Liu Mingquan, Wu Feng, Bai Ying, Li Ying, Ren Haixia, Zhao Ran, Feng Xin, Song Tinglu, Wu Chuan
School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, PR China.
Yangtze Delta Region Academy of Beijing Institute of Technology, Jiaxing 314019, PR China.
ACS Appl Mater Interfaces. 2021 Oct 13;13(40):47671-47683. doi: 10.1021/acsami.1c14738. Epub 2021 Oct 1.
Hard carbon (HC) displays great potential for high-performance sodium-ion batteries (SIBs) due to its cost-effective, simple fabrication and most likely to be commercialized. However, the complicated microstructures of HC lead to difficulties in deeply understanding the structure-performance correlation. Particularly, evaluation of influence of pore structure on Na storage performances is still causing disputes and rational strategies of designing pore architecture of HC are still necessary. In this work, the skillful and controllable phase-inversion method is applied to construct porous HC with abundantly interconnected and permeable tunnel-like pores, which can promote ionic diffusion and improve electrode-electrolyte interfacial affinity. Structure-performance investigation reveals that porous HC with cross-coupled macropore architecture can boost Na storage performances comprehensively. Compared to pristine HC with negligible pores, well-regulated porous HC anodes show an obvious enhancement on initial Coulombic efficiency (ICE) of 68.3% (only 51.5% for pristine HC), reversible capacity of 332.7 mAh g at 0.05 A g, rate performance with 67.4% capacity retention at 2 A g (46.5% for pristine HC), and cycling stability with 95% capacity maintained for 90 cycles (86.4% for pristine HC). Additionally, the ICE can be optimized up to 76% by using sodium carboxymethyl cellulose as a binder. This work provides an important view of optimizing Na storage performances of HC anodes by pore engineering, which can be broadened into other electrode materials.
硬碳(HC)因其成本效益高、制备简单且最有可能实现商业化,在高性能钠离子电池(SIB)中展现出巨大潜力。然而,硬碳复杂的微观结构导致难以深入理解其结构与性能的关系。特别是,孔隙结构对钠存储性能影响的评估仍存在争议,设计硬碳孔隙结构的合理策略仍然必要。在这项工作中,采用巧妙且可控的相转化法构建了具有大量相互连通且可渗透的隧道状孔隙的多孔硬碳,这可以促进离子扩散并改善电极与电解质的界面亲和力。结构 - 性能研究表明,具有交叉耦合大孔结构的多孔硬碳可以全面提升钠存储性能。与孔隙可忽略不计的原始硬碳相比,调控良好的多孔硬碳阳极在初始库仑效率(ICE)方面有明显提高,达到68.3%(原始硬碳仅为51.5%),在0.05 A g下的可逆容量为332.7 mAh g,倍率性能方面,在2 A g时容量保持率为67.4%(原始硬碳为46.5%),循环稳定性方面,90次循环后容量保持95%(原始硬碳为86.4%)。此外,使用羧甲基纤维素钠作为粘结剂时,初始库仑效率可优化至76%。这项工作为通过孔隙工程优化硬碳阳极的钠存储性能提供了重要视角,这一方法可推广到其他电极材料。