Zhang Jianli, Ai Qinghui, Wang Yang, Du Zepu, Chen Qiang, Hou Guangya, Tang Yiping
College of Material Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Small. 2025 Feb;21(6):e2410226. doi: 10.1002/smll.202410226. Epub 2024 Dec 30.
Lithium-sulfur batteries (LSBs) face challenges from the shuttle effect of lithium polysulfides (LiPSs) and slow redox kinetics. In this study, a NiCo-Doped 3D Ordered Mesoporous Carbon (NiCo-3DOMC) composite material is synthesized using a gel-crystalline template and sol-gel method to modify polypropylene separators in LSBs. Density Functional Theory calculations and experiment results demonstrate that under a magnetic field, the NiCo-3DOMC enhances adsorption and catalyzes the conversion of LiPSs, effectively mitigating the shuttle effect and boosting redox kinetics. This improvement is due to the material's porous structure and active catalytic sites. Enhanced by magnetohydrodynamic effects and NiCo spin polarization, the modified separators in LSBs deliver a high initial capacity of 1544.21 mAh g at 0.1 C, maintain superior rate performance at 565.49 mAh g at 3 C, and show prolonged cycling stability with only 0.06% capacity decay per cycle over 470 cycles. Even with a sulfur loading of 3.78 mg cm, an initial capacity of 884 mAh g at 0.2 C is achieved. This approach marks a significant advancement in LSB performance, leveraging magnetic field applications to improve battery technology.
锂硫电池（LSBs）面临着多硫化锂（LiPSs）穿梭效应和缓慢氧化还原动力学的挑战。在本研究中，采用凝胶-晶体模板法和溶胶-凝胶法合成了一种镍钴掺杂的三维有序介孔碳（NiCo-3DOMC）复合材料，用于修饰锂硫电池中的聚丙烯隔膜。密度泛函理论计算和实验结果表明，在磁场作用下，NiCo-3DOMC增强了对LiPSs的吸附并催化其转化，有效减轻了穿梭效应并加快了氧化还原动力学。这种改善归因于该材料的多孔结构和活性催化位点。受磁流体动力学效应和镍钴自旋极化的增强作用，锂硫电池中经修饰的隔膜在0.1 C时具有1544.21 mAh g的高初始容量，在3 C时以565.49 mAh g保持优异的倍率性能，并在470次循环中显示出仅0.06%的低容量衰减，循环稳定性良好。即使硫负载量为3.78 mg cm，在0.2 C时仍可实现884 mAh g的初始容量。这种方法标志着锂硫电池性能的重大进步，利用磁场应用改进了电池技术。
