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年能源系统完全脱碳。人们普遍预计，低碳液体燃料将成为英国中期(2025-2040年)脱碳努力的关键组成部分，而在长期(2040-2050年)，将需要部署具有碳捕获和封存功能的生物能源，以实现英国和全球的净负碳承诺。因此，开发低碳液体燃料对英国未来的低碳能源系统至关重要。生物质是生产可再生有机化学品的唯一可持续原料。木质纤维生物质可生产的最有趣的化学物质之一是Y-戊内酯(GVL)。GVL可以与汽油混合高达10%，是柴油和喷气燃料范围内液态烷烃的前体，也是一些用作环保溶剂和聚合物生产的有用化学品。目前，从生物质原料中生产GVL的过程是基于级联过程，从木质纤维生物质和糖的生产开始。随后，糖将经过酸催化转化为乙酰丙酸，然后贵金属催化的乙酰丙酸在氢气中加氢为GVL。然而，这种方法也有一些明显的缺点，如使用昂贵的金属催化剂(如Ru或Pt)用于乙酰丙酸加氢步骤，以及高压氢气(大于30bar)，这可能对工艺的安全性、可持续性和经济性产生巨大的负面影响。这一所谓的“催化转移氢化”(CTH)过程可以被廉价的金属(如锆或镍)催化，从而允许氢从供氢体转移到目标分子。通过实验方法，这项计划将开发一种新的能源效率和成本效益高的催化过程，以酒精为氢源，从生物原料中生产GVL。将通过严格的自下而上的催化剂设计、合成、表征和测试方法来开发具有商业意义的新型固体催化剂

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