An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI:10.1016/S1872-2067(24)60067-7
{"title":"An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction","authors":"","doi":"10.1016/S1872-2067(24)60067-7","DOIUrl":null,"url":null,"abstract":"<div><p>High-entropy alloy (HEA) catalysts exhibit enhanced hydrogen evolution reaction (HER) activity in water electrolysis, yet the understanding of their structure and active sites in reaction environments remains unclear. Here, we systematically investigated the HER activity and stability of PtPdRhRuCu/C through a combination of electrochemical measurements, <em>in situ</em> synchrotron radiation X-ray absorption spectroscopy (XAS) at the Cu <em>K</em>-edge and Pt <em>L</em><sub>3</sub>-edge, and density functional theory (DFT) calculations. Uniformly sized PtPdRhRuCu HEA nanoparticles were prepared <em>via</em> a facile one-step solvothermal method. <em>In situ</em> XAS results revealed that the HEA nanoparticles maintained metallic states and a disordered arrangement of the overall structure at hydrogen evolution potential, implying the absence of the separated phases. Relying on multi-metal active sites, PtPdRhRuCu/C demonstrated a remarkably low overpotential of 23.3 mV at 10 mA cm<sup>–2</sup> in alkaline HER, which is significantly lower than the overpotential observed in commercial Pt/C (50.3 mV), and achieving a mass activity 7.9 times that of Pt/C. DFT calculations show that the synergy of each metal site optimizes the dissociation energy barrier of water molecules. This study not only demonstrates the advancement of high-entropy alloys in electrocatalysis but also provides a comprehensive understanding of the structure-activity relationship of these unique catalysts through detailed characterizations. Our findings further contribute to the rational design and application of high-entropy alloy catalysts, specifically in HER.</p></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":15.7000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600677","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0

Abstract

High-entropy alloy (HEA) catalysts exhibit enhanced hydrogen evolution reaction (HER) activity in water electrolysis, yet the understanding of their structure and active sites in reaction environments remains unclear. Here, we systematically investigated the HER activity and stability of PtPdRhRuCu/C through a combination of electrochemical measurements, in situ synchrotron radiation X-ray absorption spectroscopy (XAS) at the Cu K-edge and Pt L3-edge, and density functional theory (DFT) calculations. Uniformly sized PtPdRhRuCu HEA nanoparticles were prepared via a facile one-step solvothermal method. In situ XAS results revealed that the HEA nanoparticles maintained metallic states and a disordered arrangement of the overall structure at hydrogen evolution potential, implying the absence of the separated phases. Relying on multi-metal active sites, PtPdRhRuCu/C demonstrated a remarkably low overpotential of 23.3 mV at 10 mA cm–2 in alkaline HER, which is significantly lower than the overpotential observed in commercial Pt/C (50.3 mV), and achieving a mass activity 7.9 times that of Pt/C. DFT calculations show that the synergy of each metal site optimizes the dissociation energy barrier of water molecules. This study not only demonstrates the advancement of high-entropy alloys in electrocatalysis but also provides a comprehensive understanding of the structure-activity relationship of these unique catalysts through detailed characterizations. Our findings further contribute to the rational design and application of high-entropy alloy catalysts, specifically in HER.

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
用于氢气进化反应的高效稳定的高熵合金电催化剂
高熵合金(HEA)催化剂在电解水过程中表现出更强的氢进化反应(HER)活性,但人们对其结构和反应环境中的活性位点的了解仍不清楚。在此,我们结合电化学测量、铜 K 边和铂 L3 边的原位同步辐射 X 射线吸收光谱 (XAS) 以及密度泛函理论 (DFT) 计算,系统地研究了 PtPdRhRuCu/C 的氢进化反应活性和稳定性。通过简单的一步溶热法制备了大小均匀的 PtPdRhRuCu HEA 纳米粒子。原位 XAS 结果表明,在氢进化电位下,HEA 纳米粒子保持金属态,整体结构排列无序,这意味着不存在分离相。依靠多金属活性位点,PtPdRhRuCu/C 在碱性 HER 中的过电位非常低,在 10 mA cm-2 的条件下仅为 23.3 mV,大大低于在商用 Pt/C 中观察到的过电位(50.3 mV),其质量活性是 Pt/C 的 7.9 倍。DFT 计算表明,每个金属位点的协同作用优化了水分子的解离能垒。这项研究不仅证明了高熵合金在电催化领域的先进性,还通过详细的表征全面了解了这些独特催化剂的结构-活性关系。我们的发现进一步促进了高熵合金催化剂的合理设计和应用,特别是在 HER 中的应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
期刊最新文献
Mechanism study on the influence of surface properties on the synthesis of dimethyl carbonate from CO2 and methanol over ceria catalysts Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon Unraveling the roles of atomically-dispersed Au in boosting photocatalytic CO2 reduction and aryl alcohol oxidation Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction Activating d10 electronic configuration to regulate p-band centers as efficient active sites for solar energy conversion into H2 by surface atomic arrangement
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1