Yi Jing Jia, Jin Quan Tao, Hao Ran Liu, Wen Bin Huang, Rongpeng Yao, Miaomiao Niu, Rongrong Li, Qiang Wei, Ya Song Zhou
{"title":"钴钾协同改性对二氧化碳加氢制取低碳烯烃的铁基催化剂的影响","authors":"Yi Jing Jia, Jin Quan Tao, Hao Ran Liu, Wen Bin Huang, Rongpeng Yao, Miaomiao Niu, Rongrong Li, Qiang Wei, Ya Song Zhou","doi":"10.1002/aoc.7715","DOIUrl":null,"url":null,"abstract":"<div>\n \n <p>To enhance the CO<sub>2</sub> hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al<sub>2</sub>O<sub>3</sub> catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H<sub>2</sub>-TPR, XPS, CO<sub>2</sub>-TPD, NH<sub>3</sub>-TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO<sub>2</sub> hydrogenation activity and low-carbon olefin selectivity of Fe/Al<sub>2</sub>O<sub>3</sub> catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO<sub>2</sub>, while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C<sub>2+</sub> hydrocarbon products. Under the synergistic effect of K and Co, the CO<sub>2</sub> conversion activity of the Fe-based catalyst significantly increased, achieving a CO<sub>2</sub> conversion rate of 37%, while the selectivity towards C<sub>2</sub>-C<sub>4=</sub> increased to 31.9%.</p>\n </div>","PeriodicalId":8344,"journal":{"name":"Applied Organometallic Chemistry","volume":"38 12","pages":""},"PeriodicalIF":3.7000,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cobalt-Potassium Synergistic Modification Effects on Fe-Based Catalysts for CO2 Hydrogenation to Low-Carbon Olefins\",\"authors\":\"Yi Jing Jia, Jin Quan Tao, Hao Ran Liu, Wen Bin Huang, Rongpeng Yao, Miaomiao Niu, Rongrong Li, Qiang Wei, Ya Song Zhou\",\"doi\":\"10.1002/aoc.7715\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div>\\n \\n <p>To enhance the CO<sub>2</sub> hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al<sub>2</sub>O<sub>3</sub> catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H<sub>2</sub>-TPR, XPS, CO<sub>2</sub>-TPD, NH<sub>3</sub>-TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO<sub>2</sub> hydrogenation activity and low-carbon olefin selectivity of Fe/Al<sub>2</sub>O<sub>3</sub> catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO<sub>2</sub>, while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C<sub>2+</sub> hydrocarbon products. Under the synergistic effect of K and Co, the CO<sub>2</sub> conversion activity of the Fe-based catalyst significantly increased, achieving a CO<sub>2</sub> conversion rate of 37%, while the selectivity towards C<sub>2</sub>-C<sub>4=</sub> increased to 31.9%.</p>\\n </div>\",\"PeriodicalId\":8344,\"journal\":{\"name\":\"Applied Organometallic Chemistry\",\"volume\":\"38 12\",\"pages\":\"\"},\"PeriodicalIF\":3.7000,\"publicationDate\":\"2024-09-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Organometallic Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/aoc.7715\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Organometallic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/aoc.7715","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
为提高铁基催化剂的二氧化碳加氢活性和低碳烯烃选择性,提出了一种在催化剂制备过程中使用金属促进剂调节活性金属中心结构的策略。在铁/Al2O3 催化剂中引入改性剂 K 和/或 Co 时,采用了初湿浸渍法。采用 XRD、BET、SEM、HRTEM、H2-TPR、XPS、CO2-TPD、NH3-TPD 和 TG 等表征技术研究了改性剂对活性金属物种的分散性、还原性、电子特性和酸碱特性的影响。此外,还探讨了 K 和 Co 改性对 Fe/Al2O3 催化剂 CO2 加氢活性和低碳烯烃选择性的影响。结果表明,K 的引入在催化剂中产生了更多的碱性位点和富含电子的活性金属中心,促进了 CO2 的吸附和活化,同时抑制了烯烃的氢化和甲烷的生成,从而提高了对低碳烯烃的选择性。Co 促进剂促进了 Fe 物种的分散,暴露出更多的活性位点,提高了 FTS 反应活性,导致更多的 CO 转化为 C2+ 碳氢化合物产物。在 K 和 Co 的协同作用下,铁基催化剂的 CO2 转化活性显著提高,CO2 转化率达到 37%,对 C2-C4= 的选择性提高到 31.9%。
Cobalt-Potassium Synergistic Modification Effects on Fe-Based Catalysts for CO2 Hydrogenation to Low-Carbon Olefins
To enhance the CO2 hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al2O3 catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H2-TPR, XPS, CO2-TPD, NH3-TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO2 hydrogenation activity and low-carbon olefin selectivity of Fe/Al2O3 catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO2, while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C2+ hydrocarbon products. Under the synergistic effect of K and Co, the CO2 conversion activity of the Fe-based catalyst significantly increased, achieving a CO2 conversion rate of 37%, while the selectivity towards C2-C4= increased to 31.9%.
期刊介绍:
All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.