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首页> 外文期刊>ACS catalysis >Reaction Design for the Compartmented Combination of Heterogeneous and Enzyme Catalysis
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Reaction Design for the Compartmented Combination of Heterogeneous and Enzyme Catalysis

机译：非均相和酶催化反应的组合反应设计

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摘要

The combination of a heterogeneously catalyzed reaction with a biotransformation as a one-pot cascade process is an important strategy to reduce costs, time, and labor efforts in the production of chemicals from biogenic resources. Although one-pot cascade-type approaches generally result in more efficient chemical processes by reducing the number of workup operations needed and time consumed, the combination of different types of catalysts, both chemical and enzymatic, into a single reaction vessel often remains challenging. During our study, aimed at the direct synthesis of 2-keto-3-deoxy sugar acids as one intermediate toward biobased building blocks starting from the corresponding sugars by combining heterogeneous inorganic catalysis with enzyme catalysis, we encountered several incompatibility problems. These were overcome by a chemoenzymatic method in different compartments, which involves the gold-catalyzed direct oxidation by molecular oxygen and the subsequent conversion of the sugar acids through an enzymatic dehydration step. The described procedure represents an efficient synthesis route toward four different 2-keto-3-deoxy sugar acids and serves as a proof of concept for the combination of one-pot-incompatible catalysts under continuous flow.
机译：将多相催化反应与生物转化作为一锅级联过程相结合，是一种重要的策略，可降低从生物资源生产化学品的成本，时间和劳力。尽管一锅级联方法通常通过减少所需的后处理操作次数和消耗的时间来提高化学过程的效率，但是将不同类型的化学和酶促催化剂组合到单个反应容器中通常仍然具有挑战性。在我们的研究中，旨在通过将异种无机催化与酶催化相结合，从相应的糖开始直接合成2-酮-3-脱氧糖酸作为一种向生物基构件的中间体，我们遇到了一些不相容的问题。通过在不同隔室中进行化学酶促方法克服了这些问题，该方法涉及通过分子氧进行金催化的直接氧化以及随后通过酶促脱水步骤进行糖酸的转化。所述方法代表了向四种不同的2-酮-3-脱氧糖酸的有效合成路线，并且用作在连续流下结合一锅不相容的催化剂的概念证明。

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