澳大利亚伍伦贡大学Weijie Li团队开发出了基于功能群组装策略的长效锌金属电池双层稳压器设计。相关研究成果于2024年5月7日发表在国际顶尖学术期刊《德国应用化学》。

通过使用电解质添加剂来调节锌金属阳极的双电层（EDL）结构，是抑制界面副反应和促进锌均匀沉积的有效方法。然而，在实验开始之前，没有研究EDL调节添加剂的主动设计报告。

该文中，研究人员提出了一种官能团组装策略来设计用于调节EDL的电解质添加剂，从而实现持久的锌金属阳极。具体而言，通过筛选10个常见官能团，N，N-二甲基-1H-咪唑-1-磺酰胺（IS）是通过组装咪唑基和砜基而设计的，咪唑基的特征在于其在锌阳极上的高吸附能力，砜基表现出与Zn²⁺离子的强结合。

得益于咪唑基团的吸附功能化，IS分子占据了EDL内部亥姆霍兹层中H₂O的位置，形成了分子保护层以抑制H₂O诱导的副反应。同时，IS中的砜基作为与Zn²⁺的结合位点，促进Zn²⁺离子的去溶剂化，促进致密的锌沉积。因此，IS的利用显著延长了Zn||Zn和Zn||NaV₃O₈·1.5H₂O全电池的循环稳定性。

该项研究为高性能锌金属电池的EDL调节器的设计提供了一种创新的方法。

附：英文原文

Title: Electric Double Layer Regulator Design through a Functional Group Assembly Strategy towards Long-lasting Zinc Metal Batteries

Author: Liyang Liu, Xin-Yi Wang, Zewei Hu, Xin Wang, Qingqing Zheng, Chao Han, Jiantie Xu, Xun Xu, Hua-Kun Liu, Shi-Xue Dou, Weijie Li

Issue&Volume: 2024-05-07

Abstract: Regulating the electric double layer (EDL) structure of the zinc metal anode by using electrolyte additives is an efficient way to suppress interface side reactions and facilitate uniform zinc deposition. Nevertheless, there are no reports investigating the proactive design of EDL-regulating additives before the start of experiments. Herein, a functional group assembly strategy is proposed to design electrolyte additives for modulating the EDL, thereby realizing a long-lasting zinc metal anode. Specifically, by screening ten common functional groups, N, N-dimethyl-1H-imidazole-1-sulfonamide (IS) is designed by assembling an imidazole group, characterized by its high adsorption capability on the zinc anode, and a sulfone group, which exhibits strong binding with Zn2+ ions. Benefiting from the adsorption functionalization of the imidazole group, the IS molecules occupy the position of H2O in the inner Helmholtz layer of the EDL, forming a molecular protective layer to inhibit H2O-induced side reactions. Meanwhile, the sulfone group in IS, acting as a binding site to Zn2+, promotes the de-solvation of Zn2+ ions, facilitating compact zinc deposition. Consequently, the utilization of IS significantly extending the cycling stability of Zn||Zn and Zn||NaV3O8·1.5H2O full cell. This study offers an innovative approach to the design of EDL regulators for high-performance zinc metal batteries.

DOI: 10.1002/anie.202405209

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202405209