{"title":"Constructing stable Cu-Fe5C2 interfaces for efficient syngas conversion to higher alcohols","authors":"Di Xu, Haifeng Fan, Guoqiang Hou, Kaidi Liu, Yangyang Li, Siyi Huang, Mingyue Ding","doi":"10.1016/j.cej.2024.155624","DOIUrl":null,"url":null,"abstract":"Direct and efficient synthesis of higher alcohols (HA) from syngas over Cu-Fe binary catalysts is promising, but remaining big challenge due to the complex reaction networks and poor stability of Cu-Fe<ce:inf loc=\"post\">5</ce:inf>C<ce:inf loc=\"post\">2</ce:inf> interfaces. Herein, we constructed a K-CuFe@SiO<ce:inf loc=\"post\">2</ce:inf> core–shell catalyst, which showed high HA selectivity of 51.1 %, HA yield of 14.6 % and low CO<ce:inf loc=\"post\">2</ce:inf> selectivity of 15.3 % at a mild reaction temperature of 240 °C, outperforming most of the reported advanced Cu-Fe binary catalysts. Structural characterizations confirmed that SiO<ce:inf loc=\"post\">2</ce:inf> shell played critical role in stabilizing Cu-Fe<ce:inf loc=\"post\">5</ce:inf>C<ce:inf loc=\"post\">2</ce:inf> interfaces during long-term operation. Moreover, SiO<ce:inf loc=\"post\">2</ce:inf> shell could regulate the electronic interactions between K promoter and active phases, and then regulating the H<ce:inf loc=\"post\">2</ce:inf> and CO activations. Mechanism studies suggested that HA synthesis followed *CO–*CH<ce:inf loc=\"post\">x</ce:inf> coupling mechanism. The balance of H<ce:inf loc=\"post\">2</ce:inf> activation, CO dissociated and non-dissociated activation was critical to realize the dynamic matching of *CO–*CH<ce:inf loc=\"post\">x</ce:inf> coupling and *CH<ce:inf loc=\"post\">3</ce:inf>CO hydrogenation reactions, thus maximizing HAS activity.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":null,"pages":null},"PeriodicalIF":13.3000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.155624","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Direct and efficient synthesis of higher alcohols (HA) from syngas over Cu-Fe binary catalysts is promising, but remaining big challenge due to the complex reaction networks and poor stability of Cu-Fe5C2 interfaces. Herein, we constructed a K-CuFe@SiO2 core–shell catalyst, which showed high HA selectivity of 51.1 %, HA yield of 14.6 % and low CO2 selectivity of 15.3 % at a mild reaction temperature of 240 °C, outperforming most of the reported advanced Cu-Fe binary catalysts. Structural characterizations confirmed that SiO2 shell played critical role in stabilizing Cu-Fe5C2 interfaces during long-term operation. Moreover, SiO2 shell could regulate the electronic interactions between K promoter and active phases, and then regulating the H2 and CO activations. Mechanism studies suggested that HA synthesis followed *CO–*CHx coupling mechanism. The balance of H2 activation, CO dissociated and non-dissociated activation was critical to realize the dynamic matching of *CO–*CHx coupling and *CH3CO hydrogenation reactions, thus maximizing HAS activity.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.