Tuning Pd-nanoparticle@MIL-101(Cr) Catalysts for Tandem Reductive Amination

The versatility of MOFs as highly porous Lewis acidic supports for precious metal nanoparticles has been exploited for one-pot tandem reductive amination catalysis. MIL-101(Cr) loaded with Pd nanoparticles ca. 3 nm in size at 0.2–1 wt% has been used to catalyse the reaction of 4′-fluoroacetophenone...

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Bibliographic Details
Published in:Catalysis letters 2018-01, Vol.148 (1), p.154-163
Main Authors: Anderson, Amanda E., Baddeley, Christopher J., Wright, Paul A.
Format: Article
Language:English
Subjects:
Amines
Analysis
Catalysis
Chemistry
Chemistry and Materials Science
Hydrogenation
Industrial Chemistry/Chemical Engineering
Organometallic Chemistry
Palladium
Palladium catalysts
Physical Chemistry
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Summary:The versatility of MOFs as highly porous Lewis acidic supports for precious metal nanoparticles has been exploited for one-pot tandem reductive amination catalysis. MIL-101(Cr) loaded with Pd nanoparticles ca. 3 nm in size at 0.2–1 wt% has been used to catalyse the reaction of 4′-fluoroacetophenone with benzylamine under 10 bar of H 2 to give the secondary amine, 4′-fluoro-α-methyl- N -phenylmethylbenzenemethanamine. For the highest Pd loading, major hydrogenolysis of the secondary amine occurs in a second tandem reaction, but by changing the ratio of Pd to Lewis acidic Cr 3+ active sites it is possible to tune the catalytic selectivity to the desired 2° amine product. An empirical kinetic analysis was performed to demonstrate this active site complementarity. Graphical Abstract
ISSN:1011-372X
1572-879X
DOI:10.1007/s10562-017-2208-0