Structurally diverse γ‐ and δ‐lactones were efficiently synthesized stereoselectively using an engineered carbonyl reductase from Serratia marcescens (SmCRV4). SmCRV4 exhibited improved activity (up to 500‐fold) and thermostability toward 14 γ‐/δ‐keto acids and esters, compared with the wild‐type enzyme, with 110‐fold enhancement in catalytic efficiency (kcat/Km) toward methyl 4‐oxodecanoate. The preparative synthesis of alkyl and aromatic γ‐ and δ‐lactones with 95 %–>99 % ee and 78 %–90 % yields was demonstrated. The highest space‐time yield, 1175 g L−1 d−1, was achieved for (R)‐γ‐decalactone.
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