{"title":"Self-building sodium modified g-C<sub>3</sub>N<sub>4</sub>/CN for fast kinetics in sodium‑sulfur batteries by first-principles calculations.","authors":"Wanlin Xu, Bensen Ye, Qi Wu","doi":"10.1016/j.jcis.2025.138780","DOIUrl":null,"url":null,"abstract":"<p><p>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-C<sub>3</sub>N<sub>4</sub> and CN as sulfur hosts in NaSBs is hindered by their inherently low electrical conductivity and high energy barriers for Na<sup>+</sup> 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-C<sub>3</sub>N<sub>4</sub> and Na@CN after the initial discharge. Notably, within the Na-embedded substrates, the trapped Na effectively balances the polarity of the N<sub>6</sub> cavity, accompanied with a moderate binding with NaPSs and effective dissociation of Na<sub>2</sub>S. Electronic structure analysis reveals that the incorporation of Na significantly enhances the electrical conductivity of g-C<sub>3</sub>N<sub>4</sub>/CN and creates efficient channels for Na<sup>+</sup> diffusion. This promotes the transport of Na<sup>+</sup> with lower migration energy barriers (0.61 and 0.69 eV) in Na@g-C<sub>3</sub>N<sub>4</sub> 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-C<sub>3</sub>N<sub>4</sub> and CN, and provides valuable guidance for the subsequent design and experimental research of high-performance Na-S battery catalysts.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"701 ","pages":"138780"},"PeriodicalIF":9.7000,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.jcis.2025.138780","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/8/19 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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.
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