Kaisi Liu, Tongtong Liu, Xinyi Wu, Jiao Dai, Qingjun Chen, Jun Wan, Lei Liu
{"title":"Frustrated lewis pair chemistry in 2D CeO₂ for efficient alkaline hydrogen evolution","authors":"Kaisi Liu, Tongtong Liu, Xinyi Wu, Jiao Dai, Qingjun Chen, Jun Wan, Lei Liu","doi":"10.1039/d4ta06191h","DOIUrl":null,"url":null,"abstract":"The alkaline hydrogen evolution reaction (HER) is pivotal for sustainable energy production but is hindered by sluggish kinetics due to the necessity of water dissociation to supply protons, which presents a high energy barrier. To overcome this challenge, a novel approach is proposed involving the introduction and tuning of oxygen vacancies on the surface of CeO2 to construct and control frustrated Lewis pairs (FLPs) with dual active sites for enhanced water dissociation. First-principles calculations reveal that increasing the number of oxygen vacancies significantly improves the quantity and activity of FLP sites for efficient water dissociation. Guided by these calculations, 2D CeO2 nanosheets with varying concentrations of oxygen vacancies were synthesized, showing that those with the highest vacancy content exhibit exceptional HER performance, with an overpotential of 132 mV and a Tafel slope of 73 mV·dec-1. These findings validate the theoretical model and underscore the potential of 2D CeO2 with FLP active sites as effective and stable HER catalysts. This study is anticipated to inform the development of advanced catalysts with FLP active sites for hydrogen evolution reactions in alkaline media.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta06191h","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The alkaline hydrogen evolution reaction (HER) is pivotal for sustainable energy production but is hindered by sluggish kinetics due to the necessity of water dissociation to supply protons, which presents a high energy barrier. To overcome this challenge, a novel approach is proposed involving the introduction and tuning of oxygen vacancies on the surface of CeO2 to construct and control frustrated Lewis pairs (FLPs) with dual active sites for enhanced water dissociation. First-principles calculations reveal that increasing the number of oxygen vacancies significantly improves the quantity and activity of FLP sites for efficient water dissociation. Guided by these calculations, 2D CeO2 nanosheets with varying concentrations of oxygen vacancies were synthesized, showing that those with the highest vacancy content exhibit exceptional HER performance, with an overpotential of 132 mV and a Tafel slope of 73 mV·dec-1. These findings validate the theoretical model and underscore the potential of 2D CeO2 with FLP active sites as effective and stable HER catalysts. This study is anticipated to inform the development of advanced catalysts with FLP active sites for hydrogen evolution reactions in alkaline media.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.