Wang Qian, Qiao Shaoming, Huang Chunhong, Wang Xu, Cai Chuan, He Gaohong, Zhang Fengxiang
State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116023, P.R. China.
School of Chemical Engineering, Dalian University of Technology, Panjin 124221, P.R. China.
ACS Appl Mater Interfaces. 2024 May 15;16(19):24502-24513. doi: 10.1021/acsami.4c00660. Epub 2024 May 5.
The severe shuttle effect of polysulfides (LiPSs) and the slow liquid-solid phase conversion are the main obstacles hindering the practical application of lithium-sulfur (Li-S) batteries. Separator modification with a high-activity catalyst can boost LiPSs conversion and suppress their shuttle effect. In this work, multi-heterostructured MXene/NiS/CoS with rich S-vacancies was constructed facilely with a hydrothermal and high-temperature annealing strategy for separator modification. The MXene sheet not only provides a physical barrier but also ensures a high conductivity and adsorption capacity of the catalyst; the dual active centers of NiS and CoS catalyze LiPSs conversion. In addition, the vacancies and heterostructures can modulate the electronic structure of the catalyst, improve its intrinsic activity, and reduce the polysulfides reaction barrier, thus facilitating ion/electron transport and inhibiting the shuttle effect. Benefiting from these advantages, the Li-S battery with MXene/NiS/CoS modified separator exhibits exciting discharge capacities (1495.4 mAh g at 0.1C and 549.0 mAh g at 6C) and an excellent ultra-long cycle life (average capacity decay rate of 0.026% for 2000 cycles at 2C); at a high sulfur loading of 10.0 mg cm, the battery operates for nearly 80 cycles at 0.2C, giving a capacity retention rate of 75.76%. This work provides a high-activity catalyst for Li-S batteries.
多硫化物(LiPSs)严重的穿梭效应以及缓慢的液固相变是阻碍锂硫(Li-S)电池实际应用的主要障碍。用高活性催化剂对隔膜进行改性可以促进LiPSs的转化并抑制其穿梭效应。在这项工作中,采用水热和高温退火策略,简便地构建了具有丰富硫空位的多异质结构MXene/NiS/CoS用于隔膜改性。MXene片不仅提供了物理屏障,还确保了催化剂的高导电性和吸附能力;NiS和CoS的双活性中心催化LiPSs的转化。此外,空位和异质结构可以调节催化剂的电子结构,提高其本征活性,降低多硫化物的反应势垒,从而促进离子/电子传输并抑制穿梭效应。受益于这些优点,采用MXene/NiS/CoS改性隔膜的Li-S电池表现出令人兴奋的放电容量(0.1C时为1495.4 mAh g,6C时为549.0 mAh g)和出色的超长循环寿命(2C下2000次循环的平均容量衰减率为0.026%);在10.0 mg cm的高硫负载下,电池在0.2C下运行近80次循环,容量保持率为75.76%。这项工作为Li-S电池提供了一种高活性催化剂。