非均相催化剂的设计美国西北大学ppt课件.PPT
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1、Towards Total Design of Heterogeneous Catalysts,Harold H. Kung Chemical Engineering Department Northwestern University Evanston, IL 60208-3120,October 13, 2003,Metal Crystallite Catalytic Active Phase,Surface arrangement of atoms Composition Nature of support Location of crystallite on support (defe
2、ct 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. 26
3、2 (2000) 189.,MS signal of C16O18O in TPD after exposure to 18O2 and then CO,Aaron S. Eppler, Gnther Rupprechter, Lszl 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 a
4、tom 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 s
5、ites of aluminum oxide (Al2O3) by synthesis,NRH2,H2O,Strategy: use amine (Lewis base) to preserve Lewis acidity.,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
6、with piperidine catalyzed by various aluminas. PPD-Al2O3, SG-Al2O3-200, SG-Al2O3-500-H2O-200, SG-Al2O3-500-H2O, PA-Al2O3-500-H2O-200 PA-Al2O3-500-H2O, blank.,Xue, Kung, Kozlov, Popp, and Kung, Catal. Today, 2003.,Generation of active site by building on a well-defined structure,001203c,J.M. Thomas,
7、et al. Nature 398 (1999) 227; Angew. Chem. Int. Ed. 39 (2000) 2310.,Two Co(III) ions in CoAlPO-18 at the desired distance apart in Co/P = 0.1 samples. CoAlPO-36 of larger pore structure and shape, produces much more 3-ol and 3-one.,Importance in controlling relative location of sites,29Si NMR of (Si
8、-O)n oligomer units,Atom-by-Atom Synthesis of Metal-Oxygen Chain,Chang, Kung, and Kung, Chem. Comm. submittted.,Metal-Oxygen Backbone of Designed Sequence and Structure,Molecules diffuse through silica wall into and out of cavity.,Preparing sites with predetermined spacing,Dufaud and Davis, JACS 125
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