TY - JOUR
T1 - Asymmetric photoenzymatic incorporation of fluorinated motifs into olefins
AU - Li, Maolin
AU - Yuan, Yujie
AU - Harrison, Wesley
AU - Zhang, Zhengyi
AU - Zhao, Huimin
PY - 2024/7/26
Y1 - 2024/7/26
N2 - Enzymes capable of assimilating fluorinated feedstocks are scarce. This situation poses a challenge for the biosynthesis of fluorinated compounds used in pharmaceuticals, agrochemicals, and materials. We developed a photoenzymatic hydrofluoroalkylation that integrates fluorinated motifs into olefins. The photoinduced promiscuity of flavin-dependent ene-reductases enables the generation of carbon-centered radicals from iodinated fluoroalkanes, which are directed by the photoenzyme to engage enantioselectively with olefins. This approach facilitates stereocontrol through interaction between a singular fluorinated unit and the enzyme, securing high enantioselectivity at β, γ, or δ positions of fluorinated groups through enzymatic hydrogen atom transfer-a process that is notably challenging with conventional chemocatalysis. This work advances enzymatic strategies for integrating fluorinated chemical feedstocks and opens avenues for asymmetric synthesis of fluorinated compounds.
AB - Enzymes capable of assimilating fluorinated feedstocks are scarce. This situation poses a challenge for the biosynthesis of fluorinated compounds used in pharmaceuticals, agrochemicals, and materials. We developed a photoenzymatic hydrofluoroalkylation that integrates fluorinated motifs into olefins. The photoinduced promiscuity of flavin-dependent ene-reductases enables the generation of carbon-centered radicals from iodinated fluoroalkanes, which are directed by the photoenzyme to engage enantioselectively with olefins. This approach facilitates stereocontrol through interaction between a singular fluorinated unit and the enzyme, securing high enantioselectivity at β, γ, or δ positions of fluorinated groups through enzymatic hydrogen atom transfer-a process that is notably challenging with conventional chemocatalysis. This work advances enzymatic strategies for integrating fluorinated chemical feedstocks and opens avenues for asymmetric synthesis of fluorinated compounds.
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UR - http://www.scopus.com/inward/citedby.url?scp=85199670428&partnerID=8YFLogxK
U2 - 10.1126/science.adk8464
DO - 10.1126/science.adk8464
M3 - Article
C2 - 39052813
AN - SCOPUS:85199670428
SN - 0036-8075
VL - 385
SP - 416
EP - 421
JO - Science (New York, N.Y.)
JF - Science (New York, N.Y.)
IS - 6707
ER -