Catalytic transfer hydrogenation of bio-based feedstocks to valuable chemicals and fuels

英国致力于严格的碳预算承诺，要求到2050年实现能源系统的完全脱碳。人们普遍预计，低碳液体燃料将成为英国中期脱碳努力（2025-2040年）的关键组成部分，而从长远来看（2040-2050年），将需要部署具有碳捕获和储存的生物能源，以满足英国和全球净负碳承诺。因此，发展低碳液体燃料是英国未来低碳能源体系的关键，生物质是生产可再生有机化学品的唯一可持续原料。可以从木质纤维素生物质生产的最令人感兴趣的化学品之一是γ-戊内酯（GVL）。GVL可以与汽油共混高达10%，并且是柴油和喷气燃料范围内的液体烷烃的前体，以及一些有用的化学品，其作为生态友好溶剂和聚合物生产中的应用。目前，从生物质衍生的原料生产GVL的方法基于级联方法，从木质纤维素生物质和糖生产的分馏开始。随后，糖将经历酸催化转化为乙酰丙酸，然后使用H2气体将乙酰丙酸催化氢化为GVL。然而，该方法具有一些显著的缺点，例如用于乙酰丙酸氢化步骤的昂贵的金属催化剂（例如Ru或Pt）的应用以及高压H2（大于30巴），其可对工艺安全性、可持续性和经济性具有巨大的负面影响。该催化转移氢化（CTH）过程可以通过廉价的金属（如Zr或Ni）催化，使氢从氢供体转移到目标分子。通过实验方法，本项目将开发一种新的能源效率和成本效益高的催化工艺，用于以醇为氢源从生物基原料生产GVL。新的和商业上相关的固体催化剂将通过严格的自下而上的方法来开发催化剂设计，合成，表征和测试

The UK is committed to stringent carbon budget commitments requiring complete decarbonisation of the energy system by 2050. It is generally expected that low carbon liquid fuels will form a key component of the UK's mid-term decarbonisation efforts (2025-2040) and that in the long term (2040-2050) deployment of bioenergy with carbon capture and storage will be required to meet UK and global net negative carbon commitments. Development of low-carbon liquid fuels is therefore essential for the UK future low carbon energy system.Biomass is the only sustainable feedstock to produce renewable organic chemicals. One of the most interesting chemicals that can be produced from lignocellulosic biomass is Y-valerolactone (GVL). GVL can be blended with gasoline up to 10% and is a precursor to liquid alkanes in the diesel and jet fuel range, as well as some useful chemicals with applications as eco-friendly solvents and in polymers production.Currently the process of GVL production from biomass-derived feedstocks is based on a cascade process, starting with the fractionation of lignocellulosic biomass and sugar productions. Subsequently, the sugars will undergo acid catalysed transformation to levulinic acid, followed by noble-metal catalysed hydrogenation of levulinic acid to GVL using H2 gas. However, this approach comes with some significant drawbacks such as the application of expensive metal catalysts (e.g. Ru or Pt) for the levulinic acid hydrogenation step and also high pressure H2 (greater than 30 bar) which can have a huge negative impact on the process safety, sustainability and economics.Alternatively, hydrogenation can be performed using liquid hydrogen donors such as renewable alcohols. This so-called "catalytic transfer hydrogenation" (CTH) process can be catalysed by inexpensive metals (e.g. Zr or Ni), allowing hydrogen transfer from the H-donor to the target molecules.Through experimental methodologies, this project will develop a new energy-efficient and cost-effective catalytic process for GVL production from bio-based feedstocks by utilising alcohols as hydrogen source. New and commercially relevant solid catalysts will be developed through a rigorous bottom-up approach to catalyst design, synthesis, characterisation, and testing