Engineering the convergence of chemistry and biology: resolving the incompatibility of bio- and chemical catalysis

该项目将开发新的方法，以实现从石化产品到生物（可再生）原料供应链的过渡。挑战在于如何从高度功能化的散装原料、复杂的混合原料和新型副产品中有效地生产合成有用的化学品。生物催化转化将被用来将大量的原料聚合成少量的构建块，用于进一步的合成，利用生物催化剂与化学催化剂相比优异的适应性和选择性。这些积木小分子将进一步利用化学催化有效转化为功能性高价值产品。由于在化学转化之前分离生物产物既不经济又不实际，我们应该开发具有完全集成的生物和化学催化的新型反应系统。由于化学催化剂和生物催化剂在操作条件（温度、盐度、溶剂）以及小分子对许多生物催化剂的毒性方面存在根本的不相容性，目前这种反应体系的例子很少。我们将通过生物和化学催化系统的空间和时间微分离来解决这个问题，使两者在相互兼容的条件下运行，接近两者的最佳条件。这需要设计新的材料和反应器概念，并对催化剂进行修改。这一原理验证项目旨在以整个细胞将葡萄糖和甘油转化为1,3-丙二醇和乳酸为例，演示已开发的概念，然后进行一系列化学转化，产生酯、烯烃、醚、醛等。

This project will develop new approaches to enable the transition from petrochemicals to the bio (renewable) feedstocks supply chain. The challenge is to obtain efficient production of synthetically useful chemicals from highly functionalized bulk feedstock materials, complex mixed feedstocks and new types of by-products. Biocatalytic transformations will be used to converge a large variety of feedstocks into a small number of building blocks for further synthesis, exploiting the excellent adaptability and selectivity of biocatalysts compared with chemical catalysts. These building block small molecules will be further effectively transformed using chemical catalysis into functional high-value products. Since it is not cost effective or practical to separate the biological products prior to chemical transformation, we shall develop novel reaction systems with fully integrated bio- and chemo-catalysis. There are very few examples of such reaction systems at present, due to the fundamental incompatibility between chemo- and biocatalysts in terms of operating conditions (temperature, salinity, solvents), and toxicity of small molecules to many biocatalysts. We shall solve this problem by spatial and temporal micro-separation of bio- and chemocatalytic systems such that both are operated within mutually compatible conditions, approaching the optimal conditions for both. This requires the design of new materials and reactor concepts, and modification of catalysts. This proof-of-principle project aims to demonstrate the developed concepts on the example of conversion of glucose and glycerol to 1,3-propanediol and lactic acid by whole cells, followed by a number of chemical transformations leading to esters, olefins, ethers, aldehydes, inter alia.