{"title":"Boosting Hydrogen Evolution Reaction by Sequential Modulation of Elementary Steps on Ru–Ni–P-Coated Cu Nanowires","authors":"Xiaodong Chen, Xiaofei Wei, Zhaojie Wang*, Shoufu Cao, Xiaojing Lin, Xingheng Zhang, Jianye Wang, Siyuan Liu, Shuxian Wei and Xiaoqing Lu*, ","doi":"10.1021/acssuschemeng.4c09858","DOIUrl":null,"url":null,"abstract":"<p >Understanding and controlling the elementary steps in catalytic processes during electrochemical reactions are crucial for advancing sustainable energy technologies. Herein, a promising concept of designing both elementary steps (water adsorption/dissociation and adsorbed hydrogen intermediate desorption) simultaneously is proposed for a robust hydrogen evolution reaction on Ru/Ni–P@Cu. The customized structure affords superb alkaline/neutral HER activity regarding reduced overpotential of 15/26 mV at 10 mA cm<sup>–2</sup>. Notably, the alkaline/neutral HER mass activity (0.66/0.28 A mg<sup>–1</sup>) and price activity (45.66/19.34 A dollar<sup>–1</sup>) of Ru/Ni–P@Cu are 11.8/12.2 and 25.7/26.9 times higher than those of Pt/C, respectively. Experimental results and computational analyses reveal that the accessible Ru–Ni–P moieties on the interface confers the desired electronic structure, thereby promoting first elementary reaction of H<sub>2</sub>O adsorption/dissociation, and simultaneously accelerating second elementary reaction of H* intermediate desorption via a hydrogen spillover. This work affords a transformative paradigm for elevating multistep catalytic reaction kinetics and paves the way for synergistic advancements in catalyst performance and cost-effectiveness.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 6","pages":"2586–2595 2586–2595"},"PeriodicalIF":7.3000,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c09858","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
Abstract
Understanding and controlling the elementary steps in catalytic processes during electrochemical reactions are crucial for advancing sustainable energy technologies. Herein, a promising concept of designing both elementary steps (water adsorption/dissociation and adsorbed hydrogen intermediate desorption) simultaneously is proposed for a robust hydrogen evolution reaction on Ru/Ni–P@Cu. The customized structure affords superb alkaline/neutral HER activity regarding reduced overpotential of 15/26 mV at 10 mA cm–2. Notably, the alkaline/neutral HER mass activity (0.66/0.28 A mg–1) and price activity (45.66/19.34 A dollar–1) of Ru/Ni–P@Cu are 11.8/12.2 and 25.7/26.9 times higher than those of Pt/C, respectively. Experimental results and computational analyses reveal that the accessible Ru–Ni–P moieties on the interface confers the desired electronic structure, thereby promoting first elementary reaction of H2O adsorption/dissociation, and simultaneously accelerating second elementary reaction of H* intermediate desorption via a hydrogen spillover. This work affords a transformative paradigm for elevating multistep catalytic reaction kinetics and paves the way for synergistic advancements in catalyst performance and cost-effectiveness.
了解和控制电化学反应中催化过程的基本步骤对推进可持续能源技术至关重要。本文提出了一个有希望的概念,即同时设计两个基本步骤(水吸附/解离和吸附的氢中间体解吸),以实现Ru/Ni - P@Cu上稳健的析氢反应。定制的结构提供了极好的碱性/中性HER活性,在10 mA cm-2下降低了15/26 mV的过电位。Ru/Ni - P@Cu的碱性/中性HER质量活性(0.66/0.28 A mg-1)和价格活性(45.66/19.34 A dollar-1)分别是Pt/C的11.8/12.2和25.7/26.9倍。实验结果和计算分析表明,界面上可接近的Ru-Ni-P基团提供了所需的电子结构,从而促进了H2O吸附/解离的第一元素反应,同时通过氢溢出加速了H*中间脱附的第二元素反应。这项工作为提高多步催化反应动力学提供了一个变革性的范例,并为催化剂性能和成本效益的协同进步铺平了道路。
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.