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Accessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light.(Report)

Enzymes are ideal for use in asymmetric catalysis by the chemical industry, because their chemical compositions can be tailored to a specific substrate and selectivity pattern while providing efficiencies and selectivities that surpass those of classical synthetic methods. However, enzymes are limit... Full description

Journal Title: Nature Dec 15, 2016, Vol.540(7633), p.414(4)
Main Author: Emmanuel, Megan A.
Other Authors: Greenberg, Norman R. , Oblinsky, Daniel G. , Hyster, Todd K.
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: ISSN: 0028-0836 ; DOI: 10.1038/nature20569
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recordid: gale_ofa473942052
title: Accessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light.(Report)
format: Article
creator:
  • Emmanuel, Megan A.
  • Greenberg, Norman R.
  • Oblinsky, Daniel G.
  • Hyster, Todd K.
subjects:
  • Catalysis – Innovations
  • Nuclear Excitation – Research
  • Radiation Exposure – Observations
ispartof: Nature, Dec 15, 2016, Vol.540(7633), p.414(4)
description: Enzymes are ideal for use in asymmetric catalysis by the chemical industry, because their chemical compositions can be tailored to a specific substrate and selectivity pattern while providing efficiencies and selectivities that surpass those of classical synthetic methods. However, enzymes are limited to reactions that are found in nature and, as such, facilitate fewer types of transformation than do other forms of catalysis. Thus, a longstanding challenge in the field of biologically mediated catalysis has been to develop enzymes with new catalytic functions. Here we describe a method for achieving catalytic promiscuity that uses the photoexcited state of nicotinamide co-factors (molecules that assist enzyme-mediated catalysis). Under irradiation with visible light, the nicotinamidedependent enzyme known as ketoreductase can be transformed from a carbonyl reductase into an initiator of radical species and a chiral source of hydrogen atoms. We demonstrate this new reactivity through a highly...
language: eng
source:
identifier: ISSN: 0028-0836 ; DOI: 10.1038/nature20569
fulltext: fulltext
issn:
  • 0028-0836
  • 00280836
url: Link


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titleAccessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light.(Report)
creatorEmmanuel, Megan A. ; Greenberg, Norman R. ; Oblinsky, Daniel G. ; Hyster, Todd K.
ispartofNature, Dec 15, 2016, Vol.540(7633), p.414(4)
identifierISSN: 0028-0836 ; DOI: 10.1038/nature20569
subjectCatalysis – Innovations ; Nuclear Excitation – Research ; Radiation Exposure – Observations
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descriptionEnzymes are ideal for use in asymmetric catalysis by the chemical industry, because their chemical compositions can be tailored to a specific substrate and selectivity pattern while providing efficiencies and selectivities that surpass those of classical synthetic methods. However, enzymes are limited to reactions that are found in nature and, as such, facilitate fewer types of transformation than do other forms of catalysis. Thus, a longstanding challenge in the field of biologically mediated catalysis has been to develop enzymes with new catalytic functions. Here we describe a method for achieving catalytic promiscuity that uses the photoexcited state of nicotinamide co-factors (molecules that assist enzyme-mediated catalysis). Under irradiation with visible light, the nicotinamidedependent enzyme known as ketoreductase can be transformed from a carbonyl reductase into an initiator of radical species and a chiral source of hydrogen atoms. We demonstrate this new reactivity through a highly...
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