Stabilization of 2D Imine‐Linked Covalent Organic Frameworks: From Linkage Chemistry to Interlayer Interaction

Imine‐linked covalent organic frameworks (imine‐COFs) represent the most sought‐after class of COFs due to their broad monomer scope and ease of synthesis. Owing to the reversible nature of imine linkages, however, the chemical stability of most imine‐COFs is still far from adequate. In this context, emerging strategies, ranging from linkage chemistry to interlayer interaction, have been employed to construct stable imine‐COFs for their applications in electronics, sensing, and energy storage devices. This Concept article summarizes the latest advances aimed at tuning the structural stability of imine‐COFs. Furthermore, this Concept provides a prospective for the precise design of stable imine‐COFs based on the characteristics of structure, physical properties, and chemical functions, as well as the mechanism of structure locking and stabilization during crystal growth. Stabilizing methodology: Emerging strategies, such as linkage transformation strategy, bond protection strategy, and interlayer interaction engineering, have recently been developed to regulate the stability of 2D imine‐linked COFs. This provides a facile solution to the instability of imine‐linked COFs while simultaneously conserving their structural crystallinity and functionality.