Despite the promise of aqueous zinc ion batteries (AZIBs) for safe and sustainable grid storage, water-induced side reactions at the Zn anode, such as hydrogen evolution reactions (HER), corrosion and dendrite growth, make interfacial water suppression a critical research focus. The incorporated dual-site MBA additive anchors water molecules via ─C═O and ─NH functional groups, thereby disrupting the original hydrogen bond network among water molecules and significantly suppressing water activity and HER. The proposed strategy reveals the importance of hydrogen bond network regulation for the design of stable aqueous electrolyte, which provides inspiration for electrolyte design for safe, stable, and efficient electrochemical energy storage devices in the future.
Abstract:
Irregular dendrite growth and complex side reactions pose critical challenges that significantly impede the further industrialization of aqueous zinc-ion batteries (AZIBs). The “competitive co-solvents” strategy could introduce hydrogen bond (H-bond) accepting sites to effectively alleviate the free water molecules. however, it suffers from low conductivity, high cost, and safety risks. Herein, we selected N, N‘-methylenebisacrylamide (MBA) as a trace additive with amide groups to decrease the activity of water by disrupting the H-bond. The MBA additive, which incorporates both hydrogen bond donor and acceptor functionalities, successfully restricts H2O molecules within a double-site anchoring configuration. This configuration enhances hydrogen-bonding interactions and breaks part of the original hydrogen bond network among H2O molecules, thereby significantly restraining parasitic side reactions due to the decomposition of active water. Additionally, MBA molecules adsorbed on the surface of the Zn anode could regulate the desolvation and nucleation processes of zinc ions, achieving dense and flat zinc deposition. A high Zn reversibility with Coulombic efficiency (CE) of 99.74% and ultra-long lifespan of 2800 cycles at 1 and 0.5 mAh cm−2 was demonstrated. Besides, a highly reversible Zn electrode significantly boosted the overall performance of Zn//Zn symmetric cells of 1500 h at 5 mA cm−2 and Zn//V2O5 full cell of 2000 cycles at 5 A g−1.
Author list:
Dongping Chen†, Xipo Ma†, Weihao Xu†, Chunshuang Yan*, Pengbo Lyu*, Qiang Zhu, Huaming Yu, Zhenren Gao, Chade Lv*
How to cite:
D. Chen, X. Ma, W. Xu, C. Yan, P. Lyu, Q. Zhu, H. Yu, Z. Gao, C. Lv, Exploration 2025, 5, 20240007.
https://doi.org/10.1002/EXP.20240007