Modulating the Local Charge Distribution of Single-Atomic Ru Sites for an Efficient Hydrogen Evolution Reaction

IF 19.5 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon Energy Pub Date : 2025-03-07 DOI:10.1002/cey2.690

Youyu Long, Lingfeng Yang, Min Xi, Yifan Zhao, Hua Zhang, Tingting Liu, Anran Chen, Xuguang An, Guangzhi Hu, Zitao Ni

{"title":"Modulating the Local Charge Distribution of Single-Atomic Ru Sites for an Efficient Hydrogen Evolution Reaction","authors":"Youyu Long, Lingfeng Yang, Min Xi, Yifan Zhao, Hua Zhang, Tingting Liu, Anran Chen, Xuguang An, Guangzhi Hu, Zitao Ni","doi":"10.1002/cey2.690","DOIUrl":null,"url":null,"abstract":"Ruthenium (Ru)-based electrocatalysts show great promise as substitutes for platinum (Pt) for the alkaline hydrogen evolution reaction (HER) because of their efficient water dissociation capabilities. Nevertheless, the strong adsorption of Ru–OH intermediates (Ru-OHad) blocks the active site, leading to unsatisfactory HER performance. In this study, we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP–CoP heterostructure-anchored Ru single-atom site catalyst (Ru-FeP-CoP/NPC). The obtained catalyst shows a low overpotential (28 mV at 10 mA cm−2) and a high mass activity (9.29 A mg−1 at 100 mV), surpassing the performance of commercial Pt/C by a factor of 46. Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH− blockages, accelerating water dissociation and facilitating hydrogen adsorption/desorption, thus enhancing HER activity. This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5000,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.690","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Energy","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cey2.690","RegionNum":1,"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

Ruthenium (Ru)-based electrocatalysts show great promise as substitutes for platinum (Pt) for the alkaline hydrogen evolution reaction (HER) because of their efficient water dissociation capabilities. Nevertheless, the strong adsorption of Ru–OH intermediates (Ru-OH_ad) blocks the active site, leading to unsatisfactory HER performance. In this study, we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP–CoP heterostructure-anchored Ru single-atom site catalyst (Ru-FeP-CoP/NPC). The obtained catalyst shows a low overpotential (28 mV at 10 mA cm⁻²) and a high mass activity (9.29 A mg⁻¹ at 100 mV), surpassing the performance of commercial Pt/C by a factor of 46. Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH⁻ blockages, accelerating water dissociation and facilitating hydrogen adsorption/desorption, thus enhancing HER activity. This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.

查看原文本刊更多论文

调节单原子Ru位的局部电荷分布以实现高效析氢反应

钌基电催化剂由于其高效的水解离能力，在碱性析氢反应（HER）中作为铂（Pt）的替代品具有很大的前景。然而，Ru-OH中间体的强吸附（Ru-OHad）阻断了活性位点，导致HER性能不理想。在这项研究中，我们报道了一种通用的配体交换策略，用于合成mof -on- mof衍生的FeP-CoP异质结构锚定的Ru单原子位点催化剂（Ru-FeP-CoP/NPC）。所制得的催化剂具有低过电位（10 mA cm−2时为28 mV）和高质量活性（100 mV时为9.29 a mg−1），比商用Pt/C性能高出46倍。理论研究表明，调节Ru单原子位的局部电荷分布可以缓解周围OH−的堵塞，加速水的解离，促进氢的吸附/解吸，从而提高HER活性。这项工作旨在启发进一步设计具有定制电子特性的高活性和耐用的电催化剂，用于高纯度的氢气生产。

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分钟内获得全文求助全文

来源期刊

Carbon Energy Multiple-

CiteScore

25.70

自引率

10.70%

发文量

116

审稿时长

4 weeks

期刊介绍： Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.