Sustainability By Advanced Chemoenzymatic Technologies

大自然利用经过数百万年优化的反应序列，以高度可持续的方式产生立体选择性化合物。该项目的主要目的是开发一种多步反应，以仿生的方式合成具有高对映选择性和非对映选择性的产品，从简单的构建块开始，如烯烃和二烯。作为反应序列的第一步，使用均溶大分子催化剂，即所谓的“化学酶”。在自然界中，一层膜保留了这种人工催化剂。有机产物流被传递到第二个反应器，没有进一步的净化，在那里立体选择性氢氰化是由羟基腈裂解酶催化的。酶或化学酶将催化可能的第三个转化步骤，导致具有手性侧链的功能化环己烯基。这种类型的结构很难通过其他方法以立体控制的方式获得，并将为药物和农用化学品的应用提供新的手性构建块。这些修改步骤也将被整合到整个生产过程中。这种先进的化学酶技术能够从像烯和二烯这样的简单材料开始，可持续地合成大量高度非对映选择性的产品。多步合成将在连续流反应器中进行。通过这种设置，工作协议将被最小化。全面的可持续合成是可能的，因为整合了原位产物去除，有机相的再循环以及化学酶和酶的再循环。这项先进技术的高效开发是由涵盖技术化学、聚合物化学、化学和分子/结构生物学领域的研究团队的专业知识保证的。

Nature uses reaction sequences optimized over millions of years to produce stereoselective compounds in a highly sustainable way. The major aim of this project is to develop a multi-step reaction in a biomimetic way for the synthesis of products with a high enantio- and diastereoselectivity, starting from simple building blocks, such as an alken and a diene. As first step of the reaction sequence a homogeneously soluble macromolecular catalyst, a so-called "chemzyme", is applied. A membrane, as in nature, retains this artificial catalyst. The organic product stream is passed on to a second reactor without further purification, where a stereoselective hydrocyanation is catalyzed by a hydroxynitrile lyase. Enzymes or chemzymes will catalyze a possible third transformation step leading to functionalized cyclohexenyl with chiral sidechains. This type of structure is difficult to access by other methods in a stereocontrolled fashion and will provide new chiral building blocks for application in drugs and agrochemicals. These modification steps will also be integrated in the whole production process. This advanced chemoenzymatic technology enables the sustainable synthesis of a vast spectrum of highly diastereoselective products starting from simple materials like an alken and a diene. The multi-step synthesis will be carried out in a continuous flow reactor. By this setup the work-up protocols will be minimized. An overall sustainable synthesis is possible because of the integration of in situ product removal, recycling of the organic phase as well as recycling of the chemzymes and the enzymes. The efficient development of this advanced technology is assured by the expertise of the research teams covering the areas of technical chemistry, polymer chemistry, chemistry, and molecular/structural biology.