Self-building sodium modified g-C3N4/CN for fast kinetics in sodium‑sulfur batteries by first-principles calculations.

IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL
Journal of Colloid and Interface Science Pub Date : 2026-01-01 Epub Date: 2025-08-19 DOI:10.1016/j.jcis.2025.138780
Wanlin Xu, Bensen Ye, Qi Wu
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引用次数: 0

Abstract

The development of triple-functional catalysts to inhibit the shuttle effect of polysulfide (NaPSs) and speed up the kinetics of charge-discharge events is crucial to advance the practical use of sodium‑sulfur batteries (NaSBs). However, the application of g-C3N4 and CN as sulfur hosts in NaSBs is hindered by their inherently low electrical conductivity and high energy barriers for Na+ migration. In this work, the density functional theory (DFT) and ab-initio molecular dynamics (AIMD) simulations reveal that the Na atoms have a tendency to favor a "self-building" process, which result in the formation of Na@g-C3N4 and Na@CN after the initial discharge. Notably, within the Na-embedded substrates, the trapped Na effectively balances the polarity of the N6 cavity, accompanied with a moderate binding with NaPSs and effective dissociation of Na2S. Electronic structure analysis reveals that the incorporation of Na significantly enhances the electrical conductivity of g-C3N4/CN and creates efficient channels for Na+ diffusion. This promotes the transport of Na+ with lower migration energy barriers (0.61 and 0.69 eV) in Na@g-C3N4 and Na@CN, thereby accelerating the dynamic transformation and desorption of intermediates. Overall, this study offers new insights into the structural evolution mechanisms of g-C3N4 and CN, and provides valuable guidance for the subsequent design and experimental research of high-performance Na-S battery catalysts.

基于第一性原理计算的自构建钠修饰g-C3N4/CN在钠硫电池中的快速动力学。
开发抑制多硫化物穿梭效应和加速充放电动力学的三功能催化剂对推进钠硫电池的实用化至关重要。然而,g-C3N4和CN在nasb中作为硫宿主的应用受到其固有的低电导率和Na+迁移的高能量势垒的阻碍。本文通过密度泛函理论(DFT)和ab-initio分子动力学(AIMD)模拟表明,Na原子在初始放电后倾向于“自构建”过程,从而形成Na@g-C3N4和Na@CN。值得注意的是,在Na嵌入的衬底中,被捕获的Na有效地平衡了N6空腔的极性,伴随着与NaPSs的适度结合和Na2S的有效解离。电子结构分析表明,Na的加入显著提高了g-C3N4/CN的电导率,并为Na+的扩散创造了有效的通道。这促进了Na+以较低的迁移能垒(0.61 eV和0.69 eV)在Na@g-C3N4和Na@CN中的迁移,从而加速了中间产物的动态转化和解吸。总体而言,本研究为g-C3N4和CN的结构演化机制提供了新的见解,为后续高性能Na-S电池催化剂的设计和实验研究提供了有价值的指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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