High-Entropy Ultrathin Amorphous Metal–Organic Framework-Stabilized Ru(Mo) Dual-Atom Sites for Water Oxidation

High-entropy metal–organic frameworks (HE-MOFs) offer immense potential in electrocatalysis due to their diverse metallic compositions and high densities of active sites. Integrating bimetallic single-atom catalysts (SACs) with HE-MOFs for enhanced oxygen evolution reaction (OER) performance remains challenging. Here, we stabilize atomically dispersed Ru and Mo in amorphous HE-MOF nanosheets (HE(Ru,Mo)-MOFs) via in situ-formed amorphous high-entropy oxides, elucidating the deprotonation mechanism. Evidence supports the presence of high-density O-bridged Ru and Mo dual-atom sites. The multimetallic composition induces electronic redistribution and balances the oxidation state of metal sites, enhancing intrinsic OER activity. HE(Ru,Mo)-MOFs exhibit low OER overpotentials of 267 mV@10 mA cm–2 and 266 mV@10 mA cm–2 in alkaline freshwater and industrial wastewater, respectively, with exceptional durability surpassing that of commercial RuO2 catalysts. Mechanistic insights reveal that high atomic dispersion facilitates rapid charge transfer and intermediate transformation, promising advanced catalysts for energy conversion.