A supramolecular approach to combining enzymatic and transition metal catalysis.
The ability of supramolecular host-guest complexes to catalyse organic reactions collaboratively with an enzyme is an important goal in the research and discovery of synthetic enzyme mimics. Herein we present a variety of catalytic tandem reactions that employ esterases, lipases or alcohol dehydrogenases and gold(I) or ruthenium(II) complexes encapsulated in a Ga(4)L(6) tetrahedral supramolecular cluster. The host-guest complexes are tolerated well by the enzymes and, in the case of the gold(I) host-guest complex, show improved reactivity relative to the free cationic guest. We propose that supramolecular encapsulation of organometallic complexes prevents their diffusion into the bulk solution, where they can bind amino-acid residues on the proteins and potentially compromise their activity. Our observations underline the advantages of the supramolecular approach and suggest that encapsulation of reactive complexes may provide a general strategy for carrying out classic organic reactions in the presence of biocatalysts.
Division of Chemical Sciences, Lawrence Berkeley National Laboratory, and Department of Chemistry, University of California, Berkeley, California 94720-1460, USA.
Z Jane
ZJ
Wang
Kristen N
KN
Clary
Robert G
RG
Bergman
Kenneth N
KN
Raymond
F Dean
FD
Toste
D000818:Animals; D002384:Catalysis; D004950:Esterases / Q000737:chemistry* / Q000378:metabolism*; D006736:Horses; D006868:Hydrolysis; D007700:Kinetics; D008049:Lipase / Q000737:chemistry / Q000378:metabolism; D008099:Liver / Q000201:enzymology; D008670:Metals / Q000737:chemistry*; D008958:Models, Molecular; D015394:Molecular Structure; D009089:Mucor / Q000201:enzymology; D009942:Organometallic Compounds / Q000737:chemistry; D011817:Rabbits; D013552:Swine
D008670:Metals; D009942:Organometallic Compounds; D004950:Esterases; D008049:Lipase