Zhong Yunpeng, Xie Xuesong, Zeng Zhiyuan, Lu Bingan, Chen Gen, Zhou Jiang
School of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South University, Changsha, Hunan, 410083, P. R. China.
Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, P. R. China.
Angew Chem Int Ed Engl. 2023 Oct 2;62(40):e202310577. doi: 10.1002/anie.202310577. Epub 2023 Aug 24.
Aqueous rechargeable zinc-ion batteries (ARZBs) are impeded by the mutual problems of unstable cathode, electrolyte parasitic reactions, and dendritic growth of zinc (Zn) anode. Herein, a triple-functional strategy by introducing the tetramethylene sulfone (TMS) to form a hydrated eutectic electrolyte is reported to ameliorate these issues. The activity of H O is inhibited by reconstructing hydrogen bonds due to the strong interaction between TMS and H O. Meanwhile, the preferentially adsorbed TMS on the Zn surface increases the thickness of double electric layer (EDL) structure, which provides a shielding buffer layer to suppress dendrite growth. Interestingly, TMS modulates the primary solvation shell of Zn ultimately to achieve a novel solvent co-intercalation ((Zn-TMS) ) mechanism, and the intercalated TMS works as a "pillar" that provides more zincophilic sites and stabilizes the structure of cathode (NH V O , (NVO)). Consequently, the Zn||NVO battery exhibits a remarkably high specific capacity of 515.6 mAh g at a low current density of 0.2 A g for over 40 days. This multi-functional electrolytes and solvent co-intercalation mechanism will significantly propel the practical development of aqueous batteries.
水系可充电锌离子电池（ARZBs）受到阴极不稳定、电解质寄生反应以及锌（Zn）阳极枝晶生长等共同问题的阻碍。在此，报道了一种通过引入四亚甲基砜（TMS）形成水合共晶电解质的三功能策略来改善这些问题。由于TMS与H₂O之间的强相互作用，通过重建氢键抑制了H₂O的活性。同时，优先吸附在Zn表面的TMS增加了双电层（EDL）结构的厚度，这提供了一个屏蔽缓冲层来抑制枝晶生长。有趣的是，TMS最终调节Zn的初级溶剂化壳层以实现一种新型的溶剂共嵌入（(Zn-TMS)₂⁺）机制，并且嵌入的TMS充当“支柱”，提供更多亲锌位点并稳定阴极（NH₄V₆O₁₆，(NVO)）的结构。因此，Zn||NVO电池在0.2 A g的低电流密度下表现出高达515.6 mAh g的比容量，持续超过40天。这种多功能电解质和溶剂共嵌入机制将显著推动水系电池的实际发展。
