Self-Activation and Dynamic Surface Reconstruction of Metal–Organic Frameworks Enable Durable Oxygen Evolution Reaction

Abstract Metal–organic frameworks (MOFs) have emerged as prospective oxygen evolution reaction (OER) electrodes, yet their activity is contingent upon irreversible reconstruction into metal oxyhydroxides (MOOH), resulting in structural degradation and compromising long-term durability. Here, we report a self-supported Co-BPM/NF electrode (BPM = 4,4′-dihydroxybiphenyl-3,3′-dicarboxylic acid) that undergoes self-activation and dynamic surface reconstruction during OER. In situ spectroscopic investigations combined with electrochemical analysis reveal dynamic transformation between the initial MOF skeleton and the surface CoOOH active phase under operating potentials. This dynamic surface reconstruction accelerates charge-transfer kinetics while preserving structural integrity. The resulting electrode delivers 100 mA cm–2 at an overpotential of 387 mV while maintaining stable operation for 300 h and 4000 cycles. This work proposes self-activation combined with dynamic surface reconstruction as a strategy to achieve durable MOF electrocatalysts.