Enhancing Alkaline Hydrogen Evolution Reaction on Ru-Decorated TiO2 Nanotube Layers: Synergistic Role of Ti3+, Ru Single Atoms, and Ru Nanoparticles

IF 13 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Energy & Environmental Materials Pub Date : 2025-01-08 DOI:10.1002/eem2.12864

Sitaramanjaneya Mouli Thalluri, Jhonatan Rodriguez-Pereira, Jan Michalicka, Eva Kolíbalová, Ludek Hromadko, Stanislav Slang, Miloslav Pouzar, Hanna Sopha, Raul Zazpe, Jan M. Macak

{"title":"Enhancing Alkaline Hydrogen Evolution Reaction on Ru-Decorated TiO2 Nanotube Layers: Synergistic Role of Ti3+, Ru Single Atoms, and Ru Nanoparticles","authors":"Sitaramanjaneya Mouli Thalluri, Jhonatan Rodriguez-Pereira, Jan Michalicka, Eva Kolíbalová, Ludek Hromadko, Stanislav Slang, Miloslav Pouzar, Hanna Sopha, Raul Zazpe, Jan M. Macak","doi":"10.1002/eem2.12864","DOIUrl":null,"url":null,"abstract":"Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers (TNT) and ruthenium (Ru) species comprising of both single atoms (SAs) and nanoparticles (NPs) augment the alkaline hydrogen evolution reaction (HER) by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H* desorption. Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8 ± 0.4 nm NPs present on TNT layers, and it emerges with the highest HER activity among all the electrodes synthesized. A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti3+ states and the coexistence of Ru SAs and NPs. With insights from literature, the role of Ti3+, appropriate work functions of TNT layers and Ru, and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified. The aforementioned characteristics led to a remarkable performance by having 9 mV onset potentials and 33 mV dec−1 of Tafel slopes and a higher turnover frequency of 1.72 H2 s−1 at 30 mV. Besides, a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0000,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12864","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Environmental Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/eem2.12864","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Synergistic interplays involving multiple active centers originating from TiO₂ nanotube layers (TNT) and ruthenium (Ru) species comprising of both single atoms (SAs) and nanoparticles (NPs) augment the alkaline hydrogen evolution reaction (HER) by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H* desorption. Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8 ± 0.4 nm NPs present on TNT layers, and it emerges with the highest HER activity among all the electrodes synthesized. A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti³⁺ states and the coexistence of Ru SAs and NPs. With insights from literature, the role of Ti³⁺, appropriate work functions of TNT layers and Ru, and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified. The aforementioned characteristics led to a remarkable performance by having 9 mV onset potentials and 33 mV dec⁻¹ of Tafel slopes and a higher turnover frequency of 1.72 H₂ s⁻¹ at 30 mV. Besides, a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.

Abstract Image

查看原文本刊更多论文

增强Ru修饰TiO2纳米管层上碱性析氢反应：Ti3+、Ru单原子和Ru纳米颗粒的协同作用

来自TiO2纳米管层（TNT）的多个活性中心和由单原子（SAs）和纳米粒子（NPs）组成的钌（Ru）物种的协同相互作用通过增强快速水解离产生的Volmer动力学和有效H*解吸产生的Tafel动力学来增强碱性析氢反应（HER）。经过50个工艺循环的Ru原子层沉积，在TNT层上形成了Ru SAs和2.8±0.4 nm NPs的混合物，其she活性在所有合成的电极中最高。利用不同的高分辨率技术对Ti和Ru进行了详细的研究，证实了Ti3+态的存在以及Ru sa和NPs的共存。结合文献，阐述并论证了Ti3+的作用、TNT层与Ru的适当做功功能以及Ru SAs和Ru NPs在提高碱性HER性能中的协同作用。上述特性使其具有9 mV的起始电位和33 mV的Tafel斜率，以及在30 mV时1.72 H2 s−1的较高周转频率。此外，通过28小时楼梯计时电位测量，TNT@Ru的稳定性明显优于TNT@Pt。

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

Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

17.60

自引率

6.00%

发文量

期刊介绍： Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.