Zhong Wei, Cheng Hao, Zhang Shichao, Li Laixi, Tan Chaoqiang, Chen Wei, Lu Yingying
State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou, 311215, China.
Nat Commun. 2025 May 17;16(1):4586. doi: 10.1038/s41467-025-59894-w.
Aqueous Zn-halogen batteries, valued for high safety, large capacity, and low cost, suffer from the polyhalide shuttle effect and chaotic zinc electrodeposition, reducing energy efficiency and lifespan. Here we show a cation-driven positive electrode phase transition to suppress the shuttle effect and achieve uniform zinc electrodeposition, along with an anion kinetic enhancement strategy to improve energy efficiency and lifespan. Taking tetramethylammonium halide (TMAX, X = F, Cl, Br) as a subject, TMA promotes oriented zinc (101) deposition on the negative electrode through electrostatic shielding, significantly extending cycling life. Concurrently, it captures I on the positive electrode, forming a stable solid-phase interhalide complex that enhances coulombic efficiency. Compared to I and TMAI, X anions lower the Gibbs free energy differences of I → IX and IX → TMAIX, accelerating I/IX/TMAIX conversions and improving voltage efficiency. In TMAF-modified electrolytes, zinc interhalide complex batteries achieve a high energy efficiency of 95.2% at 0.2 A g with good reversibility, showing only 0.1% capacity decay per cycle over 1000 cycles. At 1 A g, they show a low decay rate of 0.1‰ per cycle across 10,000 cycles. This study provides insights into enhancing energy efficiency and long-term stability for sustainable energy storage.
水系锌卤电池因其高安全性、大容量和低成本而受到重视，但存在多卤化物穿梭效应和混乱的锌电沉积问题，从而降低了能量效率和使用寿命。在此，我们展示了一种阳离子驱动的正极相变，以抑制穿梭效应并实现均匀的锌电沉积，同时还有一种阴离子动力学增强策略来提高能量效率和延长使用寿命。以卤化四甲基铵（TMAX，X = F、Cl、Br）为研究对象，TMA通过静电屏蔽促进锌（101）在负极上的定向沉积，显著延长循环寿命。同时，它在正极捕获I，形成稳定的固相间卤化物络合物，提高库仑效率。与I和TMAI相比，X阴离子降低了I→IX和IX→TMAIX的吉布斯自由能差，加速了I/IX/TMAIX的转化并提高了电压效率。在TMAF改性电解质中，锌卤化物络合物电池在0.2 A g下实现了95.2%的高能量效率且具有良好的可逆性，在1000次循环中每循环仅显示0.1%的容量衰减。在1 A g下，它们在10000次循环中每循环显示出0.1‰的低衰减率。这项研究为提高可持续储能的能量效率和长期稳定性提供了见解。
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