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1. Spectroscopic evidence for direct flavin-flavin contact in a bifurcating electron transfer flavoprotein

   https://doi.org/10.1074/jbc.RA120.013174  

   Duan, H. Diessel; Mohamed-Raseek, Nishya; Miller, Anne-Frances (September 2020, Journal of Biological Chemistry)

   null (Ed.)
2. Understanding flavin electronic structure and spectra

   https://doi.org/10.1002/wcms.1541  

   Kar, Rajiv K.; Miller, Anne‐Frances; Mroginski, Maria‐Andrea (January 2021, WIREs Computational Molecular Science)

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3. New frontiers in flavin-dependent monooxygenases

   https://doi.org/10.1016/j.abb.2021.108765  

   Reis, Renata A.G.; Li, Hao; Johnson, Maxim; Sobrado, Pablo (March 2021, Archives of Biochemistry and Biophysics)

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4. Role of reduced flavin in dehalogenation reactions

   https://doi.org/10.1016/j.abb.2020.108696  

   Sobrado, Pablo (January 2021, Archives of Biochemistry and Biophysics)

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5. Flavin-dependent halogenases catalyze enantioselective olefin halocyclization

   https://doi.org/10.1038/s41467-021-23503-3  

   Mondal, Dibyendu; Fisher, Brian F.; Jiang, Yuhua; Lewis, Jared C. (December 2021, Nature Communications)

   null (Ed.)

   Abstract Halocyclization of alkenes is a powerful bond-forming tool in synthetic organic chemistry and a key step in natural product biosynthesis, but catalyzing halocyclization with high enantioselectivity remains a challenging task. Identifying suitable enzymes that catalyze enantioselective halocyclization of simple olefins would therefore have significant synthetic value. Flavin-dependent halogenases (FDHs) catalyze halogenation of arene and enol(ate) substrates. Herein, we reveal that FDHs engineered to catalyze site-selective aromatic halogenation also catalyze non-native bromolactonization of olefins with high enantioselectivity and near-native catalytic proficiency. Highly selective halocyclization is achieved by characterizing and mitigating the release of HOBr from the FDH active site using a combination of reaction optimization and protein engineering. The structural origins of improvements imparted by mutations responsible for the emergence of halocyclase activity are discussed. This expansion of FDH catalytic activity presages the development of a wide range of biocatalytic halogenation reactions. 

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