Rational Design of Covalent Organic Frameworks as Gas Diffusion Layers for Multi‐atmosphere Lithium‐Air Batteries

Non-aqueous Li-air batteries, despite their high energy density and low cost, have not been deployed practically due to their instability in ambient air, where moisture causes parasitic reactions and shortens their life drastically. Here, we demonstrate the rational design of nanoporous covalent organic frameworks (COFs) as effective gas diffusion layers (GDLs) to address this constraint. The COF GDLs, with a tailor-made pore size of ≈1.4 nm and superhydrophobicity, can limit the intrusion of organic electrolytes and moisture into the gas diffusion channels, enabling high capacity, fast kinetics, and excellent stability of the Li-air batteries. Moreover, we achieve multi-atmosphere Li-air batteries, which can stably cycle under open ambient air (relative humidity up to 95 %) and even in various atmospheres with looping oxygen, humid air, and carbon dioxide. The design principles of our COF GDLs can be universally applied in energy storage and electrochemical systems using organic electrolytes.