Tuning Pd-nanoparticle@MIL-101(Cr) catalysts for tandem reductive amination
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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.
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 . DOI: 10.1007/s10562-017-2208-0
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The authors thank the EPSRC (EP/L505079/1), SASOL Technology UK and the University of St Andrews for funding.
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