{"title":"邻近的铁锰双金属位点对提高二氧化碳加氢性能的协同效应","authors":"Haoting Liang, Qiao Zhao, Shengkun Liu, Chongyang Wei, Yidan Wang, Yue Wang, Shouying Huang, Xinbin Ma","doi":"10.1007/s11705-024-2491-4","DOIUrl":null,"url":null,"abstract":"<div><p>The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO<sub>2</sub> into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO<sub>2</sub> hydrogenation activity and inhibited CH<sub>4</sub> formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H<sub>2</sub> temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO<sub>2</sub> and the identification of reaction intermediates were analyzed using CO<sub>2</sub>-temperature programed desorption and <i>in situ</i> Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO<sub>2</sub> adsorption and the formation of HCOO* species, ultimately leading to increased CO<sub>2</sub> conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 11","pages":""},"PeriodicalIF":4.3000,"publicationDate":"2024-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic effect of Fe-Mn bimetallic sites with close proximity for enhanced CO2 hydrogenation performance\",\"authors\":\"Haoting Liang, Qiao Zhao, Shengkun Liu, Chongyang Wei, Yidan Wang, Yue Wang, Shouying Huang, Xinbin Ma\",\"doi\":\"10.1007/s11705-024-2491-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO<sub>2</sub> into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO<sub>2</sub> hydrogenation activity and inhibited CH<sub>4</sub> formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H<sub>2</sub> temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO<sub>2</sub> and the identification of reaction intermediates were analyzed using CO<sub>2</sub>-temperature programed desorption and <i>in situ</i> Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO<sub>2</sub> adsorption and the formation of HCOO* species, ultimately leading to increased CO<sub>2</sub> conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.\\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":571,\"journal\":{\"name\":\"Frontiers of Chemical Science and Engineering\",\"volume\":\"18 11\",\"pages\":\"\"},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2024-07-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Frontiers of Chemical Science and Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11705-024-2491-4\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Frontiers of Chemical Science and Engineering","FirstCategoryId":"5","ListUrlMain":"https://link.springer.com/article/10.1007/s11705-024-2491-4","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
铁锰双金属催化剂是将二氧化碳转化为高附加值化学品的潜在候选催化剂。然而,两种金属之间的相互作用在决定催化性能方面起着重要作用,这一点仍存在争议。在本研究中,我们旨在研究调整具有相似纳米颗粒尺寸的铁锰双金属催化剂的接近度所产生的影响。并研究了其对催化剂理化性质和相应性能的影响。结果发现,Fe-Mn 间的距离越近,CO2 加氢活性越强,同时抑制了 CH4 的生成。利用 X 射线衍射、H2 温度编程还原和 X 射线光电子能谱对所制备催化剂的理化性质进行了表征,结果表明,较近的铁-锰距离促进了电子从锰向铁的转移,从而促进了铁的渗碳。利用 CO2 温度编程解吸和原位傅立叶变换红外光谱分析了 CO2 的吸附行为和反应中间产物的鉴定,证实了亲密的 Fe-Mn 位点有助于 CO2 的吸附和 HCOO* 物种的形成,最终提高了 CO2 转化率和碳氢化合物产量。这项研究发现了铁锰亲密位点的协同效应,为深入了解活性位点与促进剂之间的关系提供了宝贵的见解。
Synergistic effect of Fe-Mn bimetallic sites with close proximity for enhanced CO2 hydrogenation performance
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO2 hydrogenation activity and inhibited CH4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO2 and the identification of reaction intermediates were analyzed using CO2-temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO2 adsorption and the formation of HCOO* species, ultimately leading to increased CO2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
期刊介绍:
Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.