{"title":"不对称乙炔活化增强了电化学乙烯形成动力学。","authors":"Yanran Han,Chuanqi Cheng,Fanpeng Chen,Bin Zhang,Bo-Hang Zhao","doi":"10.1002/anie.202516885","DOIUrl":null,"url":null,"abstract":"Copper (Cu)-based catalysts with weak ethylene (C2H4) adsorption exhibit a robust ability to suppress the overhydrogenation of electrocatalytic acetylene (C2H2) hydrogenation (EAH), providing a green alternative for C2H4 production. However, the unsatisfactory C2H4 formation kinetics due to the sluggishness of C2H2 reactants still limit its practical application potential. Herein, borate-decorated oxide-derived copper nanoparticles (OD Cu-B NPs) are designed to promote C2H2 activation and adsorption. As a result, the as-prepared catalysts deliver a partial current density of 720 mA cm-2 with a turnover frequency of 48.33 s-1, greatly outperforming the bare OD Cu counterpart. The symmetric electron distribution of C2H2 is revealed to be broken over the Cu-borate interface, making it easier to activate and adsorb, which accounts for the lowered hydrogenation barrier and enhanced selectivity, consequently promoting C2H4 formation kinetics through the EAH process.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"39 1","pages":"e202516885"},"PeriodicalIF":16.9000,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Asymmetric Acetylene Activation Enables Enhanced Electrochemical Ethylene Formation Kinetics.\",\"authors\":\"Yanran Han,Chuanqi Cheng,Fanpeng Chen,Bin Zhang,Bo-Hang Zhao\",\"doi\":\"10.1002/anie.202516885\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Copper (Cu)-based catalysts with weak ethylene (C2H4) adsorption exhibit a robust ability to suppress the overhydrogenation of electrocatalytic acetylene (C2H2) hydrogenation (EAH), providing a green alternative for C2H4 production. However, the unsatisfactory C2H4 formation kinetics due to the sluggishness of C2H2 reactants still limit its practical application potential. Herein, borate-decorated oxide-derived copper nanoparticles (OD Cu-B NPs) are designed to promote C2H2 activation and adsorption. As a result, the as-prepared catalysts deliver a partial current density of 720 mA cm-2 with a turnover frequency of 48.33 s-1, greatly outperforming the bare OD Cu counterpart. The symmetric electron distribution of C2H2 is revealed to be broken over the Cu-borate interface, making it easier to activate and adsorb, which accounts for the lowered hydrogenation barrier and enhanced selectivity, consequently promoting C2H4 formation kinetics through the EAH process.\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\"39 1\",\"pages\":\"e202516885\"},\"PeriodicalIF\":16.9000,\"publicationDate\":\"2025-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202516885\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202516885","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
弱乙烯(C2H4)吸附铜(Cu)基催化剂对电催化乙炔(C2H2)加氢反应(EAH)的过加氢反应具有较强的抑制作用,为C2H4的生产提供了绿色替代方案。然而,由于C2H2反应物反应缓慢,导致C2H4生成动力学不理想,限制了其实际应用潜力。本文设计了硼酸修饰的氧化物衍生铜纳米粒子(OD Cu-B NPs),以促进C2H2的活化和吸附。结果表明,所制备的催化剂的局部电流密度为720 mA cm-2,周转频率为48.33 s-1,大大优于裸外径铜催化剂。C2H2的对称电子分布在cu -硼酸盐界面上被打破,使其更容易被激活和吸附,从而降低了氢化势垒,提高了选择性,从而促进了EAH过程中C2H4的形成动力学。
Copper (Cu)-based catalysts with weak ethylene (C2H4) adsorption exhibit a robust ability to suppress the overhydrogenation of electrocatalytic acetylene (C2H2) hydrogenation (EAH), providing a green alternative for C2H4 production. However, the unsatisfactory C2H4 formation kinetics due to the sluggishness of C2H2 reactants still limit its practical application potential. Herein, borate-decorated oxide-derived copper nanoparticles (OD Cu-B NPs) are designed to promote C2H2 activation and adsorption. As a result, the as-prepared catalysts deliver a partial current density of 720 mA cm-2 with a turnover frequency of 48.33 s-1, greatly outperforming the bare OD Cu counterpart. The symmetric electron distribution of C2H2 is revealed to be broken over the Cu-borate interface, making it easier to activate and adsorb, which accounts for the lowered hydrogenation barrier and enhanced selectivity, consequently promoting C2H4 formation kinetics through the EAH process.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.