Journal
SCIENCE
Volume 350, Issue 6265, Pages 1235-1238Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aad3087
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Funding
- Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
- NIH National Institute of General Medical Sciences [R01 GM073932]
- NSF Graduate Research Fellowship Program (GRFP) [DGE 1106400]
- ARCS Foundation
- NSF GRFP
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A self-assembled supramolecular complex is reported to catalyze alkyl-alkyl reductive elimination from high-valent transition metal complexes [such as gold(III) and platinum(IV)], the central bond-forming elementary step in many catalytic processes. The catalytic microenvironment of the supramolecular assembly acts as a functional enzyme mimic, applying the concepts of enzymatic catalysis to a reactivity manifold not represented in biology. Kinetic experiments delineate a Michaelis-Menten-type mechanism, with measured rate accelerations (k(cat)/k(uncat)) upto 1.9x10(7) (here k(cat) and k(uncat) are the Michaelis-Menten enzymatic rate constant and observed uncatalyzed rate constant, respectively). This modality has further been incorporated into a dual catalytic cross-coupling reaction, which requires both the supramolecular microenvironment catalyst and the transition metal catalyst operating in concert to achieve efficient turnover.
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