A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides ...A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.展开更多
文摘A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.
