ACS Catalysis · 2024 · 40 citations · 53 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistryReaction EngineeringBiofuel ProductionCatalyst DesignCatalytic MaterialsCatalytic MechanismsCatalytic Reaction EngineeringSupported CatalystsBimetallic CatalysisC - C Coupling CatalysisC-c Coupling CatalysisConversion RatesCopper-catalyzed CouplingElectrocatalystsElectron DensityHydrogenation
Electrochemically driven carbon–carbon coupling utilizing renewable electricity under ambient conditions has emerged as an innovative approach for synthesizing high-value chemicals, which still faces inherent challenges such as low conversion rates and poor selectivity. While electroreducing furfural to hydrofuroin can produce high-quality biofuel, its efficiency need to be promoted. Herein, Cu–Sn bimetallic catalyst has been developed with a conversion rate of furfural of >97% and hydrofuroin selectivity of >67% through equilibrium of the interfacial intermediate *H and * fur -CHOH, which exhibits the greatest state-of-the-art overall performance. Characterization and theoretical calculation reveal that Cu serves as the active site for generating * fur -CHOH, whose electron density can be decreased by introducing Sn, and results in a higher * fur -CHOH coverage and a lower energy barrier of dimerization. Moreover, adding Sn also enables sluggish *H formation to balance interfacial * fur -CHOH and *H, leading to reduced hydrogenation byproducts. The as-developed approach provides valuable insights for optimizing other C–C electrocoupling reactions for the synthesis of high-value chemicals.
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Generalized Gradient Approximation Made Simple
John P. Perdew, Kieron Burke, Matthias Ernzerhof · Physical Review Letters · 1996 · 211.5K citations · Full text
Natural Sciences, Chemistry, Physics +16