Understanding and Harnessing Enzymes for Organosilicon Chemistry

了解和利用酶进行有机硅化学

• 批准号: 2284910
• 金额: --
• 依托单位: University of Manchester
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2019
• 资助国家: 英国
• 起止时间: 2019 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2284910
• 关键词: Understanding; Harnessing; Enzymes; Organosilicon; Chemistry

In synthetic chemistry, there has been increasing prominence in the use of engineered enzymes to execute chemical transformations. These biocatalysts are attractive since they offer highly efficient synthesis in terms of yields and selectivity; together with an inherent environmental sustainability. However, one area where biocatalysis has been relatively unexplored is in silicon-containing (organosilicon) chemistry. Such organosilicon compounds are present in a huge variety of consumer products and play a major role in organic synthesis. Furthermore, such compounds exhibit desirable physical properties that are difficult to achieve by other materials. Marine sponges use silicon (in the form of silica) as part of their inorganic skeleton and utilise an enzyme termed "silicatein" to polymerise silicic acid (H4SiO4) into silica. This family of enzymes are uniquely interesting as they catalyse a reaction that is rare in living systems, the formation of Si-O bonds. Recently, work by the supervisory team has shown that silicatein is also able to catalyse the hydrolysis and condensation (i.e. bond forming and bond breaking) with organosiloxanes, opening the possibility of using this enzyme to facilitate the synthesis of advanced organic-inorganic hybrid materials. This research therefore proposes to exploit the silicateins through rational modification of their structure and apply them to the development of new synthetic reactions. The goals of this project will be two-fold: (i) to improve our understanding of the enzymes' molecular mechanism; and (ii) develop new biocatalysts for organosilicon chemistry with wide scope yet high selectivity. Together this research will contribute to the application of enzyme catalysts in industrial biotechnology

在合成化学中，使用工程化酶来执行化学转化已经越来越突出。这些生物催化剂是有吸引力的，因为它们在产率和选择性方面提供了高效的合成;以及固有的环境可持续性。然而，生物催化的一个相对未开发的领域是含硅（有机硅）化学。这种有机硅化合物存在于各种各样的消费品中，并在有机合成中发挥重要作用。此外，这样的化合物表现出通过其它材料难以实现的期望的物理性质。 海绵使用硅（以二氧化硅的形式）作为其无机骨架的一部分，并利用一种称为“silicatein”的酶将硅酸（H4 SiO 4）聚合成二氧化硅。这个家族的酶是独特的有趣，因为它们催化的反应是在生命系统中罕见的，Si-O键的形成。最近，监督团队的工作表明，silicatein还能够催化有机硅氧烷的水解和缩合（即键形成和键断裂），从而打开了使用这种酶促进先进的有机-无机杂化材料合成的可能性。因此，本研究建议通过对其结构的合理修饰来开发硅质，并将其应用于新的合成反应的开发。该项目的目标有两个方面：（i）提高我们对酶分子机制的理解;（ii）开发具有宽范围但高选择性的新型有机硅化学生物催化剂。这些研究将有助于酶催化剂在工业生物技术中的应用