Xia Ji-Li, Yan Dong, Guo Li-Ping, Dong Xiao-Ling, Li Wen-Cui, Lu An-Hui
State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
Adv Mater. 2020 May;32(21):e2000447. doi: 10.1002/adma.202000447. Epub 2020 Apr 6.
Hard carbon attracts considerable attention as an anode material for sodium-ion batteries; however, their poor rate capability and low realistic capacity have motivated intense research effort toward exploiting nanostructured carbons in order to boost their comprehensive performance. Ultramicropores are considered essential for attaining high-rate capacity as well as initial Coulombic efficiency by allowing the rapid diffusion of Na and inhibiting the contact of the electrolyte with the inner carbon surfaces. Herein, hard carbon nanosheets with centralized ultramicropores (≈0.5 nm) and easily accessible carbonyl groups (CO)/hydroxy groups (OH) are synthesized via interfacial assembly and carbonization strategies, delivering a large capacity (318 mA h g at 0.02 A g ), superior rate capability (145 mA h g at 5.00 A g ), and approximately 95% of reversible capacity below 1.00 V. Notably, a new charge model favoring fast capacitive sodium storage with dual potential plateaus is proposed. That is, the deintercalation of Na from graphitic layers is manifested as the low-potential plateau region (0.01-0.10 V), contributing to stable insertion capacity; meanwhile, the surface desodiation process of the CO and OH groups corresponds to the high-potential plateau region (0.40-0.70 V), contributing to a fast capacitive storage.
硬碳作为钠离子电池的负极材料备受关注;然而,其较差的倍率性能和较低的实际容量促使人们对开发纳米结构碳进行了深入研究,以提高其综合性能。超微孔被认为对于实现高倍率容量以及初始库仑效率至关重要,因为它能使钠离子快速扩散,并抑制电解质与碳内部表面的接触。在此,通过界面组装和碳化策略合成了具有集中超微孔(≈0.5纳米)和易于接触的羰基(CO)/羟基(OH)的硬碳纳米片,其在0.02 A g 时具有大容量(318 mA h g)、优异的倍率性能(在5.00 A g 时为145 mA h g),并且在1.00 V以下具有约95%的可逆容量。值得注意的是,提出了一种有利于快速电容性储钠的新电荷模型,该模型具有双电位平台。也就是说,钠离子从石墨层的脱嵌表现为低电位平台区域(0.01 - 0.10 V),有助于稳定的嵌入容量;同时,CO和OH基团的表面去钠过程对应于高电位平台区域(0.40 - 0.70 V),有助于快速电容性存储。