{"title":"Mechanistic insights into the hydrogen evolution reaction catalyzed by ConMoP (n = 1–5) clusters","authors":"Tinghui Wu, Zhigang Fang","doi":"10.1016/j.chemphys.2024.112527","DOIUrl":null,"url":null,"abstract":"<div><div>To investigate the catalytic activity of Co<em><sub>n</sub></em>MoP (n = 1–5) clusters with water molecules for hydrogen evolution reaction (HER), a systematic analysis was performed using density functional theory (DFT). Using the B3LYP functional and def2-TZVP basis set, the structures of the clusters with different spin multiplicities were optimized and theoretically calculated using the Gaussian16 software package. To evaluate the catalytic performance of these clusters, we focused on analyzing their HOMO-LUMO energy gaps, Gibbs free energy changes (Δ<em>G</em>), and electron density distributions. The results show that the Δ<em>G</em><sub>H*</sub> value of configuration 1-a is closest to 0, indicating its excellent catalytic performance for HER; additionally, the Co atom was identified as the primary active site. Configuration (5-b)-H<sub>ads</sub> exhibited the smallest energy gap, demonstrating the strongest catalytic activity. Configurations 1-a, 2-a, and 5-b were identified as the most promising catalysts in this series of clusters. This study reveals the behavior of transition metal clusters in catalytic reactions and provides a reference for future experimental and theoretical research.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"590 ","pages":"Article 112527"},"PeriodicalIF":2.0000,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0301010424003562","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
To investigate the catalytic activity of ConMoP (n = 1–5) clusters with water molecules for hydrogen evolution reaction (HER), a systematic analysis was performed using density functional theory (DFT). Using the B3LYP functional and def2-TZVP basis set, the structures of the clusters with different spin multiplicities were optimized and theoretically calculated using the Gaussian16 software package. To evaluate the catalytic performance of these clusters, we focused on analyzing their HOMO-LUMO energy gaps, Gibbs free energy changes (ΔG), and electron density distributions. The results show that the ΔGH* value of configuration 1-a is closest to 0, indicating its excellent catalytic performance for HER; additionally, the Co atom was identified as the primary active site. Configuration (5-b)-Hads exhibited the smallest energy gap, demonstrating the strongest catalytic activity. Configurations 1-a, 2-a, and 5-b were identified as the most promising catalysts in this series of clusters. This study reveals the behavior of transition metal clusters in catalytic reactions and provides a reference for future experimental and theoretical research.
期刊介绍:
Chemical Physics publishes experimental and theoretical papers on all aspects of chemical physics. In this journal, experiments are related to theory, and in turn theoretical papers are related to present or future experiments. Subjects covered include: spectroscopy and molecular structure, interacting systems, relaxation phenomena, biological systems, materials, fundamental problems in molecular reactivity, molecular quantum theory and statistical mechanics. Computational chemistry studies of routine character are not appropriate for this journal.