bb |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-09T14:01:32Z |
| publishDate | 2023-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-d0a4d069f5da4c889b51a880a9d779bb2023-05-07T11:17:18ZengNature PortfolioNature Communications2041-17232023-05-0114111410.1038/s41467-023-38336-5Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalystHan Wang0Sheng Fan1Shujia Guo2Sen Wang3Zhangfeng Qin4Mei Dong5Huaqing Zhu6Weibin Fan7Jianguo Wang8State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of SciencesAbstract Direct conversion of CO2 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 CO2 hydrogenation, a high selectivity of 53.4% to butane is achieved in hydrocarbons (CO free) under 315 °C and 3.0 MPa, at a CO2 conversion of 20.4%. Various characterizations and DFT calculation reveal that the generation of methanol-related intermediates by CO2 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 CO2 hydrogenation is considerably improved by a surface silica protection strategy which can effectively inhibit the indium migration.https://doi.org/10.1038/s41467-023-38336-5 |
| spellingShingle | Han Wang Sheng Fan Shujia Guo Sen Wang Zhangfeng Qin Mei Dong Huaqing Zhu Weibin Fan Jianguo Wang Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst Nature Communications |
| title | Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst |
| title_full | Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst |
| title_fullStr | Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst |
| title_full_unstemmed | Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst |
| title_short | Selective conversion of CO2 to isobutane-enriched C4 alkanes over InZrO x -Beta composite catalyst |
| title_sort | selective conversion of co2 to isobutane enriched c4 alkanes over inzro x beta composite catalyst |
| url | https://doi.org/10.1038/s41467-023-38336-5 |
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