带有 3d-5d 过渡金属核的银基核壳纳米团簇在氧还原反应中的第一性原理研究

IF 2.7 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Inorganica Chimica Acta Pub Date : 2024-08-09 DOI:10.1016/j.ica.2024.122301
{"title":"带有 3d-5d 过渡金属核的银基核壳纳米团簇在氧还原反应中的第一性原理研究","authors":"","doi":"10.1016/j.ica.2024.122301","DOIUrl":null,"url":null,"abstract":"<div><p>The depletion of traditional fossil fuels, as well as the increase in global energy demand, is currently driving the need for sustainable energy solutions. The primary challenge in the practical application of hydrogen fuel cells is to reduce or replace the use of platinum material in the electrode catalysts. In this work, by using density functional theory (DFT) we investigate the oxygen reduction reaction of Ag-based core-shell nanoclusters with 12 different 3d-5d transition metal (TM) cores (groups 8–11). The stability is assessed by calculating the binding, excess and segregation energies, indicating that the most stable mixing is found in the noble metal-encapsulated structures, such as Pd@Ag, Pt@Ag, Rh@Ag and Ir@Ag particles. The reaction barrier for OH formation is found to be the limiting step with values ranging from 0.59 to 1.36 eV among the core-shell Ag-based nanoclusters, which are comparable with the energy barrier of the Pt(111) surface (0.97 eV). However, the correlation of the d-band center and activation barriers indicate that Ru@Ag, Rh@Ag, and Os@Ag mixings are the most suitable for the oxygen reduction reaction. These results indicate that small Ag-based core-shell nanoclusters with transition metal cores are active for the ORR application in alkaline media.</p></div>","PeriodicalId":13599,"journal":{"name":"Inorganica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"First principles study for Ag-based core-shell nanoclusters with 3d-5d transition metal cores for the oxygen reduction reaction\",\"authors\":\"\",\"doi\":\"10.1016/j.ica.2024.122301\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The depletion of traditional fossil fuels, as well as the increase in global energy demand, is currently driving the need for sustainable energy solutions. The primary challenge in the practical application of hydrogen fuel cells is to reduce or replace the use of platinum material in the electrode catalysts. In this work, by using density functional theory (DFT) we investigate the oxygen reduction reaction of Ag-based core-shell nanoclusters with 12 different 3d-5d transition metal (TM) cores (groups 8–11). The stability is assessed by calculating the binding, excess and segregation energies, indicating that the most stable mixing is found in the noble metal-encapsulated structures, such as Pd@Ag, Pt@Ag, Rh@Ag and Ir@Ag particles. The reaction barrier for OH formation is found to be the limiting step with values ranging from 0.59 to 1.36 eV among the core-shell Ag-based nanoclusters, which are comparable with the energy barrier of the Pt(111) surface (0.97 eV). However, the correlation of the d-band center and activation barriers indicate that Ru@Ag, Rh@Ag, and Os@Ag mixings are the most suitable for the oxygen reduction reaction. These results indicate that small Ag-based core-shell nanoclusters with transition metal cores are active for the ORR application in alkaline media.</p></div>\",\"PeriodicalId\":13599,\"journal\":{\"name\":\"Inorganica Chimica Acta\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-08-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganica Chimica Acta\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S002016932400392X\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S002016932400392X","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0

摘要

传统化石燃料的枯竭以及全球能源需求的增长,促使人们需要可持续的能源解决方案。氢燃料电池实际应用的首要挑战是减少或取代电极催化剂中铂材料的使用。在这项工作中,我们利用密度泛函理论(DFT)研究了具有 12 种不同 3d-5d 过渡金属 (TM) 内核(第 8-11 组)的银基核壳纳米簇的氧还原反应。通过计算结合能、过剩能和偏析能评估了稳定性,结果表明贵金属封装结构的混合最为稳定,如 Pd@Ag、Pt@Ag、Rh@Ag 和 Ir@Ag 颗粒。在核壳银基纳米团簇中,形成 OH 的反应势垒是限制步骤,其值在 0.59 至 1.36 eV 之间,与 Pt(111) 表面的能垒(0.97 eV)相当。然而,d 带中心和活化能垒的相关性表明,Ru@Ag、Rh@Ag 和 Os@Ag 混合体最适合氧还原反应。这些结果表明,带有过渡金属核的小型银基核壳纳米团簇在碱性介质中的氧还原反应中具有活性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

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
First principles study for Ag-based core-shell nanoclusters with 3d-5d transition metal cores for the oxygen reduction reaction

The depletion of traditional fossil fuels, as well as the increase in global energy demand, is currently driving the need for sustainable energy solutions. The primary challenge in the practical application of hydrogen fuel cells is to reduce or replace the use of platinum material in the electrode catalysts. In this work, by using density functional theory (DFT) we investigate the oxygen reduction reaction of Ag-based core-shell nanoclusters with 12 different 3d-5d transition metal (TM) cores (groups 8–11). The stability is assessed by calculating the binding, excess and segregation energies, indicating that the most stable mixing is found in the noble metal-encapsulated structures, such as Pd@Ag, Pt@Ag, Rh@Ag and Ir@Ag particles. The reaction barrier for OH formation is found to be the limiting step with values ranging from 0.59 to 1.36 eV among the core-shell Ag-based nanoclusters, which are comparable with the energy barrier of the Pt(111) surface (0.97 eV). However, the correlation of the d-band center and activation barriers indicate that Ru@Ag, Rh@Ag, and Os@Ag mixings are the most suitable for the oxygen reduction reaction. These results indicate that small Ag-based core-shell nanoclusters with transition metal cores are active for the ORR application in alkaline media.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Inorganica Chimica Acta
Inorganica Chimica Acta 化学-无机化学与核化学
CiteScore
6.00
自引率
3.60%
发文量
440
审稿时长
35 days
期刊介绍: Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.
期刊最新文献
Optimizing synthesis and catalytic performance of novel β-keto-enamine complexes of Ni (II) using BBD design and PSO-ANN Zn(II)-based mechanically flexible metallosupramolecular network: Investigating rheology, morphology, anti-bacterial effect and semiconducting device performances A multifunctional metal–organic complex fluorescent probe for highly sensitive detection of lysine, CrO42-/Cr2O72-, Fe3+ and nitro-aromatic compounds Activation of persulfate by MOF-derived MnFeOx to efficiently degrade sulfadiazine: Synergistic effects from free radicals and singlet oxygen Synthesis and characterization of 3,5-bis((2-hydroxybenzylidene)amino)-N-(2-hydroxyphenyl)benzamide and Zn(II) complex: Investigation of chromic, fluorescence and DPPH radical scavenging behaviours
×
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