Trace Rh Activates Surface Ni with Increased Local Charge for Efficient pH-Universal Hydrogen Generation

IF 19.3 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2024-10-28 DOI:10.1021/acsenergylett.4c0265010.1021/acsenergylett.4c02650

Minmin Cai, Qian Zhu, Xiangyan Hou, Lu Yao, Yuan Zhang, Xiaofeng Wu, Xiangdong Yao*, Hao Chen, Yi Jia*, Shouhua Feng and Keke Huang*,

{"title":"Trace Rh Activates Surface Ni with Increased Local Charge for Efficient pH-Universal Hydrogen Generation","authors":"Minmin Cai, Qian Zhu, Xiangyan Hou, Lu Yao, Yuan Zhang, Xiaofeng Wu, Xiangdong Yao*, Hao Chen, Yi Jia*, Shouhua Feng and Keke Huang*, ","doi":"10.1021/acsenergylett.4c0265010.1021/acsenergylett.4c02650","DOIUrl":null,"url":null,"abstract":"The unbefitting binding energy for H*/OH* with Ni sites greatly restrains the electrochemical activity of Ni for the hydrogen evolution reaction (HER). Herein, Ni nanograins incorporated with trace Rh (denoted as 3D RhNi) are synthesized through combining a facile ion-absorption and subsequent thermal reduction treatment, in which Rh increases the local charge density of Ni sites, dramatically accelerating the electrochemical kinetics of HER. Experimentally, the Rh–Ni catalyst with only 0.1 at. % Rh element exhibits superior HER activity among the reported Ni-based materials, whose overpotential is only 37 mV and 18 mV at 10 mA/cm2 in 1.0 M KOH and 0.5 M H2SO4, respectively. DFT calculations further identify that the resultant catalyst possesses appropriate intermediate binding energy in both acidic and alkaline conditions toward HER. This study provides a strategy to manipulate the local electronic structure for significantly improving the activity in surface catalysis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 11","pages":"5587–5595 5587–5595"},"PeriodicalIF":19.3000,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Energy Letters ","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsenergylett.4c02650","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

The unbefitting binding energy for H*/OH* with Ni sites greatly restrains the electrochemical activity of Ni for the hydrogen evolution reaction (HER). Herein, Ni nanograins incorporated with trace Rh (denoted as 3D RhNi) are synthesized through combining a facile ion-absorption and subsequent thermal reduction treatment, in which Rh increases the local charge density of Ni sites, dramatically accelerating the electrochemical kinetics of HER. Experimentally, the Rh–Ni catalyst with only 0.1 at. % Rh element exhibits superior HER activity among the reported Ni-based materials, whose overpotential is only 37 mV and 18 mV at 10 mA/cm² in 1.0 M KOH and 0.5 M H₂SO₄, respectively. DFT calculations further identify that the resultant catalyst possesses appropriate intermediate binding energy in both acidic and alkaline conditions toward HER. This study provides a strategy to manipulate the local electronic structure for significantly improving the activity in surface catalysis.

Abstract Image

查看原文本刊更多论文

痕量 Rh 激活表面镍，增加局部电荷，实现高效的 pH 值万能制氢

H*/OH* 与镍位点的结合能不合适，极大地限制了镍在氢进化反应（HER）中的电化学活性。本文通过简便的离子吸附和后续的热还原处理合成了掺有微量 Rh 的纳米镍晶粒（称为三维 RhNi），Rh 增加了镍位点的局部电荷密度，显著加快了氢进化反应的电化学动力学过程。实验结果表明，Rh 元素含量仅为 0.1 at.%的 Rh-Ni 催化剂在 1.0 M KOH 和 0.5 M H2SO4 溶液中 10 mA/cm2 的过电位分别仅为 37 mV 和 18 mV，在已报道的 Ni 基材料中表现出更高的 HER 活性。DFT 计算进一步确定，由此产生的催化剂在酸性和碱性条件下对 HER 都具有适当的中间结合能。这项研究为操纵局部电子结构以显著提高表面催化活性提供了一种策略。

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

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.