Phospholipid-Bioinspired Hydrogen-Bonded Organic Frameworks for Ultrahigh Proton Conductivity

Abstract

Achieving ultrahigh proton conductivities coupled with excellent performance durability through the biomimetic engineering of hydrogen-bonded organic frameworks (HOFs) remains a critical challenge in solid-state electrolyte research. Herein, inspired by phospholipids and charge-assisted hydrogen bonds, we developed bioinspired ZSTU-88 and ZSTU-99 via rational molecular self-assembly design. The ZSTU-88 (ZSTU-88: C₁₇H₂₄FN₃O₁₁P₂) and ZSTU-99 (ZSTU-99: C₁₆H₂₄FN₃O₁₁P₂) exhibit ultrahigh proton conductivities of 4.64 × 10^–1 S cm^–1 and 2.48 × 10^–1 S cm^–1, respectively, at 98% relative humidity and 70 °C due to the formation of extensive hydrogen-bonding networks constructed by protonated amines, dihydrogen phosphate ions, and phosphoric acid molecules. Notably, they demonstrate remarkable durability with no degradation in performance for at least 300 h. This work establishes a new paradigm for designing durable, high-performance HOF electrolytes.