{"title":"从了解催化剂功能到控制铁基催化剂在 CO2 加氢生成更高碳氢化合物过程中的选择性","authors":"Qingxin Yang, Evgenii V. Kondratenko","doi":"10.1021/accountsmr.4c00160","DOIUrl":null,"url":null,"abstract":"The conversion of carbon dioxide (CO<sub>2</sub>) with hydrogen (H<sub>2</sub>), generated by renewable energy sources, into value-added products is a promising approach to meet future demands for sustainable development. In this context, the hydrogenation of CO<sub>2</sub> (CO<sub>2</sub>-FTS) to higher hydrocarbons (C<sub>2+</sub>), lower olefins, and fuels should be mentioned in particular. These products are used in our daily lives but are currently produced by energy-intensive and CO<sub>2</sub>-emitting oil-based cracking processes. The environmental compatibility and abundance of iron (Fe) used in CO<sub>2</sub>-FTS catalysts are also relevant to sustainable development. The CO<sub>2</sub>-FTS reaction was inspired by the experience accumulated in long-term research on Fischer–Tropsch synthesis with CO (CO-FTS). A simple grafting of catalyst formulations and reaction mechanisms from CO-FTS to CO<sub>2</sub>-FTS has, however, been proven unsatisfactory, likely due to differences in surface adsorbates, chemical potentials of CO and CO<sub>2</sub>, and H<sub>2</sub>O partial pressure. These characteristics affect both the catalyst structure and the reaction pathways. Consequently, CO<sub>2</sub>-FTS provides higher CH<sub>4</sub> selectivity but lower C<sub>2+</sub>-selectivity than does CO-FTS, which appeals to fundamental research to hinder CH<sub>4</sub> formation.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":null,"pages":null},"PeriodicalIF":14.0000,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"From Understanding of Catalyst Functioning toward Controlling Selectivity in CO2 Hydrogenation to Higher Hydrocarbons over Fe-Based Catalysts\",\"authors\":\"Qingxin Yang, Evgenii V. Kondratenko\",\"doi\":\"10.1021/accountsmr.4c00160\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The conversion of carbon dioxide (CO<sub>2</sub>) with hydrogen (H<sub>2</sub>), generated by renewable energy sources, into value-added products is a promising approach to meet future demands for sustainable development. In this context, the hydrogenation of CO<sub>2</sub> (CO<sub>2</sub>-FTS) to higher hydrocarbons (C<sub>2+</sub>), lower olefins, and fuels should be mentioned in particular. These products are used in our daily lives but are currently produced by energy-intensive and CO<sub>2</sub>-emitting oil-based cracking processes. The environmental compatibility and abundance of iron (Fe) used in CO<sub>2</sub>-FTS catalysts are also relevant to sustainable development. The CO<sub>2</sub>-FTS reaction was inspired by the experience accumulated in long-term research on Fischer–Tropsch synthesis with CO (CO-FTS). A simple grafting of catalyst formulations and reaction mechanisms from CO-FTS to CO<sub>2</sub>-FTS has, however, been proven unsatisfactory, likely due to differences in surface adsorbates, chemical potentials of CO and CO<sub>2</sub>, and H<sub>2</sub>O partial pressure. These characteristics affect both the catalyst structure and the reaction pathways. Consequently, CO<sub>2</sub>-FTS provides higher CH<sub>4</sub> selectivity but lower C<sub>2+</sub>-selectivity than does CO-FTS, which appeals to fundamental research to hinder CH<sub>4</sub> formation.\",\"PeriodicalId\":72040,\"journal\":{\"name\":\"Accounts of materials research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.0000,\"publicationDate\":\"2024-09-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Accounts of materials research\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/accountsmr.4c00160\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Accounts of materials research","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/accountsmr.4c00160","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
From Understanding of Catalyst Functioning toward Controlling Selectivity in CO2 Hydrogenation to Higher Hydrocarbons over Fe-Based Catalysts
The conversion of carbon dioxide (CO2) with hydrogen (H2), generated by renewable energy sources, into value-added products is a promising approach to meet future demands for sustainable development. In this context, the hydrogenation of CO2 (CO2-FTS) to higher hydrocarbons (C2+), lower olefins, and fuels should be mentioned in particular. These products are used in our daily lives but are currently produced by energy-intensive and CO2-emitting oil-based cracking processes. The environmental compatibility and abundance of iron (Fe) used in CO2-FTS catalysts are also relevant to sustainable development. The CO2-FTS reaction was inspired by the experience accumulated in long-term research on Fischer–Tropsch synthesis with CO (CO-FTS). A simple grafting of catalyst formulations and reaction mechanisms from CO-FTS to CO2-FTS has, however, been proven unsatisfactory, likely due to differences in surface adsorbates, chemical potentials of CO and CO2, and H2O partial pressure. These characteristics affect both the catalyst structure and the reaction pathways. Consequently, CO2-FTS provides higher CH4 selectivity but lower C2+-selectivity than does CO-FTS, which appeals to fundamental research to hinder CH4 formation.