Catalytic conversion of biomass derived molecules over metal organic frameworks for the sustainable and renewable production of chemicals and fuels

生物质衍生分子在金属有机框架上的催化转化，用于化学品和燃料的可持续和可再生生产

• 批准号: 1917327
• 金额: --
• 依托单位: University of Warwick
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2017
• 资助国家: 英国
• 起止时间: 2017 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-1917327
• 关键词: Catalytic; conversion; biomass; derived; molecules

Catalytic synthesis of value-added chemicals from renewable biomass or biomass-derived platform chemicals is an important way to reduce current dependence on fossil-fuel resources and reduce the carbon footprint of chemical industry. In this regard, heterogeneously catalysed reactions will play a major role in the processing of the platform molecules to valuable chemicals, biofuel and biopolymer precursors by means of aqueous-phase processing and environmentally sound methodologies. A simple and efficient process for conversion to useful chemicals and fuels offers significant potential to deliver economic, environmental and societal impact. New catalysts need to be developed and their role in these catalytic processes need be fully understood in order to develop more economical processing routes competitive enough to replace the current crude oil based industrial production processes. The aim of this project is to devise and develop new catalytic architectures with desired functional chemical groups. In this project we will follow a novel bottom up approach for catalyst development; we will examine the required catalytic reaction, and design and develop novel chemical architectures with desired functional groups. Our particular focus will be on the oxidation reactions in biomass conversion. Catalytic oxidation of biomass can lead to multiple products, and the challenge is to direct the reaction pathways to the desired products. Biomass derived compounds, such as 5-hydroxymethylfurfural (HMF) has hydroxyl groups and their oxidation lead to the formation of carboxylic acids; an important precursor to replace the PET (Polyethylene terephthalate) plastics. The aqueous phase conversion of biomass compounds into valuable organic acids can be achieved, but a step change is required to broaden the scope of this chemistry and improve product yield. The current processes work in dilute solutions, require high catalyst loadings and employ high alkaline conditions. Our novel bottom up approach will identify the transition metal cations and coordinate them in well-defined high crystalline metal organic frameworks to oxidise the biomass-derived compounds into their organic acid counterparts. Developing stable metal organic frameworks with oxidation and reduction (redox) capability in aqueous phase is an unexplored chemistry. We will combine fundamental science with engineering studies in an integrated approach, to develop a detailed fundamental understanding of the catalytic chemistry that is practical and easily applicable. Experimental studies will deliver fundamental understanding of new catalysts and processes and a detailed fundamental understanding of the chemistry will support development of improved technology. The experimental approach will build on our experience and expertise of design of catalysts with controlled composition, morphology and structure. Detailed catalyst characterisation, both ex situ and in situ, will provide essential information on catalyst structure and chemical properties. The catalytic results will feedback to the material synthesis in an iterative fashion to optimise and fine-tune the materials properties for an efficient process. Final stage in the project will be the economic analysis for a scale up of the process from laboratory to industrial application. This project is in line with the EPSRC theme of Physical sciences and the research area of Catalysis.

利用可再生生物质或生物质衍生平台化学品催化合成高附加值化学品是降低当前对化石燃料资源依赖、减少化学工业碳足迹的重要途径。在这方面，多相催化反应将在通过水相处理和无害环境方法将平台分子加工成有价值的化学品、生物燃料和生物聚合物前体方面发挥重要作用。一个简单而有效的转化为有用的化学品和燃料的过程具有巨大的潜力，可以产生经济、环境和社会影响。需要开发新的催化剂，并且需要充分理解它们在这些催化过程中的作用，以便开发更经济的加工路线，其具有足够的竞争力以取代当前基于原油的工业生产过程。该项目的目的是设计和开发具有所需功能化学基团的新催化结构。在这个项目中，我们将遵循一种新的自下而上的催化剂开发方法;我们将研究所需的催化反应，并设计和开发具有所需官能团的新型化学结构。我们将特别关注生物质转化中的氧化反应。生物质的催化氧化可产生多种产物，挑战在于将反应途径引导至所需产物。生物质衍生的化合物，如5-羟甲基糠醛（HMF）具有羟基，它们的氧化导致羧酸的形成;取代PET（聚对苯二甲酸乙二醇酯）塑料的重要前体。可以实现生物质化合物到有价值的有机酸的水相转化，但是需要步骤改变以拓宽该化学的范围并提高产物产率。目前的方法在稀溶液中工作，需要高催化剂负载量并采用高碱性条件。我们的新的自下而上的方法将确定过渡金属阳离子，并将它们协调在定义明确的高结晶金属有机框架中，以将生物质衍生的化合物氧化成它们的有机酸对应物。在水相中开发具有氧化和还原（氧化还原）能力的稳定金属有机框架是一种未探索的化学。我们将联合收割机基础科学与工程研究相结合，以综合的方法，开发一个详细的催化化学的基本理解，是实用的，易于应用。实验研究将提供对新催化剂和工艺的基本理解，对化学的详细基本理解将支持改进技术的开发。实验方法将建立在我们的经验和专业知识的催化剂设计与控制的组成，形态和结构。详细的催化剂表征（非原位和原位）将提供有关催化剂结构和化学性质的重要信息。催化结果将以迭代的方式反馈到材料合成中，以优化和微调材料性能，从而实现高效的工艺。该项目的最后阶段将是对从实验室到工业应用的工艺规模进行经济分析。该项目符合EPSRC的物理科学主题和催化研究领域。