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
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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。

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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.

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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.
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