Hu Honghao, Zhang Qingxu, Liu Jiucong, Li Junjie, Wu Pingli, Li Caicai, Du Peipei, Li Huiqiao, Liu Xizheng
Key Laboratory of Flexible Optoelectronic Materials and Technology, Ministry of Education, School of Optoelectronic Materials & Technology, Jianghan University, Wuhan, 430056, China.
Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Adv Sci (Weinh). 2025 Aug;12(32):e05539. doi: 10.1002/advs.202505539. Epub 2025 May 29.
Low round-trip efficiency and limited cycle durability remain significant challenges for commercial of Lithium-air batteries (LABs). This study introduces a novel electrolyte additive, diaminopropane (DAP), that simultaneously addresses anode stability and cathode reaction kinetics in ambient LABs. The proposed mechanism involves a bi-function approach: 1) at the anode, DAP spontaneously reacts with metallic Li to form Li-DAP, which subsequently cross-links with ether solvents to create a protective gel layer. This layer effectively mitigates Li dendrite formation and shields the anode from ambient moisture and CO corrosion. 2) At the cathode, DAP modifies the oxygen reduction pathway from surface-mediated to solution-mediated, while simultaneously acting as an efficient redox mediator during charging. This dual functionality results in a remarkable reduction of the initial charging potential from 4.2 to 3.4 V, accompanied by observed singlet oxygen quenching. The implemented DAP additive enables LABs to achieve unprecedented cycling stability, demonstrating continuous operation for 1000 h in ambient air while maintaining energy efficiency exceeding 70%. This work establishes an effective electrolyte additive strategy for developing high-performance ambient LABs through simultaneous anode protection and enhanced cathode reaction reversibility.
低往返效率和有限的循环耐久性仍然是锂空气电池(LABs)商业化面临的重大挑战。本研究引入了一种新型电解质添加剂二氨基丙烷(DAP),它同时解决了环境LABs中的阳极稳定性和阴极反应动力学问题。所提出的机制涉及一种双功能方法:1)在阳极,DAP与金属锂自发反应形成Li-DAP,随后Li-DAP与醚类溶剂交联形成一层保护凝胶层。该层有效地减轻了锂枝晶的形成,并保护阳极免受环境水分和CO腐蚀。2)在阴极,DAP将氧还原途径从表面介导转变为溶液介导,同时在充电过程中作为一种有效的氧化还原介质。这种双重功能导致初始充电电位从4.2 V显著降低到3.4 V,同时观察到单线态氧猝灭。所采用的DAP添加剂使LABs能够实现前所未有的循环稳定性,在环境空气中连续运行1000小时,同时保持超过70%的能量效率。这项工作通过同时保护阳极和提高阴极反应可逆性,建立了一种有效的电解质添加剂策略,用于开发高性能的环境LABs。