Mantel Marvin, Giesler Markus, Guder Marian, Rüthlein Elisabeth, Hartmann Laura, Pietruszka Jörg
Institut für Bioorganische Chemie, Heinrich-Heine-Universität Düsseldorf im Forschungszentrum Jülich, Stetternicher Forst, Geb. 15.8, 52426, Jülich, Germany.
Institut für Organische und Makromolekulare Chemie, Heinrich-Heine-Universität Düsseldorf, 40225, Düsseldorf, Germany.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16700-16706. doi: 10.1002/anie.202103406. Epub 2021 May 1.
Establishing one-pot, multi-step protocols combining different types of catalysts is one important goal for increasing efficiency in modern organic synthesis. In particular, the high potential of biocatalysts still needs to be harvested. Based on an in-depth mechanistic investigation of a new organocatalytic protocol employing two catalysts {1,4-diazabicyclo[2.2.2]octane (DABCO); benzoic acid (BzOH)}, a sequence was established providing starting materials for enzymatic refinement (ene reductase; alcohol dehydrogenase): A gram-scale access to a variety of enantiopure key building blocks for natural product syntheses was enabled utilizing up to six catalytic steps within the same reaction vessel.
建立结合不同类型催化剂的一锅多步反应方案是提高现代有机合成效率的一个重要目标。特别是，生物催化剂的巨大潜力仍有待挖掘。基于对一种使用两种催化剂{1,4-二氮杂双环[2.2.2]辛烷（DABCO）；苯甲酸（BzOH）}的新型有机催化方案的深入机理研究，建立了一个为酶促精制（烯还原酶；醇脱氢酶）提供起始原料的序列：利用同一反应容器内多达六个催化步骤，实现了克级规模地获得用于天然产物合成的各种对映体纯关键构件。
