Harnessing the structural evolution of metal–organic frameworks under electrocatalytic conditions

Abstract Metal–organic frameworks (MOFs) are often dismissed in electrocatalysis due to their structural “instability” under operating conditions. In this Perspective, we reframe MOF evolution in electrocatalytic conditions as a controllable pathway for accessing highly active catalytic species, such as metal (oxy)hydroxides, surface defects, and open metal centers. We highlight how leveraging structural evolution, rather than complete degradation, can be harnessed through rational design and activation strategies. Operando/in-situ techniques are highlighted as essential tools for tracking in-situ structural dynamics and associated evolution mechanisms. By integrating these design, characterization, and modeling insights, this Perspective outlines a framework for turning structural evolution into a powerful tool for catalytic functionality.