Li Zhengang, Wu Xiaohong, Yu Xiaoyu, Zhou Shiyuan, Qiao Yu, Zhou Haoshen, Sun Shi-Gang
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen 361005, People's Republic of China.
Nano Lett. 2022 Mar 23;22(6):2538-2546. doi: 10.1021/acs.nanolett.2c00460. Epub 2022 Mar 10.
Aqueous zinc iodide (Zn-I) batteries are promising large-scale energy-storage devices. However, the uncontrollable diffuse away/shuttle of soluble I leads to energy loss (low Coulombic efficiency, CE), and poor reversibility (self-discharge). Herein, we employ an ordered framework window within a zeolite molecular sieve to restrain I crossover and prepare zeolite molecular sieve particles into compact, large-scale, and flexible membranes at the engineering level. The as-prepared membrane can confine I within the catholyte region and restrain its irreversible escape, which is proved via space-resolution and electrochemical in situ time-resolution Raman technologies. As a result, overcharge/self-discharge and Zn corrosion are effectively controlled by zeolite separator. After replacing the typically used glass fiber separator to a zeolite membrane, the CE of Zn-I battery improves from 78.9 to 98.6% at 0.2 A/g. Besides, after aging at the fully charged state for 5.0 h, self-discharge is restrained and CE is enhanced from 44.0 to 85.65%. Moreover, the Zn-I cell maintains 91.0% capacity over 30,000 cycles at 4.0 A/g.
水系碘化锌（Zn-I）电池是很有前景的大规模储能装置。然而，可溶性碘的不可控扩散/穿梭导致能量损失（库仑效率低，CE）和可逆性差（自放电）。在此，我们在沸石分子筛中采用有序框架窗口来抑制碘的交叉，并在工程层面将沸石分子筛颗粒制备成致密、大规模且柔性的膜。所制备的膜可将碘限制在阴极电解液区域内，并抑制其不可逆逸出，这通过空间分辨率和电化学原位时间分辨拉曼技术得到了证实。结果，沸石隔膜有效地控制了过充/自放电和锌的腐蚀。将典型使用的玻璃纤维隔膜替换为沸石膜后，Zn-I电池在0.2 A/g时的CE从78.9%提高到98.6%。此外，在完全充电状态下老化5.0小时后，自放电受到抑制，CE从44.0%提高到85.65%。而且，Zn-I电池在4.0 A/g下经过30000次循环后仍保持91.0%的容量。
