Xin Diheng, Zhang Xianchi, Zhang Zhanrui, Sun Jie, Li Qi, He Xuexia, Jiang Ruibin, Liu Zonghuai, Lei Zhibin
Key Laboratory of Applied Surface and Colloid Chemistry, MOE, Shaanxi Engineering Lab for Advanced Energy Technology, Shaanxi Key Laboratory for Advanced Energy Devices, School of Materials Science and Engineering, Shaanxi Normal University, 620 West Chang'an Street, Xi'an, Shaanxi, 710119, China.
Small. 2024 Nov;20(44):e2403050. doi: 10.1002/smll.202403050. Epub 2024 Jul 10.
Applications of aqueous zinc ion batteries (ZIBs) for grid-scale energy storage are hindered by the lacking of stable cathodes with large capacity and fast redox kinetics. Herein, the intercalation of tetramethylammonium (TMA) cations is reported into MoS interlayers to expand its spacing from 0.63 to 1.06 nm. The pre-intercalation of TMA induces phase transition of MoS from 2H to 1T phase, contributing to an enhanced conductivity and better wettability. Besides, The calculation from density functional theory indicates that those TMA can effectively shield the interactions between Zn and MoS layers. Consequently, two orders magnitude high Zn ions diffusion coefficient and 11 times enhancement in specific capacity (212.4 vs 18.9 mAh g at 0.1 A g) are achieved. The electrochemical investigations reveal both Zn and H can be reversibly co-inserted into the MoS-TMA electrode. Moreover, the steady habitat of TMA between MoS interlayers affords the MoS-TMA with remarkable cycling stability (90.1% capacity retention after 2000 cycles at 5.0 A g). These performances are superior to most of the recent zinc ion batteries assembled with MoS or VS-based cathodes. This work offers a new avenue to tuning the structure of MoS for aqueous ZIBs.
水系锌离子电池（ZIBs）在电网规模储能领域的应用受到缺乏大容量且具有快速氧化还原动力学的稳定阴极的阻碍。在此，据报道四甲基铵（TMA）阳离子嵌入到MoS的层间，使其层间距从0.63纳米扩大到1.06纳米。TMA的预嵌入诱导MoS从2H相转变为1T相，有助于提高导电性和润湿性。此外，密度泛函理论计算表明，这些TMA可以有效屏蔽Zn与MoS层之间的相互作用。因此，实现了两个数量级高的Zn离子扩散系数以及比容量提高11倍（在0.1 A g下，分别为212.4和18.9 mAh g）。电化学研究表明，Zn和H都可以可逆地共嵌入到MoS-TMA电极中。此外，TMA在MoS层间的稳定存在赋予MoS-TMA显著的循环稳定性（在5.0 A g下循环2000次后容量保持率为90.1%）。这些性能优于最近大多数用MoS或VS基阴极组装的锌离子电池。这项工作为水系ZIBs中MoS结构的调控提供了一条新途径。
