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

Xueqin Mu, Min Yu, Xingyu Liu, Yuru Liao, Fanjiao Chen, Haozhe Pan, Ziyue Chen, Suli Liu, Dingsheng Wang, Shichun Mu

2024ACS Energy Letters66 citationsDOI

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.

Topics & Concepts

Amorphous solidDual (grammatical number)MetalAtom (system on chip)Materials scienceAmorphous metalInorganic chemistryChemical engineeringChemistryNanotechnologyCrystallographyMetallurgyComputer scienceLiteratureEmbedded systemEngineeringArtMetal-Organic Frameworks: Synthesis and ApplicationsElectrocatalysts for Energy ConversionElectrochemical Analysis and Applications
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