Advanced Functional Materials · 2024 · 36 citations · 50 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistryInorganic ChemistryCatalyst DesignCatalytic MaterialsCatalytic MechanismsRedox CatalysisRedox-active MaterialsSupported CatalystsCatalyst MechanismsCo-catalystsElectrocatalytic ReactorsSingle-atom CatalysisStructured CatalystsTandem CatalysisTandem ReactionsUrea Production
Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) provides an alternative route for realizing efficient and sustainable urea production. In this work, single‐atom Ru dispersed on Co (Ru 1 Co) is demonstrated as an effective and robust catalyst for the UENC. In situ spectroscopic measurements and theoretical simulations unravel the cooperative effect of Ru 1 and Co sites to promote the UENC process via a tandem catalysis mechanism, where the Ru 1 site activates the adsorption and hydrogenation of NO 3 − to form * NH 2 , while the Co site activates the adsorption and hydrogenation/deoxygenation of CO 2 to form * CO. The generated * CO is then transferred from the Co site to the nearby Ru 1 site which promotes the C─N coupling of * NH 2 and * CO toward the urea formation. Strikingly, Ru 1 Co assembled in a flow cell shows the highest urea‐Faradaic efficiency of 50.1% with the corresponding urea yield rate of 22.34 mmol h −1 g −1 at −0.5 V (RHE), superior to most reported UENC catalysts for urea production.
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