Journal of the American Chemical Society · 2016 · 292 citations · 25 references
Natural SciencesChemistryMaterials ScienceCatalysisCrystal StructureInorganic ChemistryCatalyst DesignCatalyst PreparationCatalyst SynthesisCatalytic MaterialsCatalytic MechanismsCatalytic Reaction EngineeringActivation EnergyAmmonia SynthesisAmmonia Synthesis CatalysisCatalyst Promoter DesignCatalytic ActivityCatalytic Activity EnhancementDirect SynthesisElectron-donating Groups
We report an air and water stable electride Y5Si3 and its catalytic activity for direct ammonia synthesis. It crystallizes in the Mn5Si3-type structure and confines 0.79/f.u. anionic electrons in the quasi-one-dimensional holes. These anionic electrons strongly hybridize with yttrium 4d electrons, giving rise to improved chemical stability. The ammonia synthesis rate using Ru(7.8 wt %)-loaded Y5Si3 was as high as 1.9 mmol/g/h under 0.1 MPa and at 400 °C with activation energy of ∼50 kJ/mol. Its strong electron-donating ability to Ru metal of Y5Si3 is considered to enhance nitrogen dissociation and reduce the activation energy of ammonia synthesis reaction. Catalytic activity was not suppressed even after Y5Si3, once dipped into water, was used as the catalyst promoter. These findings provide novel insights into the design of simple catalysts for ammonia synthesis.
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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
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