Designer Carbon Nanotube Columns for Chemo- and Bio-Catalytic Synthesis in Flow

用于流动化学和生物催化合成的设计碳纳米管柱

• 批准号: 2404164
• 金额: --
• 依托单位: University of Oxford
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2020
• 资助国家: 英国
• 起止时间: 2020 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2404164
• 关键词: Designer; Carbon; Nanotube; Columns; Chemo

Hydrogenation reactions involve addition of hydrogen gas across a double bond, and account for 10-20% of all industrial chemical steps. However, industrial hydrogenation processes often rely upon precious, heavy metals which may contaminate the final reaction product. Selectivity is also a significant challenge with metal catalysts: hydrogenation may occur in unwanted positions on a complex molecule, certain substituents on the molecule such as halogens may be lost during hydrogenation, and it is very difficult to produce single enantiomer forms of chiral (mirror image) molecules during hydrogenation with metal catalysts. In contrast, enzymes isolated from natural organisms are very good at achieving these same chemical products with exquisite selectivity, and are fully biodegradable and renewable because they are isolated from cells of micro-organisms which are easy to cultivate.Unfortunately, current methods for applying enzymes (biocatalysts) to make hydrogenated chemical products generate a lot of chemical waste which makes the processes less attractive and more costly. This is because the enzymes need expensive cofactors which must be re- charged continually during a reaction. The cofactor re-charging processes are usually powered by sugar (glucose), and most of the glucose molecule goes to waste, and may be burnt at the end of the reaction. To clean up biocatalysis, the Vincent group have developed biocatalytic strategies for driving cofactor re-charging using hydrogen gas, or avoiding the need for cofactors completely. Key themes of this research are the use of hydrogenase enzymes to oxidise dihydrogen selectively, and the use of carbon support materials for hydrogenase immobilisation. This project lies at the interface between Biocatalysis and Materials Science, and focusses on fundamental design principles for carbon materials which are suited to supporting biocatalysts for the generation of amine products.Amines are chemical compounds defined by the presence of an NH2 functional group and are of immense industrial importance in the production of pharmaceuticals, dyes, and plastics, necessitating their production on a massive scale. The project presented herein will probe various designer carbon materials for their ability to support hydrogenases and participate in the selective generation of amine chemical products. A focus will be placed on carbon nanotubes, which are of increasing interest to the scientific community because of their tuneable electronic and chemical properties and will provide a platform for investigating the relationship between fundamental material properties and catalytic efficiency. Through optimisation and scale-up of this biocatalytic hydrogenation system, a greener, selective, and commercially feasible method for generating important amine compounds could be developed, with wide applications in research, industry, and pollutant remediation.This project falls within the EPSRC Physical Sciences - Catalysis Research Area.

加氢反应包括跨双键的氢气加成，占所有工业化学步骤的10%-20%。然而，工业加氢过程往往依赖贵重的重金属，这可能会污染最终的反应产物。金属催化剂的选择性也是一个重大挑战：加氢可能发生在复杂分子上不想要的位置，分子上的某些取代基可能在加氢过程中丢失，以及在金属催化剂加氢过程中很难产生单一对映体形式的手性(镜像)分子。相比之下，从天然生物体中分离出来的酶非常擅长获得同样的化学产品，具有极高的选择性，而且完全可生物降解和可再生，因为它们是从易于培养的微生物细胞中分离出来的。不幸的是，目前应用酶(生物催化剂)来制造氢化化学产品的方法产生了大量的化学废物，这使得这一过程不那么吸引人，成本也更高。这是因为酶需要昂贵的辅因子，而辅因子必须在反应过程中不断充电。辅因子重新充电过程通常由糖(葡萄糖)提供动力，大部分葡萄糖分子被浪费，并可能在反应结束时被燃烧。为了清理生物催化，文森特团队开发了生物催化策略，利用氢气驱动辅因子再充电，或完全避免辅因子的需要。这项研究的主要主题是使用氢酶选择性地氧化双氢，以及使用碳载体材料进行氢酶固定化。该项目位于生物催化和材料科学的交界处，专注于碳材料的基本设计原则，这些材料适合于支持生物催化剂产生胺产品。胺是由NH2官能团定义的化合物，在制药、染料和塑料的生产中具有巨大的工业重要性，需要大规模生产。本文介绍的项目将探索各种设计型碳材料支持氢酶和参与选择性生成胺化工产品的能力。重点将放在碳纳米管上，它因其可调的电子和化学性质而引起科学界越来越大的兴趣，并将为研究基本材料性质和催化效率之间的关系提供一个平台。通过对生物催化加氢系统的优化和放大，可以开发出一种更绿色、更具选择性和商业可行性的生成重要胺化合物的方法，并在研究、工业和污染物修复方面得到广泛应用。该项目属于EPSRC物理科学-催化研究领域。