Enzyme and reaction engineering of unspecific peroxygenase driven hydroxylation of butane (BUPOx)

非特异性过氧化酶驱动的丁烷羟基化 (BUPOx) 的酶和反应工程

• 批准号: 465474720
• 负责人: Professor Dr.-Ing. Dirk Holtmann
• 金额: --
• 依托单位: Institut für Technische Biokatalyse V-6
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/465474720?language=en
• 关键词: Enzyme; reaction; engineering; unspecific; peroxygenase

This joint proposal of the working groups of Prof. Holtmann and Prof. Liese aims at the profound understanding of the influences and interactions of process parameters on the biocatalytic efficiency of the oxy functionalization of short chain alkanes. On the example of the asymmetric hydroxylation of butane to 2-butanol catalyzed by the recently emerging enzyme group, the unspecific peroxidases (UPO) detailed interdisciplinary process studies are carried out. The feasibility of the reaction system was already demonstrated in common preliminary research by the two groups in first bubble column experiments and at the same time the necessity for more detailed investigations to grasp the observed antagonistic effects. At first a model enzyme, the AaeUPO, will be characterized. Of particular interest is the stability regarding hydrogen peroxide feed rate and gassing effects from gaseous butane feed. To improve relevant selectivities a screening for new UPO variants (enantioselectivity) will be combined with reaction engineering, focusing on in situ product removal by extraction (process selectivity). As UPOs display a broad substrate scope, a “reversed” substrate screening is necessary to find suitable solvents that are not substrates at the same time. Lastly, promising UPO variants will be immobilized on a gas diffusion electrode that is integrated in the reactor. By this means new fundamental knowledge is generated in terms of overcoming limiting factors for hydroxylations catalyzed by UPOs.

Holtmann教授和Liese教授工作组的这一联合提案旨在深入了解工艺参数对短链烷烃氧官能化的生物催化效率的影响和相互作用。以近年来出现的非特异性过氧化物酶（unspecific peroxidases，UPO）催化丁烷不对称羟基化制2-丁醇为例，进行了详细的跨学科过程研究。反应系统的可行性已经在第一鼓泡塔实验的两个小组的共同初步研究中得到了证明，同时有必要进行更详细的研究，以掌握观察到的拮抗作用。首先，将表征模型酶AaeUPO。特别感兴趣的是关于过氧化氢进料速率和气态丁烷进料的产气效应的稳定性。为了提高相关的选择性，新的UPO变体（对映体选择性）的筛选将与反应工程相结合，重点是通过萃取（工艺选择性）原位去除产物。由于UPO显示出广泛的底物范围，因此有必要进行“反向”底物筛选，以找到同时不是底物的合适溶剂。最后，有希望的UPO变体将固定在集成在反应器中的气体扩散电极上。通过这种方法，在克服由UPO催化的羟基化的限制因素方面产生了新的基础知识。