Hui Xiaobin, Zhan Zhen, Zhang Zeyu, Yu Jingya, Jiang Pengyan, Dang Zhengzheng, Wang Jian, Cai Songhua, Wang Yanming, Xu Zheng-Long
Research Institute for Advanced Manufacturing, Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, SAR 999077, China.
State Key Laboratory of Ultra-precision Machining Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, SAR 999077, China.
ACS Nano. 2024 Sep 10;18(36):25237-25248. doi: 10.1021/acsnano.4c07907. Epub 2024 Aug 29.
Solid-state polymer electrolytes (SPEs) are promising for high-performance zinc metal batteries (ZMBs), but they encounter critical challenges of low ionic conductivity, limited Zn transference number (), and an unstable electrolyte-electrode interface. Here, we present an effective approach involving a missing-linker metallic organic framework (MOF)-catalyzed poly(ethylene glycol) diacrylate (PEGDA)/polyacrylamide (PAM) copolymer SPE for single Zn conduction and seamless electrolyte-electrode contact. The single-Zn conduction is facilitated by the anchoring of the OTF anions onto the unsaturated metal sites of missing-linker MOF, while the PEGDA and PAM chains in competitive coordination with Zn ions promote rapid Zn ion transport. Our all-solid-state electrolyte simultaneously achieves a superior ionic conductivity of 1.52 mS cm and a high of 0.83 at room temperature, alongside uniform Zn metal deposition (1000 cycles in symmetric cells) and high Zn plating/striping efficiencies (>99% after 600 cycles in asymmetric cells). Applications of our SPE in Zn//VO full cells are further demonstrated with a long lifespan of 2000 cycles and an extremely low-capacity degradation rate of 0.012% per cycle. This work provides an effective strategy for using a missing-linker MOF to catalyze competitively coordinating copolymers for accelerating Zn ion conduction, assisting the future design of all-solid-state ZMBs.
固态聚合物电解质（SPEs）在高性能锌金属电池（ZMBs）方面具有广阔前景，但它们面临着离子电导率低、锌迁移数（）有限以及电解质-电极界面不稳定等关键挑战。在此，我们提出了一种有效的方法，涉及一种缺联剂金属有机框架（MOF）催化的聚乙二醇二丙烯酸酯（PEGDA）/聚丙烯酰胺（PAM）共聚物SPE，用于单一锌传导和无缝电解质-电极接触。通过将OTF阴离子锚定在缺联剂MOF的不饱和金属位点上促进单一锌传导，而与锌离子竞争配位的PEGDA和PAM链促进锌离子快速传输。我们的全固态电解质在室温下同时实现了1.52 mS cm的优异离子电导率和0.83的高 ，以及均匀的锌金属沉积（对称电池中1000次循环）和高的锌电镀/脱镀效率（非对称电池中600次循环后>99%）。我们的SPE在Zn//VO全电池中的应用进一步得到证明，其具有2000次循环的长寿命和极低的每循环0.012%的容量降解率。这项工作为使用缺联剂MOF催化竞争性配位共聚物以加速锌离子传导提供了一种有效策略，有助于全固态ZMBs的未来设计。
