Control of Stereoselectivity in Heterogeneous Catalysis by Functionalization of Pt Nanoparticles with alpha-Amino Acids
Veröffentlichungsdatum
2019-06-14
Autoren
Betreuer
Gutachter
Zusammenfassung
The asymmetric hydrogenation of ß-keto esters over amino acid-functionalized Pt nanoparticles (NPs) was explored. The investigated catalysts are chemoselective and stereoselective due to specific ligand-reactant interactions between ligands and reactants. Based on structure-selectivity relationships, the previously for L-proline-functionalized Pt NPs suggested ligand-reactant interaction model could be validated, extended to other amino acid ligands, and further refined. Nonlinear effect analysis revealed that in most cases the stereoselectivity is determined mainly by a 1:1 ligand-reactant interaction. Adjusting the interactions between ligands and reactants allowed to improve the stereoselectivity up to an enantiomeric excess over 80%. Most amino acid ligands not only induce selectivity but also enhance the reaction rate. The results of a systematic kinetic study provided an important contribution to the understanding of the reaction mechanism.
Schlagwörter
Ligand-functionalized nanoparticles
;
ligand-reactant interactions
;
nonlinear effects
;
stereoselective heterogeneous catalysis
;
asymmetric hydrogenation
;
ligand acceleration effect
;
reaction kinetics
Institution
Fachbereich
Dokumenttyp
Dissertation
Zweitveröffentlichung
Nein
Sprache
Englisch
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00107467-1.pdf
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4.77 MB
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Adobe PDF
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