Local electronic structure constructing of layer-structured oxide cathode material for high-voltage sodium-ion batteries

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-05-17 DOI:10.1002/cey2.574
Dongrun Yang, Xuan-Wen Gao, Guoping Gao, Qingsong Lai, Tianzhen Ren, Qinfen Gu, Zhaomeng Liu, Wen-Bin Luo
{"title":"Local electronic structure constructing of layer-structured oxide cathode material for high-voltage sodium-ion batteries","authors":"Dongrun Yang,&nbsp;Xuan-Wen Gao,&nbsp;Guoping Gao,&nbsp;Qingsong Lai,&nbsp;Tianzhen Ren,&nbsp;Qinfen Gu,&nbsp;Zhaomeng Liu,&nbsp;Wen-Bin Luo","doi":"10.1002/cey2.574","DOIUrl":null,"url":null,"abstract":"<p>As the cyclable sodium ions' primary suppliers, O3-type layer-structured manganese-based oxides are recognized as one of the most competitive cathode candidates for sodium-ion batteries. Suffering from complex structural transformations and transition metal migration during the sodium intercalation/deintercalation process, particularly at high voltage, the energy density and lifespan cannot satisfy the increasing demand. The orbital and electronic structure of the octahedral center metal element plays an important role in maintaining the octahedral structural integrity and improving the Na<sup>+</sup> diffusivity by the introduced heterogeneous [Me–O] (Me: transition metals) chemical bonding. Herein, inspired by the 4f and 5d orbital bonding possibility from the abundant configuration of extranuclear electrons and large ion radius, O3-type Na[La<sub>0.01</sub>Ni<sub>0.3</sub>Mn<sub>0.54</sub>Cu<sub>0.1</sub>Ti<sub>0.05</sub>]O<sub>2</sub> was synthesized with a nearly single crystal structure. Based on the experimental and computational results, the introduced heterogeneous [La–O] chemical bond with larger bond strength can not only ensure the stability of the lattice oxygen framework and the reversibility of oxygen redox but also optimize the oxygen local electronic structure resulting from La 5d and O 2p orbital mixing due to O 2p → La 5d charge transfer. It delivers an optimal electrochemical performance with a high energy density and cycling lifespan.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"6 10","pages":""},"PeriodicalIF":19.5000,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.574","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Energy","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cey2.574","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

As the cyclable sodium ions' primary suppliers, O3-type layer-structured manganese-based oxides are recognized as one of the most competitive cathode candidates for sodium-ion batteries. Suffering from complex structural transformations and transition metal migration during the sodium intercalation/deintercalation process, particularly at high voltage, the energy density and lifespan cannot satisfy the increasing demand. The orbital and electronic structure of the octahedral center metal element plays an important role in maintaining the octahedral structural integrity and improving the Na+ diffusivity by the introduced heterogeneous [Me–O] (Me: transition metals) chemical bonding. Herein, inspired by the 4f and 5d orbital bonding possibility from the abundant configuration of extranuclear electrons and large ion radius, O3-type Na[La0.01Ni0.3Mn0.54Cu0.1Ti0.05]O2 was synthesized with a nearly single crystal structure. Based on the experimental and computational results, the introduced heterogeneous [La–O] chemical bond with larger bond strength can not only ensure the stability of the lattice oxygen framework and the reversibility of oxygen redox but also optimize the oxygen local electronic structure resulting from La 5d and O 2p orbital mixing due to O 2p → La 5d charge transfer. It delivers an optimal electrochemical performance with a high energy density and cycling lifespan.

Abstract Image

Abstract Image

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
构建用于高压钠离子电池的层状结构氧化物正极材料的局部电子结构
作为可循环钠离子的主要供应者,O3 型层结构锰基氧化物被认为是钠离子电池最具竞争力的阴极候选材料之一。由于在钠插层/脱插层过程中存在复杂的结构转变和过渡金属迁移,特别是在高电压下,其能量密度和寿命无法满足日益增长的需求。八面体中心金属元素的轨道和电子结构在维持八面体结构完整性和通过引入异质[Me-O](Me:过渡金属)化学键提高 Na+ 扩散性方面发挥着重要作用。本文受核外电子丰富构型和大离子半径带来的 4f 和 5d 轨道成键可能性的启发,合成了具有近似单晶结构的 O3 型 Na[La0.01Ni0.3Mn0.54Cu0.1Ti0.05]O2 。根据实验和计算结果,引入的键强度较大的异质[La-O]化学键不仅能保证晶格氧框架的稳定性和氧氧化还原的可逆性,还能优化由于 O 2p→La 5d 电荷转移导致的 La 5d 和 O 2p 轨道混合所产生的氧局部电子结构。它具有最佳的电化学性能、高能量密度和循环寿命。
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 去求助
来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
期刊最新文献
Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
×
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