Wenhao Yang, Qi Huang, Yingying Yan, Yaozhou Li, Tingting Xu, Ao Yu, Yihang Zhao, Ping Peng, Ying Wang, Luis Echegoyen, Fang-Fang Li
{"title":"C60 富勒烯诱导的金属离子还原:具有高电催化氢气进化性能的 C60-金属簇异质结构的合成。","authors":"Wenhao Yang, Qi Huang, Yingying Yan, Yaozhou Li, Tingting Xu, Ao Yu, Yihang Zhao, Ping Peng, Ying Wang, Luis Echegoyen, Fang-Fang Li","doi":"10.1002/anie.202414149","DOIUrl":null,"url":null,"abstract":"<p>Metal clusters, due to their small dimensions, contain a high proportion of surface atoms, thus possessing a significantly improved catalytic activity compared with their bulk counterparts and nanoparticles. Defective and modified carbon supports are effective in stabilizing metal clusters, however, the synthesis of isolated metal clusters still requires multiple steps and harsh conditions. Herein, we develop a C<sub>60</sub> fullerene-driven spontaneous metal deposition process, where C<sub>60</sub> serves as both a reductant and an anchor, to achieve uniform metal (Rh, Ir, Pt, Pd, Au and Ru) clusters without the need for any defects or functional groups on C<sub>60</sub>. Density functional theory calculations reveal that C<sub>60</sub> possesses multiple strong metal adsorption sites, which favors stable and uniform deposition of metal atoms. In addition, owing to the electron-withdrawing properties of C<sub>60</sub>, the electronic structures of metal clusters are effectively regulated, not only optimizing the adsorption behavior of reaction intermediates but also accelerating the kinetics of hydrogen evolution reaction. The synthesized Ru/C<sub>60</sub>-300 exhibits remarkable performance for hydrogen evolution in an alkaline condition. This study demonstrates a facile and efficient method for synthesizing effective fullerene-supported metal cluster catalysts without any pretreatment and additional reducing agent.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"64 2","pages":""},"PeriodicalIF":16.9000,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"C60 Fullerene-Induced Reduction of Metal Ions: Synthesis of C60-Metal Cluster Heterostructures with High Electrocatalytic Hydrogen-Evolution Performance\",\"authors\":\"Wenhao Yang, Qi Huang, Yingying Yan, Yaozhou Li, Tingting Xu, Ao Yu, Yihang Zhao, Ping Peng, Ying Wang, Luis Echegoyen, Fang-Fang Li\",\"doi\":\"10.1002/anie.202414149\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Metal clusters, due to their small dimensions, contain a high proportion of surface atoms, thus possessing a significantly improved catalytic activity compared with their bulk counterparts and nanoparticles. Defective and modified carbon supports are effective in stabilizing metal clusters, however, the synthesis of isolated metal clusters still requires multiple steps and harsh conditions. Herein, we develop a C<sub>60</sub> fullerene-driven spontaneous metal deposition process, where C<sub>60</sub> serves as both a reductant and an anchor, to achieve uniform metal (Rh, Ir, Pt, Pd, Au and Ru) clusters without the need for any defects or functional groups on C<sub>60</sub>. Density functional theory calculations reveal that C<sub>60</sub> possesses multiple strong metal adsorption sites, which favors stable and uniform deposition of metal atoms. In addition, owing to the electron-withdrawing properties of C<sub>60</sub>, the electronic structures of metal clusters are effectively regulated, not only optimizing the adsorption behavior of reaction intermediates but also accelerating the kinetics of hydrogen evolution reaction. The synthesized Ru/C<sub>60</sub>-300 exhibits remarkable performance for hydrogen evolution in an alkaline condition. This study demonstrates a facile and efficient method for synthesizing effective fullerene-supported metal cluster catalysts without any pretreatment and additional reducing agent.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\"64 2\",\"pages\":\"\"},\"PeriodicalIF\":16.9000,\"publicationDate\":\"2024-09-05\",\"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://onlinelibrary.wiley.com/doi/10.1002/anie.202414149\",\"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://onlinelibrary.wiley.com/doi/10.1002/anie.202414149","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
C60 Fullerene-Induced Reduction of Metal Ions: Synthesis of C60-Metal Cluster Heterostructures with High Electrocatalytic Hydrogen-Evolution Performance
Metal clusters, due to their small dimensions, contain a high proportion of surface atoms, thus possessing a significantly improved catalytic activity compared with their bulk counterparts and nanoparticles. Defective and modified carbon supports are effective in stabilizing metal clusters, however, the synthesis of isolated metal clusters still requires multiple steps and harsh conditions. Herein, we develop a C60 fullerene-driven spontaneous metal deposition process, where C60 serves as both a reductant and an anchor, to achieve uniform metal (Rh, Ir, Pt, Pd, Au and Ru) clusters without the need for any defects or functional groups on C60. Density functional theory calculations reveal that C60 possesses multiple strong metal adsorption sites, which favors stable and uniform deposition of metal atoms. In addition, owing to the electron-withdrawing properties of C60, the electronic structures of metal clusters are effectively regulated, not only optimizing the adsorption behavior of reaction intermediates but also accelerating the kinetics of hydrogen evolution reaction. The synthesized Ru/C60-300 exhibits remarkable performance for hydrogen evolution in an alkaline condition. This study demonstrates a facile and efficient method for synthesizing effective fullerene-supported metal cluster catalysts without any pretreatment and additional reducing agent.
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.