A low-overpotential, long-life, and “dendrite-free” lithium-O2 battery realized by integrating “iodide-redox-phobic” and “Li-ion-philic” membrane

• Published in: Journal of membrane science 2023-01, Vol.665, p.121112, Article 121112
• Main Authors: Zou, Xiaohong, Lu, Qian, Wang, Cuie, She, Sixuan, Liao, Kaiming, Ran, Ran, Zhou, Wei, An, Liang, Shao, Zongping
• Format: Article
• Language: English
• Subjects: Iodide-redox-phobic membrane; Li-ion-philic membrane; Li–O2 battery; Redox mediators; δ-MnO2 membrane
• ISSN: 0376-7388; 1873-3123
• DOI: 10.1016/j.memsci.2022.121112

Before the practical application of the Li–O2 battery (LOB), a critical issue regarding large overpotential upon charging (which causes irreversible side reactions and low energy efficiency) should be resolved. The utilization of redox mediators (RMs) which oxidatively decompose insulating discharge product, Li2O2, is one promising solution to address this issue. However, the soluble RMs can easily diffuse to and react with the Li metal anode (encountering Li dendrites is even worse). Here, a chemical self-assembly strategy is introduced into the fabrication of the iodide-redox-phobic and Li-ion-philic membrane for LOBs, in which the electronegative δ-MnO2 layer is in-situ grown on commercial polyethylene (PE) membrane (MnO2@PE). The electronegative MnO2 layer can simultaneously repel the shuttle of iodide species and regulate the uniform Li + deposition. Controlling cut-off capacity of 1000 mAh g−1, iodide-redox-based LOB with MnO2@PE demonstrates low overpotentials (∼0.7 V vs. Li+/Li), dendrite-suppressing capability, as well as impressive long-term reversibility over 500 cycles (2000 h), which urges the LOB technology competitive among the next-generation rechargeable power systems. [Display omitted] •The δ-MnO2-based membrane with iodide-redox-phobic and Li-ion-philic characters has been prepared.•In situ constructed δ-MnO2 layer on polyethylene membrane (MnO2@PE) is highly flexible and tightly linked.•The electronegative MnO2@PE membrane can simultaneously suppress the iodide-redox shuttle and Li dendrite growth.•Li–O2 battery with MnO2@PE membrane shows long-term reversibility over 500 cycles (2000 h) with a small overpotential.