单位点多相催化剂及其在烃类选择性氧化中的应用.pptVIP

Single site heterogeneous catalysts and its application in selective oxidation of hydrocarbon 1. Introduction 2. Single site catalysts 3. Application in selective oxidation of hydrocarbon 4. Conclusion and perspective Contents Introduction What is single site ? The single site (catalytically active center) may consist one or more atoms. Such single sites are spatially isolated from one another, there is no spectroscopic or cross-talk between such sites. Each site has the same energy of interaction between it and a reactant as every other single site; and each site is structurally well-characterized, just as the single sites in homogeneous molecular catalysts are. J.M. Thomas, Angew.Chem.Int.Ed.2005, 44, 6456 introduction Homogeneous enzymatic Heterogeneous Single site heterogeneous introduction Introduction Basset.J.M Angew.Chem.Int.Ed.2003,42,156 Single site heterogeneous catalysts Top. Catal. 40 (2006) 3 Why is MAlPO? The ability for small quantities of isolated transition-metal ions(M),such as CoⅡ, MnⅢ and FeⅢ, to be incorporated into the AlPO framework,thereby conferring “redox” catalytic activity at the sites of their incorporation into the resulting MAlPO, microporous Relative ease of preparation Good thermal stability Characterization of FeAlPO M. Dugal, Angew. Chem. Int. Ed. 39 (2000) 2310 R. Raja, J. Am. Chem. Soc. 121 (1999) 11926 In-situ characterization of CoAlPO-18 R. Raja, Angew. Chem. Int. Ed. 39 (2000) 2313 Synthesis of adipic acid N2O or O2 cat. U. Schuchardt, Appl. Catal. A: Gen. 211 (2001) 1 Oxidation of n-hexane in air: catalytic performance and product selectivity J. M. Thomas, Nature, 398 (1999) 227 J. M. Thomas, Nature, 398 (1999) 227 Oxidation of n-hexane in air: Product selectivity J. M. Thomas, Nature, 398 (1999) 227 0.38 X 0.38nm Catalytic performance of CoAlPO for selective oxidation of n-hexane R. Raja, Angew. Chem. Int. Ed. 39 (2000) 2313 Oxidation of n-hexane in air: kinetic plot R. Raja, Angew. Chem. Int. Ed. 39 (2000) 2313 L