Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

IF 13.1 1区 化学 Q1 Energy Journal of Energy Chemistry Pub Date : 2024-09-25 DOI:10.1016/j.jechem.2024.09.027
{"title":"Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries","authors":"","doi":"10.1016/j.jechem.2024.09.027","DOIUrl":null,"url":null,"abstract":"<div><div>Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost, yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics. Herein, we supply a strategy to optimize the electron structure of Ni<sub>2</sub>P by concurrently introducing B-doped atoms and P vacancies in Ni<sub>2</sub>P (V<sub>p</sub>-B-Ni<sub>2</sub>P), thereby enhancing the bidirectional sulfur conversion. The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni<sub>2</sub>P causes the redistribution of electron around Ni atoms, bringing about the upward shift of <em>d</em>-band center of Ni atoms and effective <em>d</em>-<em>p</em> orbital hybridization between Ni atoms and sulfur species, thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species. Meanwhile, theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni<sub>2</sub>P selectively promotes Li<sub>2</sub>S dissolution and nucleation processes. Thus, the Li-S batteries with V<sub>p</sub>-B-Ni<sub>2</sub>P-separators present outstanding rate ability of 777 mA h g<sup>−1</sup> at 5 C and high areal capacity of 8.03 mA h cm<sup>−2</sup> under E/S of 5 μL mg<sup>−1</sup> and sulfur loading of 7.20 mg cm<sup>−2</sup>. This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":null,"pages":null},"PeriodicalIF":13.1000,"publicationDate":"2024-09-25","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/S2095495624006508","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

Abstract

Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost, yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics. Herein, we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P (Vp-B-Ni2P), thereby enhancing the bidirectional sulfur conversion. The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms, bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species, thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species. Meanwhile, theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation processes. Thus, the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 mA h g−1 at 5 C and high areal capacity of 8.03 mA h cm−2 under E/S of 5 μL mg−1 and sulfur loading of 7.20 mg cm−2. This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.

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
通过在锂硫电池的 Ni2P 中引入掺硼原子和磷空位,促进硫的双向转化
锂硫(Li-S)电池因其理论能量密度高、成本低而备受关注,但其进一步商业化却因臭名昭著的穿梭效应和缓慢的氧化还原动力学而受阻。在此,我们提供了一种优化 Ni2P 电子结构的策略,即在 Ni2P 中同时引入掺 B 原子和 P 空位(Vp-B-Ni2P),从而增强硫的双向转化。研究表明,在 Ni2P 中同时引入掺杂 B 原子和 P 空位会导致镍原子周围电子的重新分布,使镍原子的 d 带中心上移,镍原子与硫元素之间产生有效的 d-p 轨道杂化,从而加强了多硫化锂(LiPSs)的化学锚定,并加快了硫元素的双向转化动力学。同时,理论计算显示,Ni2P 中掺杂的 B 原子和 P 空位选择性地促进了 Li2S 的溶解和成核过程。因此,在 5 μL mg-1 的 E/S 和 7.20 mg cm-2 的硫载荷条件下,使用 Vp-B-Ni2P 隔离剂的锂-S 电池在 5 C 时具有 777 mA h g-1 的出色速率能力和 8.03 mA h cm-2 的高平均容量。这项工作阐明了在金属磷化物中引入杂原子和空位可协同调节电子结构,从而加速双向硫转化。
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
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 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 Upcycling of monomers derived from waste polyester plastics via electrocatalysis Design principles of novel Zn fluorocarboxylate protection layer toward durable dendrite-free Zn metal anodes
×
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