铂修饰金属钴缺陷位点以实现 5-羟甲基糠醛的高效电催化氧化

IF 13.1 1区 化学 Q1 Energy Journal of Energy Chemistry Pub Date : 2024-10-17 DOI:10.1016/j.jechem.2024.09.054
Haoyu Zhan , Baixue Cheng , Yankun Lu , Danning Xing , Xingshuai Lv , Huining Huang , Thomas Frauenheim , Tao Wang , Peng Zhou
{"title":"铂修饰金属钴缺陷位点以实现 5-羟甲基糠醛的高效电催化氧化","authors":"Haoyu Zhan ,&nbsp;Baixue Cheng ,&nbsp;Yankun Lu ,&nbsp;Danning Xing ,&nbsp;Xingshuai Lv ,&nbsp;Huining Huang ,&nbsp;Thomas Frauenheim ,&nbsp;Tao Wang ,&nbsp;Peng Zhou","doi":"10.1016/j.jechem.2024.09.054","DOIUrl":null,"url":null,"abstract":"<div><div>Co<sub>3</sub>O<sub>4</sub> possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural (HMF). However, the enrichment and activation effects of Co<sub>3</sub>O<sub>4</sub> on OH<sup>−</sup> and HMF are weak, which limits its further application. Metal defect engineering can regulate the electronic structure, optimize the adsorption of intermediates, and improve the catalytic activity by breaking the symmetry of the material, which is rarely involved in the upgrading of biomass. In this work, we prepare Co<sub>3</sub>O<sub>4</sub> with metal defects and load the precious metal platinum at the defect sites (Pt-Vco). The results of in-situ characterizations, electrochemical measurements, and theoretical calculations indicate that the reduction of Co–Co coordination number and the formation of Pt–Co bond induce the decrease of electron filling in the antibonding orbitals of Co element. The resulting upward shift of the <em>d</em>-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH<sup>−</sup> species, thus exhibiting excellent HMF oxidation activity (including a lower onset potential (1.14 V) and 19 times higher current density than pure Co<sub>3</sub>O<sub>4</sub> at 1.35 V). In summary, this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail, provides a new option for improving the HMF oxidation activity of cobalt-based materials, broadens the application field of metal defect based materials, and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":null,"pages":null},"PeriodicalIF":13.1000,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Platinum modification of metallic cobalt defect sites for efficient electrocatalytic oxidation of 5-hydroxymethylfurfural\",\"authors\":\"Haoyu Zhan ,&nbsp;Baixue Cheng ,&nbsp;Yankun Lu ,&nbsp;Danning Xing ,&nbsp;Xingshuai Lv ,&nbsp;Huining Huang ,&nbsp;Thomas Frauenheim ,&nbsp;Tao Wang ,&nbsp;Peng Zhou\",\"doi\":\"10.1016/j.jechem.2024.09.054\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Co<sub>3</sub>O<sub>4</sub> possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural (HMF). However, the enrichment and activation effects of Co<sub>3</sub>O<sub>4</sub> on OH<sup>−</sup> and HMF are weak, which limits its further application. Metal defect engineering can regulate the electronic structure, optimize the adsorption of intermediates, and improve the catalytic activity by breaking the symmetry of the material, which is rarely involved in the upgrading of biomass. In this work, we prepare Co<sub>3</sub>O<sub>4</sub> with metal defects and load the precious metal platinum at the defect sites (Pt-Vco). The results of in-situ characterizations, electrochemical measurements, and theoretical calculations indicate that the reduction of Co–Co coordination number and the formation of Pt–Co bond induce the decrease of electron filling in the antibonding orbitals of Co element. The resulting upward shift of the <em>d</em>-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH<sup>−</sup> species, thus exhibiting excellent HMF oxidation activity (including a lower onset potential (1.14 V) and 19 times higher current density than pure Co<sub>3</sub>O<sub>4</sub> at 1.35 V). In summary, this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail, provides a new option for improving the HMF oxidation activity of cobalt-based materials, broadens the application field of metal defect based materials, and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.</div></div>\",\"PeriodicalId\":15728,\"journal\":{\"name\":\"Journal of Energy Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2024-10-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Energy Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S209549562400679X\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Energy Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S209549562400679X","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Energy","Score":null,"Total":0}
引用次数: 0

摘要

Co3O4 具有直接和间接氧化作用,被认为是一种很有前景的 5-hydroxymethylfurfural (HMF) 氧化催化剂。然而,Co3O4 对 OH- 和 HMF 的富集和活化效应较弱,限制了其进一步应用。金属缺陷工程可以调节电子结构,优化中间产物的吸附,并通过打破材料的对称性来提高催化活性,而这在生物质升级中很少涉及。在这项工作中,我们制备了具有金属缺陷的 Co3O4,并在缺陷位点上负载贵金属铂(Pt-Vco)。原位表征、电化学测量和理论计算的结果表明,Co-Co 配位数的减少和 Pt-Co 键的形成导致 Co 元素反键轨道中电子填充的减少。由此产生的 Co 的 d 带中心上移与 Pt 物种的吸附特性协同增强了有机分子和 OH- 物种的富集和活化,从而表现出优异的 HMF 氧化活性(包括较低的起始电位(1.14 V)和比纯 Co3O4 高 19 倍的电流密度(1.35 V))。综上所述,该研究详细探讨了贵金属修饰金属缺陷位点的吸附增强机理,为提高钴基材料的 HMF 氧化活性提供了新的选择,拓宽了金属缺陷基材料的应用领域,为金属缺陷位点在生物质转化中的功能化利用提供了创新性指导。
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
Platinum modification of metallic cobalt defect sites for efficient electrocatalytic oxidation of 5-hydroxymethylfurfural
Co3O4 possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural (HMF). However, the enrichment and activation effects of Co3O4 on OH and HMF are weak, which limits its further application. Metal defect engineering can regulate the electronic structure, optimize the adsorption of intermediates, and improve the catalytic activity by breaking the symmetry of the material, which is rarely involved in the upgrading of biomass. In this work, we prepare Co3O4 with metal defects and load the precious metal platinum at the defect sites (Pt-Vco). The results of in-situ characterizations, electrochemical measurements, and theoretical calculations indicate that the reduction of Co–Co coordination number and the formation of Pt–Co bond induce the decrease of electron filling in the antibonding orbitals of Co element. The resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species, thus exhibiting excellent HMF oxidation activity (including a lower onset potential (1.14 V) and 19 times higher current density than pure Co3O4 at 1.35 V). In summary, this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail, provides a new option for improving the HMF oxidation activity of cobalt-based materials, broadens the application field of metal defect based materials, and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.
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
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
期刊最新文献
Unraveling the exceptional kinetics of Zn||organic batteries in hydrated deep eutectic solution Improving structure stability of single-crystalline Ni-rich cathode at high voltage by element gradient doping and interfacial modification Electronic modulation towards MOFs as template derived CoP via engineered heteroatom defect for a highly efficient overall water splitting Enhanced dynamics of Al3+/H+ ions in aqueous aluminum ion batteries: Construction of metastable structures in vanadium pentoxide upon oxygen vacancies A binary eutectic electrolyte design for high-temperature interface-compatible Zn-ion batteries
×
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