Cai Da-Qian, Gao Ya-Ting, Wang Xin-Yu, Yang Jin-Lin, Zhao Shi-Xi
School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China.
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
ACS Appl Mater Interfaces. 2022 Aug 31;14(34):38651-38659. doi: 10.1021/acsami.2c06676. Epub 2022 Aug 17.
Lithium-sulfur (Li-S) batteries (LSBs) have been considered one of the most potential candidates to substitute traditional Li-ion batteries (LIBs), owing to their high theoretical energy density and low cost. Nevertheless, the shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) have long been obstacles to realizing stable LSBs with high reversible capacity. In this study, we proposed a metal-semiconductor (Mo and MoO) heterostructure with the hollow microsphere morphology as an effective Mott-Schottky electrocatalyst to boost sulfur electrochemistry. The hollow structure can physically inhibit the shuttling of LiPSs and accommodate the volume fluctuation during cycling. More importantly, the built-in electric field at the heterointerfacial sites can effectively accelerate the reduction of LiPSs and oxidation of LiS, thereby reaching a high sulfur utilization. With the assistance of the Mo/MoO catalyst, the cell exhibited prominent rate capability and stable long-term cycling performance, showing a high capacity of 630 mA h·g at 4 C and a low decay of 0.073% at 1 C after 500 cycles. Even with high areal sulfur loading of 10.0 mg·cm, high capacity and good cycle stability were achieved at 0.2 C under lean electrolyte conditions (E/S ratio of 6 μL·mg).
锂硫(Li-S)电池因其高理论能量密度和低成本,被认为是替代传统锂离子电池(LIBs)最具潜力的候选者之一。然而,多硫化锂(LiPSs)的穿梭效应和缓慢的氧化还原动力学长期以来一直是实现具有高可逆容量的稳定锂硫电池的障碍。在本研究中,我们提出了一种具有中空微球形态的金属-半导体(Mo和MoO)异质结构,作为一种有效的莫特-肖特基电催化剂来促进硫电化学。中空结构可以物理抑制LiPSs的穿梭,并适应循环过程中的体积波动。更重要的是,异质界面处的内建电场可以有效加速LiPSs的还原和LiS的氧化,从而实现高硫利用率。在Mo/MoO催化剂的辅助下,该电池表现出突出的倍率性能和稳定的长期循环性能,在4 C下容量高达630 mA h·g,在1 C下500次循环后衰减率低至0.073%。即使在高面硫负载量为10.0 mg·cm、贫电解质条件(E/S比为6 μL·mg)下的0.2 C时,也实现了高容量和良好的循环稳定性。