发表机构
Université de Haute-Alsace; Institut de Science des Matériaux de Mulhouse (IS2M); CNRS UMR 7361; Université de Strasbourg; Réseau sur le Stockage Electrochimique de l’Energie (RS2E); CNRS FR3459（阿尔萨斯大学; 穆尔豪斯材料科学研究所; 法国国家科学研究中心联合研究实验室7361; 斯特拉斯堡大学; 电化学储能网络; 法国国家科学研究中心自由研究基金3459）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究探讨了硬碳自支撑电极厚度、大孔率及电解液添加剂对钠离子电池SEI形成和循环稳定性的影响，发现FEC添加剂可改善稳定性，实现高达93%的初始库仑效率和328 mAh g-1的可逆容量。
AI 中文摘要
硬碳自支撑电极（HC SSEs）作为钠离子电池（SIBs）中传统粘合剂基负极材料的替代方案引起了广泛关注，其无需使用粘合剂、溶剂、导电碳和集流体。在本工作中，我们研究了HC厚度和大孔率以及电解液添加剂的存在/缺失对固体电解质界面（SEI）形成和电化学性能的影响。通过1500°C热解过程，使用三种不同厚度的纤维素基滤纸（FP）前驱体制备了HC SSEs，并将其与从商业碳布获得的HC SSE进行了比较。结果强调了材料适当的结构、形貌、孔隙率和表面化学性质对于实现高初始库仑效率（高达93%）和高可逆容量（在37.2 mA g-1下高达328 mAh g-1）的重要性。然而，循环稳定性受到电极厚度/大孔率和电解液添加剂的显著影响。在不含氟代碳酸乙烯酯（FEC）添加剂的NaPF6中，最薄电极（79 μm）获得了最大循环次数（50次），而电极厚度>185 μm时观察到快速衰减（约1-5次循环后）。通过使用FEC添加剂，衰减得到缓解，所有电极均达到循环稳定性（100次循环），但商业电极除外（5次循环），因其厚度最高（1042 μm）。稳定性的改善可归因于在FEC存在下形成了含有更多NaF的薄而均匀的无机富集SEI，该SEI更稳定、更具保护性且具有电子导电性。
英文摘要
Hard carbon self-supported electrodes (HC SSEs) have gained significant interest as an alternative to classical binder-based anode materials for sodium-ion batteries (SIBs), eliminating the need for binders, solvents, conductive carbon, and current collectors. In this work, we investigate the impact of HC thickness and macroporosity, as well as the presence/absence of an electrolyte additive, on the formation of the solid electrolyte interphase (SEI) and electrochemical performance. Three cellulose-based filter paper (FP) precursors with different thicknesses were used to prepare HC SSEs through a pyrolysis process at 1500 {\textdegree}C, and then these were compared with an HC SSE obtained from commercial carbon fabric. The results highlight the importance of appropriate structural, morphological, porosity, and surface chemical properties of the materials to achieve high initial Coulombic efficiency (up to 93%) and high reversible capacity (up to 328 mAh g -1 at 37.2 mA g -1 ). However, the cycle stability was greatly impacted by the electrode thickness/macroporosity and the electrolyte additive. In NaPF6 without fluoroethylene carbonate (FEC) additive, the maximum number of cycles (50) was obtained for the thinnest electrode (79 $μ$m), while rapid fading (after $\approx$1-5 cycles) was observed for electrode thicknesses >185 $μ$m. By using the FEC additive, the fading is mitigated and cycling stability (100 cycles) is reached for all the electrodes, except the commercial one (5 cycles), due to its highest thickness (1042 $μ$m). The improvement in stability could be explained by the buildup of a thin homogeneous inorganic-rich SEI containing more NaF in the presence of FEC, which is more stable, protective, and electronically conductive.
Journal refACS Applied Materials \& Interfaces, 2026, 18 (22), pp.31101-31118
