构建稳定的 Cu-Fe5C2 界面,实现合成气向高级醇的高效转化

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2024-09-19 DOI:10.1016/j.cej.2024.155624
Di Xu, Haifeng Fan, Guoqiang Hou, Kaidi Liu, Yangyang Li, Siyi Huang, Mingyue Ding
{"title":"构建稳定的 Cu-Fe5C2 界面,实现合成气向高级醇的高效转化","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":"{\"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}","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

摘要

在 Cu-Fe 二元催化剂上从合成气中直接高效合成高级醇 (HA) 具有广阔的前景,但由于 Cu-Fe5C2 界面反应网络复杂且稳定性差,因此仍是一项巨大的挑战。在本文中,我们构建了一种 K-CuFe@SiO2 核壳催化剂,该催化剂在 240 ℃ 的温和反应温度下显示出 51.1 % 的高 HA 选择性、14.6 % 的 HA 产率和 15.3 % 的低 CO2 选择性,优于大多数已报道的先进 Cu-Fe 二元催化剂。结构表征证实,二氧化硅壳在长期运行过程中对稳定 Cu-Fe5C2 界面起着关键作用。此外,二氧化硅壳还能调节 K 促进剂和活性相之间的电子相互作用,进而调节 H2 和 CO 的活化。机理研究表明,HA 的合成遵循 *CO-*CHx 耦合机理。H2活化、CO离解活化和非离解活化的平衡是实现*CO-*CHx偶联反应和*CH3CO加氢反应动态匹配的关键,从而最大限度地提高了HAS的活性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Constructing stable Cu-Fe5C2 interfaces for efficient syngas conversion to higher alcohols
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.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
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.
期刊最新文献
Self-assembly nanoparticles potentiate in-situ tumor vaccine of radiotherapy by regulating tumor immunogenicity and tumor-associated macrophages A chirality/microRNA dual-gating theranostic nanomachine for gene silencing therapy Polyimide-Coating-on-Aramid nanofiber strategy toward ultralight organic aerogels with multifunctional properties Innovative 3D Janus foam design achieves high-efficiency and stable solar desalination with improved salt resistance and heat management Constructing stable Cu-Fe5C2 interfaces for efficient syngas conversion to higher alcohols
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1