High-Resolution Single-Turnover Mapping Reveals Intraparticle Diffusion Limitation in Ti-MCM-41-Catalyzed Epoxidation

Shedding light on catalysis: For the first time, transport phenomena and their influence on catalysis are directly observed for individual catalytic particles by single‐turnover mapping using high‐resolution fluorescence microscopy. The Thiele modulus could be measured with just one experiment, prov...

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Veröffentlicht in:Angewandte Chemie International Edition Jg. 49; H. 5; S. 908 - 911
Hauptverfasser: De Cremer, Gert, Roeffaers, Maarten B.J, Bartholomeeusen, Evelyne, Lin, Kaifeng, Dedecker, Peter, Pescarmona, Paolo P, Jacobs, Pierre A, De Vos, Dirk E, Hofkens, Johan, Sels, Bert F
Format: Journal Article
Sprache:Englisch
Veröffentlicht: Weinheim Wiley-VCH Verlag 25.01.2010
WILEY-VCH Verlag
WILEY‐VCH Verlag
Wiley
Schlagworte:
Boron Compounds - chemistry
Catalysis
Chemistry
Chemistry, Multidisciplinary
Diffusion
epoxidation
Fluorescent Dyes - chemistry
fluorescent probes
heterogeneous catalysis
Microscopy, Fluorescence
Peroxides - chemistry
Physical Sciences
Science & Technology
Silicon Dioxide - chemistry
single-molecule studies
Titanium - chemistry
LOCALIZATION
diffusion
SELECTIVE OXIDATION
heterogeneous catalysis
MOLECULE FLUORESCENCE SPECTROSCOPY
MICROSCOPY
MESOPOROUS MATERIALS
fluorescent probes
single-molecule studies
PROBES
epoxidation
INTRACRYSTALLINE DIFFUSION
TI-MCM-41 NANOPARTICLES
CRYSTALS
CATALYTIC-ACTIVITY
ISSN:1433-7851, 1521-3773, 1521-3773
Online-Zugang:Volltext
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Zusammenfassung:Shedding light on catalysis: For the first time, transport phenomena and their influence on catalysis are directly observed for individual catalytic particles by single‐turnover mapping using high‐resolution fluorescence microscopy. The Thiele modulus could be measured with just one experiment, proving the existence of diffusional limitations for the Ti‐MCM‐41 catalyzed epoxidation of a fluorescent reporter molecule (see picture; TBHP=tert‐butylhydroperoxide).
Bibliographie:http://dx.doi.org/10.1002/anie.200905039
ark:/67375/WNG-5XJB898Q-M
ArticleID:ANIE200905039
FWO (Fonds voor Wetenschappelijk Onderzoek)
G.D.C., P.D., and M.B.J.R. thank the FWO (Fonds voor Wetenschappelijk Onderzoek) for two doctoral fellowships and a postdoctoral fellowship, respectively. This work was performed within the framework of the IAP-VI program "Supramolecular Chemistry and Catalysis" of the Belgian Federal government and of GOA-2/01. We also gratefully acknowledge financial support from a long-term structural funding "Methusalem" by the Flemish government and from K.U. Leuven in the framework of the Centre of Excellence CECAT.
istex:3AE58AE2A4883EC9E0C9B93B831B2201D02C27C7
G.D.C., P.D., and M.B.J.R. thank the FWO (Fonds voor Wetenschappelijk Onderzoek) for two doctoral fellowships and a postdoctoral fellowship, respectively. This work was performed within the framework of the IAP‐VI program “Supramolecular Chemistry and Catalysis” of the Belgian Federal government and of GOA‐2/01. We also gratefully acknowledge financial support from a long‐term structural funding “Methusalem” by the Flemish government and from K.U. Leuven in the framework of the Centre of Excellence CECAT.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.200905039