CONSPECTUS:Lewis acidic zeolites are microporous crystalline materials that offer promise as catalysts for the activation and conversion of biomassderived precursors in the liquid phase due to their unique water toler...CONSPECTUS:Lewis acidic zeolites are microporous crystalline materials that offer promise as catalysts for the activation and conversion of biomassderived precursors in the liquid phase due to their unique water tolerance and synthetic versatility.The active site environment in zeolite catalysts is multifaceted in nature and is composed of a primary catalytic binding site,the secondary pore structure that confines such binding sites,and occluded solvent and reactant molecules that interact with adsorbed species.Moreover,Lewis acidic heteroatoms can adopt structurally diverse coordination that selectively catalyze different classes of chemical transformations and can be difficult to control synthetically or characterize spectroscopically.Thus,precise mechanistic interpretation of liquid-phase zeolite catalysis necessitates the development of synthetic,spectroscopic,and kinetic methods that can decouple such complex active site structures and probe the interactions that occur between confined active sites,solvent and reactant molecules,and adsorbed intermediates and transition states.展开更多
基金B.A.J.,J.R.D.,and Y.R.-L.thank the U.S.Department of Energy,Office of Basic Energy Sciences under Award DE-SC0016214 for support。
文摘CONSPECTUS:Lewis acidic zeolites are microporous crystalline materials that offer promise as catalysts for the activation and conversion of biomassderived precursors in the liquid phase due to their unique water tolerance and synthetic versatility.The active site environment in zeolite catalysts is multifaceted in nature and is composed of a primary catalytic binding site,the secondary pore structure that confines such binding sites,and occluded solvent and reactant molecules that interact with adsorbed species.Moreover,Lewis acidic heteroatoms can adopt structurally diverse coordination that selectively catalyze different classes of chemical transformations and can be difficult to control synthetically or characterize spectroscopically.Thus,precise mechanistic interpretation of liquid-phase zeolite catalysis necessitates the development of synthetic,spectroscopic,and kinetic methods that can decouple such complex active site structures and probe the interactions that occur between confined active sites,solvent and reactant molecules,and adsorbed intermediates and transition states.