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Engineering a Non–Natural Photoenzyme for Improved Photon Efficiency

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [2];  [2];  [3];  [2];  [3]
  1. Cornell Univ., Ithaca, NY (United States); Princeton Univ., NJ (United States); Cornell University
  2. Princeton Univ., NJ (United States)
  3. Cornell Univ., Ithaca, NY (United States)
We developed a novel HTS engineering platform to optimize photoenzymatic activity. The improvements in variants were correlated to an increase in enzymatic photon efficiency. Here, transient absorption spectroscopy revealed a shift from a stepwise to a concerted mechanism. The platform was expanded to improve the synthesis of γ, δ, ϵ-lactams, and acyclic amides.
Research Organization:
Cornell Univ., Ithaca, NY (United States); Princeton Univ., NJ (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0019370
OSTI ID:
1843580
Alternate ID(s):
OSTI ID: 1833900
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 2 Vol. 61; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (31)

Directed Evolution of an Enantioselective Enoate-Reductase: Testing the Utility of Iterative Saturation Mutagenesis journal December 2009
Photoenzymatic Approaches in Organic Synthesis journal August 2019
Light‐Driven Kinetic Resolution of α‐Functionalized Carboxylic Acids Enabled by an Engineered Fatty Acid Photodecarboxylase journal June 2019
Directed Evolution of Enzymes for Industrial Biocatalysis journal December 2015
Revealing Additional Stereocomplementary Pairs of Old Yellow Enzymes by Rational Transfer of Engineered Residues journal March 2017
Tailoring Multipurpose Biocatalysts via Protein Engineering Approaches: A Review journal May 2019
Directed evolution for enzyme development in biocatalysis journal April 2021
The Evolution of Chemical High-Throughput Experimentation To Address Challenging Problems in Pharmaceutical Synthesis journal November 2017
Ultrafast Vibrational Energy Transfer between Protein and Cofactor in a Flavoenzyme journal June 2020
Active-Site Environmental Factors Customize the Photophysics of Photoenzymatic Old Yellow Enzymes journal November 2020
Photochemical Mechanism of Light-Driven Fatty Acid Photodecarboxylase journal May 2020
Discovery, Characterization, Engineering, and Applications of Ene-Reductases for Industrial Biocatalysis journal March 2018
Photo-Biocatalysis: Biotransformations in the Presence of Light journal April 2019
Deconvolution of Luminescence Cross-Talk in High-Throughput Gene Expression Profiling journal May 2019
Residues Controlling Facial Selectivity in an Alkene Reductase and Semirational Alterations to Create Stereocomplementary Variants journal June 2014
Site-Saturation Mutagenesis of Tryptophan 116 of Saccharomyces pastorianus Old Yellow Enzyme Uncovers Stereocomplementary Variants journal March 2009
Photoenzymatic Generation of Unstabilized Alkyl Radicals: An Asymmetric Reductive Cyclization journal August 2020
Quaternary Charge-Transfer Complex Enables Photoenzymatic Intermolecular Hydroalkylation of Olefins journal December 2020
General Strategy for Improving the Quantum Efficiency of Photoredox Hydroamidation Catalysis journal October 2018
One-Pot Biocatalytic Cascade Reduction of Cyclic Enimines for the Preparation of Diastereomerically Enriched N -Heterocycles journal November 2019
Accessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light journal December 2016
The molecular origin of high DNA-repair efficiency by photolyase journal June 2015
Photoenzymatic enantioselective intermolecular radical hydroalkylation journal June 2020
Engineering new catalytic activities in enzymes journal January 2020
Activation modes in biocatalytic radical cyclization reactions journal March 2021
An algal photoenzyme converts fatty acids to hydrocarbons journal August 2017
Photoexcitation of flavoenzymes enables a stereoselective radical cyclization journal June 2019
Mechanism and dynamics of fatty acid photodecarboxylase journal April 2021
Time- and frequency-resolved fluorescence with a single TCSPC detector via a Fourier-transform approach journal January 2018
A General Framework for Thermodynamically Consistent Parameterization and Efficient Sampling of Enzymatic Reactions journal April 2015
Minimization of between-well sample variance of antifungal activity using a high-throughput screening microplate bioassay journal February 2007