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

Abstract

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 RuO 2 catalysts. Mechanistic insights reveal that high atomic dispersion facilitates rapid charge transfer and intermediate transformation, promising advanced catalysts for energy conversion.