对用于高效氧进化反应的 Co3O4 催化剂表面和缺陷调控的 DFT 研究

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL
Chenxu Huo , Xiufeng Lang , Guoxiong Song , Yujie Wang , Shihong Ren , Weidan Liao , Hao Guo , Xueguang Chen
{"title":"对用于高效氧进化反应的 Co3O4 催化剂表面和缺陷调控的 DFT 研究","authors":"Chenxu Huo ,&nbsp;Xiufeng Lang ,&nbsp;Guoxiong Song ,&nbsp;Yujie Wang ,&nbsp;Shihong Ren ,&nbsp;Weidan Liao ,&nbsp;Hao Guo ,&nbsp;Xueguang Chen","doi":"10.1016/j.susc.2024.122544","DOIUrl":null,"url":null,"abstract":"<div><p>The electrolysis of a water for hydrogen production is a promising way to produce clean energy, but the sluggish oxygen evolution reaction (OER) limits the overall efficiency of water electrolysis. In this work, we investigated the water oxidation pathways on the perfect and defect Co<sub>3</sub>O<sub>4</sub>(111) surfaces by using density functional theory (DFT) calculations. We found that for the perfect surface the free energy barrier of the potential determining step (PDS) in the adsorbate evolution mechanism (AEM) of water is lower than that in the lattice oxygen mechanism (LOM). For the defect surfaces, cobalt vacancies are more easily formed than oxygen vacancies. The Co vacancy promotes the formation of *OH, changes the PDS of the LOM and AEM, and reduces the free energy barrier of both PDS. The PDS of the LOM pathway on the V<sub>Co2</sub><sub><img></sub>Co<sub>3</sub>O<sub>4</sub>(111) surface is the coupling step of the O adatom and lattice oxygen, which promotes the LOM process. Different from the OER mechanism on the perfect surface and the defect surface with Co vacancy, the LOM is perferred to occur on the defect surface with O vacancy. This work may provide new insight into the relationship between the surface structure and OER activity surface of the Co<sub>3</sub>O<sub>4</sub> catalyst and help to design the efficient OER catalysts by surface and vacancy engineering.</p></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":null,"pages":null},"PeriodicalIF":2.1000,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A DFT investigation on surface and defect modulation of the Co3O4 catalyst for efficient oxygen evolution reaction\",\"authors\":\"Chenxu Huo ,&nbsp;Xiufeng Lang ,&nbsp;Guoxiong Song ,&nbsp;Yujie Wang ,&nbsp;Shihong Ren ,&nbsp;Weidan Liao ,&nbsp;Hao Guo ,&nbsp;Xueguang Chen\",\"doi\":\"10.1016/j.susc.2024.122544\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The electrolysis of a water for hydrogen production is a promising way to produce clean energy, but the sluggish oxygen evolution reaction (OER) limits the overall efficiency of water electrolysis. In this work, we investigated the water oxidation pathways on the perfect and defect Co<sub>3</sub>O<sub>4</sub>(111) surfaces by using density functional theory (DFT) calculations. We found that for the perfect surface the free energy barrier of the potential determining step (PDS) in the adsorbate evolution mechanism (AEM) of water is lower than that in the lattice oxygen mechanism (LOM). For the defect surfaces, cobalt vacancies are more easily formed than oxygen vacancies. The Co vacancy promotes the formation of *OH, changes the PDS of the LOM and AEM, and reduces the free energy barrier of both PDS. The PDS of the LOM pathway on the V<sub>Co2</sub><sub><img></sub>Co<sub>3</sub>O<sub>4</sub>(111) surface is the coupling step of the O adatom and lattice oxygen, which promotes the LOM process. Different from the OER mechanism on the perfect surface and the defect surface with Co vacancy, the LOM is perferred to occur on the defect surface with O vacancy. This work may provide new insight into the relationship between the surface structure and OER activity surface of the Co<sub>3</sub>O<sub>4</sub> catalyst and help to design the efficient OER catalysts by surface and vacancy engineering.</p></div>\",\"PeriodicalId\":22100,\"journal\":{\"name\":\"Surface Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.1000,\"publicationDate\":\"2024-07-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Surface Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0039602824000955\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Surface Science","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0039602824000955","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

电解水制氢是一种前景广阔的清洁能源生产方式,但缓慢的氧进化反应(OER)限制了水电解的整体效率。在这项工作中,我们利用密度泛函理论(DFT)计算研究了完美和缺陷 Co3O4(111)表面的水氧化途径。我们发现,对于完美表面,水的吸附剂演化机制(AEM)中潜在决定步骤(PDS)的自由能垒低于晶格氧机制(LOM)。对于缺陷表面,钴空位比氧空位更容易形成。钴空位促进了*OH的形成,改变了LOM和AEM的PDS,降低了两种PDS的自由能垒。VCo2Co3O4(111) 表面上 LOM 途径的 PDS 是 O adatom 与晶格氧的耦合步骤,它促进了 LOM 过程。与完美表面和有 Co 空位的缺陷表面上的 OER 机制不同,LOM 更倾向于发生在有 O 空位的缺陷表面上。这项工作可能会对 Co3O4 催化剂表面结构与 OER 活性表面之间的关系提供新的见解,并有助于通过表面和空位工程设计高效的 OER 催化剂。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

A DFT investigation on surface and defect modulation of the Co3O4 catalyst for efficient oxygen evolution reaction

A DFT investigation on surface and defect modulation of the Co3O4 catalyst for efficient oxygen evolution reaction

The electrolysis of a water for hydrogen production is a promising way to produce clean energy, but the sluggish oxygen evolution reaction (OER) limits the overall efficiency of water electrolysis. In this work, we investigated the water oxidation pathways on the perfect and defect Co3O4(111) surfaces by using density functional theory (DFT) calculations. We found that for the perfect surface the free energy barrier of the potential determining step (PDS) in the adsorbate evolution mechanism (AEM) of water is lower than that in the lattice oxygen mechanism (LOM). For the defect surfaces, cobalt vacancies are more easily formed than oxygen vacancies. The Co vacancy promotes the formation of *OH, changes the PDS of the LOM and AEM, and reduces the free energy barrier of both PDS. The PDS of the LOM pathway on the VCo2Co3O4(111) surface is the coupling step of the O adatom and lattice oxygen, which promotes the LOM process. Different from the OER mechanism on the perfect surface and the defect surface with Co vacancy, the LOM is perferred to occur on the defect surface with O vacancy. This work may provide new insight into the relationship between the surface structure and OER activity surface of the Co3O4 catalyst and help to design the efficient OER catalysts by surface and vacancy engineering.

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
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
×
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
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
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 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信