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Tuning Pd-nanoparticle@MIL-101(Cr) catalysts for tandem reductive amination

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Date
27/11/2017
Author
Anderson, Amanda E.
Baddeley, Christopher J.
Wright, Paul A.
Keywords
Pd@MIL-101
Tandem reductive amination
Kinetic modelling
QD Chemistry
DAS
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Abstract
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 H2 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 Cr3+ 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.
Citation
Anderson , A E , Baddeley , C J & Wright , P A 2017 , ' Tuning Pd-nanoparticle@MIL-101(Cr) catalysts for tandem reductive amination ' , Catalysis Letters , vol. In press . https://doi.org/10.1007/s10562-017-2208-0
Publication
Catalysis Letters
Status
Peer reviewed
DOI
https://doi.org/10.1007/s10562-017-2208-0
ISSN
1011-372X
Type
Journal article
Rights
© The Author(s) 2017. This article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.
Description
The authors thank the EPSRC (EP/L505079/1), SASOL Technology UK and the University of St Andrews for funding.
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  • University of St Andrews Research
URL
https://link.springer.com/article/10.1007%2Fs10562-017-2208-0#SupplementaryMaterial
URI
http://hdl.handle.net/10023/12204

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