洞察气体分子吸附在二维-FeS2 上的影响:DFT 研究

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-05-13 DOI:10.1016/j.susc.2024.122509
Fen-Ning Zhao , Fu-Ling Tang , Hong-Tao Xue , Cheng-Dong Wei
{"title":"洞察气体分子吸附在二维-FeS2 上的影响:DFT 研究","authors":"Fen-Ning Zhao ,&nbsp;Fu-Ling Tang ,&nbsp;Hong-Tao Xue ,&nbsp;Cheng-Dong Wei","doi":"10.1016/j.susc.2024.122509","DOIUrl":null,"url":null,"abstract":"<div><p>Lithium-sulfur (Li-S) batteries are especially competitive in the energy sector due to their excellent performances, like preferable energy density and economic benefits. Studying the adsorption of gas molecules on electrode materials has potential engineering significance for Li-S batteries since they have a highly osmotic potential, which causes unavoidable damage to batteries. In this work, the adsorption phenomenon of common gas molecules (H<sub>2</sub>O, N<sub>2</sub>, H<sub>2</sub>, CO<sub>2</sub>, and O<sub>2</sub>) on the two-dimensional pyrite (2D-FeS<sub>2</sub>) cathode material surface, as well as the effects on the electronic and electrochemical properties, were investigated by the first-principles calculations. The adsorption capabilities were estimated by adsorption energy and Mulliken population analysis. Simulation results demonstrated that whole adsorption energies were less than -1.0 eV and larger than -0.6 eV, which shows a physisorption nature. Among them, the O-S bond of O<sub>2</sub>/2D-FeS<sub>2</sub> has the strongest strength. Electronic structure calculations suggested that 2D-FeS<sub>2</sub> maintained good conductivity after gas molecules were adsorbed, achieving efficient transfer between electron, lithium, and sulfur intermediates. Additionally, <em>ab initio</em> molecular dynamics (AIMD) simulations showed that Li<sup>+</sup> exhibits excellent diffusion performance and low activation energy at different temperatures. 2D-FeS<sub>2</sub> still has a stable electrochemical working window (1.87 ∼ 2.47 V), while the theoretical open current voltage is damaged by gas molecule adsorption. Consequently, this work theoretically reveals the effect of gas molecules on the cathode materials for Li-S batteries, which has guide meaning for engineering.</p></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"747 ","pages":"Article 122509"},"PeriodicalIF":2.1000,"publicationDate":"2024-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Insight into the effects of gas molecules-adsorbed on 2D-FeS2: A DFT study\",\"authors\":\"Fen-Ning Zhao ,&nbsp;Fu-Ling Tang ,&nbsp;Hong-Tao Xue ,&nbsp;Cheng-Dong Wei\",\"doi\":\"10.1016/j.susc.2024.122509\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Lithium-sulfur (Li-S) batteries are especially competitive in the energy sector due to their excellent performances, like preferable energy density and economic benefits. Studying the adsorption of gas molecules on electrode materials has potential engineering significance for Li-S batteries since they have a highly osmotic potential, which causes unavoidable damage to batteries. In this work, the adsorption phenomenon of common gas molecules (H<sub>2</sub>O, N<sub>2</sub>, H<sub>2</sub>, CO<sub>2</sub>, and O<sub>2</sub>) on the two-dimensional pyrite (2D-FeS<sub>2</sub>) cathode material surface, as well as the effects on the electronic and electrochemical properties, were investigated by the first-principles calculations. The adsorption capabilities were estimated by adsorption energy and Mulliken population analysis. Simulation results demonstrated that whole adsorption energies were less than -1.0 eV and larger than -0.6 eV, which shows a physisorption nature. Among them, the O-S bond of O<sub>2</sub>/2D-FeS<sub>2</sub> has the strongest strength. Electronic structure calculations suggested that 2D-FeS<sub>2</sub> maintained good conductivity after gas molecules were adsorbed, achieving efficient transfer between electron, lithium, and sulfur intermediates. Additionally, <em>ab initio</em> molecular dynamics (AIMD) simulations showed that Li<sup>+</sup> exhibits excellent diffusion performance and low activation energy at different temperatures. 2D-FeS<sub>2</sub> still has a stable electrochemical working window (1.87 ∼ 2.47 V), while the theoretical open current voltage is damaged by gas molecule adsorption. Consequently, this work theoretically reveals the effect of gas molecules on the cathode materials for Li-S batteries, which has guide meaning for engineering.</p></div>\",\"PeriodicalId\":22100,\"journal\":{\"name\":\"Surface Science\",\"volume\":\"747 \",\"pages\":\"Article 122509\"},\"PeriodicalIF\":2.1000,\"publicationDate\":\"2024-05-13\",\"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/S0039602824000608\",\"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/S0039602824000608","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

锂硫(Li-S)电池因其卓越的性能,如更高的能量密度和经济效益,在能源领域尤其具有竞争力。研究气体分子在电极材料上的吸附现象对锂硫电池具有潜在的工程意义,因为气体分子具有高渗透电位,会对电池造成不可避免的损坏。本研究通过第一性原理计算研究了常见气体分子(HO、N、H、CO 和 O)在二维黄铁矿(2D-FeS)阴极材料表面的吸附现象及其对电子和电化学性能的影响。通过吸附能和 Mulliken 种群分析估算了吸附能力。模拟结果表明,整个吸附能小于-1.0 eV,大于-0.6 eV,显示出物理吸附性质。其中,O/2D-FeS 的 O-S 键强度最强。电子结构计算表明,二维-FeS 在吸附气体分子后仍能保持良好的导电性,实现了电子、锂和硫中间体之间的高效转移。此外,分子动力学(AIMD)模拟显示,锂在不同温度下均表现出优异的扩散性能和较低的活化能。二维-FeS 仍具有稳定的电化学工作窗口(1.87 ∼ 2.47 V),而理论开路电流电压则因气体分子吸附而受到破坏。因此,这项工作从理论上揭示了气体分子对锂离子电池阴极材料的影响,对工程学具有指导意义。
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

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
Insight into the effects of gas molecules-adsorbed on 2D-FeS2: A DFT study

Lithium-sulfur (Li-S) batteries are especially competitive in the energy sector due to their excellent performances, like preferable energy density and economic benefits. Studying the adsorption of gas molecules on electrode materials has potential engineering significance for Li-S batteries since they have a highly osmotic potential, which causes unavoidable damage to batteries. In this work, the adsorption phenomenon of common gas molecules (H2O, N2, H2, CO2, and O2) on the two-dimensional pyrite (2D-FeS2) cathode material surface, as well as the effects on the electronic and electrochemical properties, were investigated by the first-principles calculations. The adsorption capabilities were estimated by adsorption energy and Mulliken population analysis. Simulation results demonstrated that whole adsorption energies were less than -1.0 eV and larger than -0.6 eV, which shows a physisorption nature. Among them, the O-S bond of O2/2D-FeS2 has the strongest strength. Electronic structure calculations suggested that 2D-FeS2 maintained good conductivity after gas molecules were adsorbed, achieving efficient transfer between electron, lithium, and sulfur intermediates. Additionally, ab initio molecular dynamics (AIMD) simulations showed that Li+ exhibits excellent diffusion performance and low activation energy at different temperatures. 2D-FeS2 still has a stable electrochemical working window (1.87 ∼ 2.47 V), while the theoretical open current voltage is damaged by gas molecule adsorption. Consequently, this work theoretically reveals the effect of gas molecules on the cathode materials for Li-S batteries, which has guide meaning for 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.
期刊最新文献
VS2/graphene heterostructures as cathode materials for sodium-sulfur batteries: A first-principles study Effect of alloying elements (Ti, Zn, Zr, Al) on the interfacial properties of Cu/Ni2Si: A DFT study Editorial Board Adsorbate-induced effects on the H− ion collisions with Na/Ag(111) and K/Ag(111) surfaces One century of evolution of surface science, a personal perspective
×
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