Zheng Shiyou, Han Pan, Han Zhuo, Zhang Huijuan, Tang Zhihong, Yang Junhe
School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
Sci Rep. 2014 Apr 29;4:4842. doi: 10.1038/srep04842.
High stable C/S composites are fabricated by a novel high-temperature sulfur infusion into micro-mesoporous carbon method following with solvent cleaning treatment. The C/S composite cathodes show high Coulombic efficiency, long cycling stability and good rate capability in the electrolyte of 1.0 M LiPF6 + EC/DEC (1:1 v/v), for instance, the reversible capacity of the treated C/S-50 (50% S) cathode retains around 860 mAh/g even after 500 cycles and the Coulombic efficiency is close to 100%, which demonstrates the best electrochemical performance of carbon-sulfur composite cathodes using the carbonate-based electrolyte reported to date. It is believed that the chemical bond of C-S is responsible for the superior electrochemical properties in Li-S battery, that is, the strong interaction between S and carbon matrix significantly improves the conductivity of S, effectively buffers the structural strain/stress caused by the large volume change during lithiation/delithiation, completely eliminates the formation of high-order polysulfide intermediates, and substantially avoids the shuttle reaction and the side reaction between polysulfide anions and carbonate solvent, and thus enables the C/S cathode to use conventional carbonate-based electrolytes and achieve outstanding electrochemical properties in Li-S battery. The results may substantially contribute to the progress of the Li-S battery technology.
通过一种新颖的高温硫注入微介孔碳方法并随后进行溶剂清洗处理来制备高稳定性的C/S复合材料。C/S复合阴极在1.0 M LiPF6 + EC/DEC(1:1 v/v)电解液中表现出高库仑效率、长循环稳定性和良好的倍率性能,例如,经过处理的C/S-50(50% S)阴极即使在500次循环后可逆容量仍保持在860 mAh/g左右,且库仑效率接近100%,这展示了迄今为止报道的使用碳酸盐基电解液的碳硫复合阴极的最佳电化学性能。据信,C-S化学键是Li-S电池中优异电化学性能的原因,即S与碳基体之间的强相互作用显著提高了S的导电性,有效缓冲了锂化/脱锂过程中由大体积变化引起的结构应变/应力,完全消除了高阶多硫化物中间体的形成,并基本避免了穿梭反应以及多硫阴离子与碳酸盐溶剂之间的副反应,从而使C/S阴极能够使用传统的碳酸盐基电解液并在Li-S电池中实现出色的电化学性能。这些结果可能会极大地推动Li-S电池技术的进步。