{"title":"通过配体工程策略制备的六原子铂催化剂用于高效氢氧化反应","authors":"Li Yan, Dunchao Wang, Mengjiao Li, Ruihu Lu, Mengge Lu, Panpan Li, Kaiyue Wang, Shao Jin, Ziyun Wang, Shubo Tian","doi":"10.1002/anie.202410832","DOIUrl":null,"url":null,"abstract":"<p><p>Atomically precise supported nanocluster catalysts (APSNCs), which feature exact atomic composition, well-defined structures, and unique catalytic properties, offer an exceptional platform for understanding the structure-performance relationship at the atomic level. However, fabricating APSNCs with precisely controlled and uniform metal atom numbers, as well as maintaining a stable structure, remains a significant challenge due to uncontrollable dispersion and easy aggregation during synthetic and catalytic processes. Herein, we developed an effective ligand engineering strategy to construct a Pt<sub>6</sub> nanocluster catalyst stabilized on oxidized carbon nanotubes (Pt<sub>6</sub>/OCNT). The structural analysis revealed that Pt<sub>6</sub> nanoclusters in Pt<sub>6</sub>/OCNT were fully exposed and exhibited a planar structure. Furthermore, the obtained Pt<sub>6</sub>/OCNT exhibited outstanding acidic HOR performances with a high mass activity of 18.37 A ⋅ mg<sub>pt</sub> <sup>-1</sup> along with excellent stability during a 24 h constant operation and good CO tolerance, surpassing those of the commercial Pt/C. Density functional theory (DFT) calculations demonstrated that the unique geometric and electronic structures of Pt<sub>6</sub> nanoclusters on OCNT altered the hydrogen adsorption energies on catalytic sites and thus lowered the HOR theoretical overpotential. This work presents a new prospect for designing and synthesizing advanced APSNCs for efficient energy electrocatalysis.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":null,"pages":null},"PeriodicalIF":16.1000,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hexa-atom Pt Catalyst Fabricated by a Ligand Engineering Strategy for Efficient Hydrogen Oxidation Reaction.\",\"authors\":\"Li Yan, Dunchao Wang, Mengjiao Li, Ruihu Lu, Mengge Lu, Panpan Li, Kaiyue Wang, Shao Jin, Ziyun Wang, Shubo Tian\",\"doi\":\"10.1002/anie.202410832\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Atomically precise supported nanocluster catalysts (APSNCs), which feature exact atomic composition, well-defined structures, and unique catalytic properties, offer an exceptional platform for understanding the structure-performance relationship at the atomic level. However, fabricating APSNCs with precisely controlled and uniform metal atom numbers, as well as maintaining a stable structure, remains a significant challenge due to uncontrollable dispersion and easy aggregation during synthetic and catalytic processes. Herein, we developed an effective ligand engineering strategy to construct a Pt<sub>6</sub> nanocluster catalyst stabilized on oxidized carbon nanotubes (Pt<sub>6</sub>/OCNT). The structural analysis revealed that Pt<sub>6</sub> nanoclusters in Pt<sub>6</sub>/OCNT were fully exposed and exhibited a planar structure. Furthermore, the obtained Pt<sub>6</sub>/OCNT exhibited outstanding acidic HOR performances with a high mass activity of 18.37 A ⋅ mg<sub>pt</sub> <sup>-1</sup> along with excellent stability during a 24 h constant operation and good CO tolerance, surpassing those of the commercial Pt/C. Density functional theory (DFT) calculations demonstrated that the unique geometric and electronic structures of Pt<sub>6</sub> nanoclusters on OCNT altered the hydrogen adsorption energies on catalytic sites and thus lowered the HOR theoretical overpotential. This work presents a new prospect for designing and synthesizing advanced APSNCs for efficient energy electrocatalysis.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2024-07-08\",\"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.202410832\",\"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.202410832","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
原子精确支撑纳米簇催化剂(APSNCs)具有精确的原子组成、定义明确的结构和独特的催化特性,为了解原子水平的结构-性能关系提供了一个特殊的平台。然而,在合成和催化过程中,由于金属原子数量不可控且容易聚集,要制造出具有精确控制和均匀金属原子数量并保持稳定结构的 APSNCs 仍是一项重大挑战。在此,我们开发了一种有效的配体工程策略,构建了稳定在氧化碳纳米管(Pt6/OCNT)上的 Pt6 纳米簇催化剂。结构分析表明,Pt6/OCNT 中的 Pt6 纳米簇完全暴露并呈现平面结构。此外,所获得的 Pt6/OCNT 具有出色的酸性 HOR 性能,其质量活性高达 18.37 A-mgpt-1,在 24 小时持续运行期间具有出色的稳定性和良好的 CO 耐受性,超过了商用 Pt/C。密度泛函理论(DFT)计算表明,OCNT 上 Pt6 纳米团簇独特的几何和电子结构改变了催化位点上的氢吸附能,从而降低了 HOR 理论过电位。这项工作为设计和合成用于高效能源电催化的先进 APSNCs 提供了新的前景。
Hexa-atom Pt Catalyst Fabricated by a Ligand Engineering Strategy for Efficient Hydrogen Oxidation Reaction.
Atomically precise supported nanocluster catalysts (APSNCs), which feature exact atomic composition, well-defined structures, and unique catalytic properties, offer an exceptional platform for understanding the structure-performance relationship at the atomic level. However, fabricating APSNCs with precisely controlled and uniform metal atom numbers, as well as maintaining a stable structure, remains a significant challenge due to uncontrollable dispersion and easy aggregation during synthetic and catalytic processes. Herein, we developed an effective ligand engineering strategy to construct a Pt6 nanocluster catalyst stabilized on oxidized carbon nanotubes (Pt6/OCNT). The structural analysis revealed that Pt6 nanoclusters in Pt6/OCNT were fully exposed and exhibited a planar structure. Furthermore, the obtained Pt6/OCNT exhibited outstanding acidic HOR performances with a high mass activity of 18.37 A ⋅ mgpt-1 along with excellent stability during a 24 h constant operation and good CO tolerance, surpassing those of the commercial Pt/C. Density functional theory (DFT) calculations demonstrated that the unique geometric and electronic structures of Pt6 nanoclusters on OCNT altered the hydrogen adsorption energies on catalytic sites and thus lowered the HOR theoretical overpotential. This work presents a new prospect for designing and synthesizing advanced APSNCs for efficient energy electrocatalysis.
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.