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如何设计催化剂
* Towards Total Design of Heterogeneous Catalysts Harold H. Kung Chemical Engineering Department Northwestern University Evanston, IL 60208-3120 October 13, 2003 What would one like to accomplish in total catalyst synthesis? Shape of the cavity Path to cavity Ability to design and position ancillary groups Complete atomic control of active site (metal, oxide) Metal Crystallite Catalytic Active Phase Surface arrangement of atoms Composition Nature of support Location of crystallite on support (defect sites) Structure sensitivity Electronic effect Ligand effect Metal clusters derived from metal carbonyl complexes BC Gates J. Molec. Catal. A Chem 163 (2000) 55 Os5C on MgO Ir4 in zeolite Size-selective cluster beam deposition of Aun clusters on MgO Heiz, Sanchez, Abbet, Schneider, Chem. Phys. 262 (2000) 189. MS signal of C16O18O in TPD after exposure to 18O2 and then CO Aaron S. Eppler, Günther Rupprechter, László Guczi, and Gabor A. Somorjai, J. Phys. Chem. B 101 (1997) 9973. Array of Pt on silica Deposition of metal clusters using lithography Insufficient control of shape, exact size, and atom locations; current limit on smallest size achieved. P-SO32- + Mn+(aq) → P-SO32-Mn+ P-SO32-Mn+ + NaBH4 → P-SO32-/Mo Preparation of uniform sized metal particles using functional resins Corain, Centomo, Ferrari Meyer-Zaika, Schmid, Gold2003, October 2003. Control of surface coordinative unsaturation sites of aluminum oxide (Al2O3) by synthesis Active sites are surface exposed Al ions (Lewis acid sites). Al O Al O O Al O O O Active site Al Al OR OR RO RO R O O R NRH2 H2O O H2RN Al Al O O O H2RN Strategy: use amine (Lewis base) to preserve Lewis acidity. Al OR NRH2 RO RO 2 monomer Can make monomer Amine protection is retained Final solid an active catalyst Kozlov, Kung, Xue, and Kung, Angew. Chem. Int. Ed. 42(2003) 2415 Conversion of cyclopentene oxide in reaction with piperidine catalyzed by various aluminas. ● PPD-Al2O3, ? SG-Al2O3-200, ○ SG-Al2O3-500-H2O-200, ▲
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