ABSTRACT Introducing magnetic interactions into electrocatalyst development enables modulation of spin states and provides a pathway to accelerate water‐splitting kinetics. In this study, a RuNP/ZIF‐67 nanocatalyst is synthesized by immobilizing ruthenium nanoparticles onto the zeolitic imidazolate framework‐67 (ZIF‐67), which facilitates interfacial charge transfer and significantly alters the cobalt divalent to trivalent cation ratio compared to pristine ZIF‐67. Such modulation in oxidation states modifies the electronic configuration of cobalt centers to enhance spin‐spin coupling and induce ferromagnetism in the electrocatalyst. Stabilization of Ru nanoparticles enables synergistic tuning of the electronic and magnetic properties, directly contributing to enhanced catalytic activity. Under a 240 mT magnetic field, RuNP/ZIF‐67 reduces the hydrogen evolution reaction (HER) overpotential from 68 to 51 mV and the oxygen evolution reaction (OER) overpotential from 210 to 182 mV, resulting in a decrease in overall cell voltage from 1.56 to 1.53 V. Control experiments using a rotating disk electrode (RDE) distinguish the spin‐polarized contribution, while long‐term chronopotentiometry and pulse‐chronoamperometry confirm stable magneto‐electrochemical performance. In situ operando studies provide mechanistic insights into the reaction pathway, supporting the observed catalytic performance and stability of RuNP/ZIF‐67. Together, these findings establish RuNP/ZIF‐67 as a robust bifunctional electrocatalyst for magnetically enhanced water splitting.
Biswal et al. (Sun,) studied this question.