Liang Puwu, Pan Duo, Hu Xiang, Yang Ke R, Liu Yangjie, Huo Zijing, Bo Zheng, Xu Lihong, Xu Junhua, Wen Zhenhai
State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques Toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, People's Republic of China.
College of Chemistry, Fuzhou University, Fuzhou, 350002, People's Republic of China.
Nanomicro Lett. 2025 Apr 28;17(1):237. doi: 10.1007/s40820-025-01767-4.
Manganese-based chalcogenides have significant potential as anodes for sodium-ion batteries (SIBs) due to their high theoretical specific capacity, abundant natural reserves, and environmental friendliness. However, their application is hindered by poor cycling stability, resulting from severe volume changes during cycling and slow reaction kinetics due to their complex crystal structure. Here, an efficient and straightforward strategy was employed to in-situ encapsulate single-phase porous nanocubic MnSSe into carbon nanofibers using electrospinning and the hard template method, thus forming a necklace-like porous MnSSe-carbon nanofiber composite (MnSSe@N-CNF). The introduction of Se significantly impacts both the composition and microstructure of MnSSe, including lattice distortion that generates additional defects, optimization of chemical bonds, and a nano-spatially confined design. In situ/ex-situ characterization and density functional theory calculations verified that this MnSSe@N-CNF alleviates the volume expansion and facilitates the transfer of Na/electron. As expected, MnSSe@N-CNF anode demonstrates excellent sodium storage performance, characterized by high initial Coulombic efficiency (90.8%), high-rate capability (370.5 mAh g at 10 A g) and long durability (over 5000 cycles at 5 A g). The MnSSe@N-CNF //NVP@C full cell, assembled with MnSSe@N-CNF as anode and NaV(PO)@C as cathode, exhibits a high energy density of 254 Wh kg can be provided. This work presents a novel strategy to optimize the design of anode materials through structural engineering and Se substitution, while also elucidating the underlying reaction mechanisms.
基于锰的硫族化合物因其高理论比容量、丰富的天然储量和环境友好性,作为钠离子电池(SIBs)的负极具有巨大潜力。然而,由于其在循环过程中会发生严重的体积变化以及复杂晶体结构导致的缓慢反应动力学,其应用受到循环稳定性差的阻碍。在此,采用了一种高效且直接的策略,通过静电纺丝和硬模板法将单相多孔纳米立方MnSSe原位封装到碳纳米纤维中,从而形成项链状多孔MnSSe-碳纳米纤维复合材料(MnSSe@N-CNF)。Se的引入对MnSSe的组成和微观结构都有显著影响,包括产生额外缺陷的晶格畸变、化学键的优化以及纳米空间受限设计。原位/非原位表征和密度泛函理论计算证实,这种MnSSe@N-CNF减轻了体积膨胀并促进了Na/电子的转移。正如预期的那样,MnSSe@N-CNF负极表现出优异的储钠性能,其特征在于高初始库仑效率(90.8%)、高倍率性能(在10 A g下为370.5 mAh g)和长耐久性(在5 A g下超过5000次循环)。以MnSSe@N-CNF作为负极和NaV(PO)@C作为正极组装的MnSSe@N-CNF//NVP@C全电池,可提供254 Wh kg的高能量密度。这项工作提出了一种通过结构工程和Se替代来优化负极材料设计的新策略,同时也阐明了潜在的反应机制。