Bio-ethanol Upgrading Catalysed by Multifunctional Zeolites

多功能沸石催化生物乙醇升级

• 批准号: 2716951
• 金额: --
• 依托单位: Durham University
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2022
• 资助国家: 英国
• 起止时间: 2022 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2716951
• 关键词: Bio; ethanol; Upgrading; Catalysed; Multifunctional

Since 2015, global production of bioethanol from biomass-based feedstocks has exceeded 25 billion gallons per year. The negative environmental impacts derived from the chemical industry's dependence on fossil fuels means that there is an ever-increasing pressure to utilise renewable alternatives. Consequently, the upgrading of bioethanol into higher value chemicals and fuels is of great interest in both academia and industry. Bioethanol is predominantly used as a drop-in renewable fuel additive to gasoline. Unfortunately, bioethanol is corrosive to most engines and so only low levels (10%) can be added to gasoline without suitable engine modification. Additionally, bioethanol has a lower energy density (70%) than gasoline and is water miscible, potentially causing problems with separation and dilution in storage tanks. Contrastingly, biobutanol, derived from bioethanol, is a much better renewable additive for gasoline engines; it has 90% the energy density of gasoline, is non-corrosive and has limited miscibility with water so it can be blended at higher concentrations, or even be used as a stand-alone biofuel. Currently, precious metal based, catalysts are typically utilised for the conversion of ethanol to butanol. These catalysts however are unsustainable for industrial manufacture of biobutanol, and their production and disposal are considered both environmentally and economically problematic. Development of effective catalysts from earth abundant, non-toxic materials would therefore overcome a major barrier in the commercialisation of this process. Zeolites are microporous aluminosilicate materials used as sustainable catalysts in a range of industrial processes such as catalytic cracking. Their highly stable, cage-like structure allows for shape-selective catalysis, and they can be structurally modified to accommodate numerous different active sites, resulting in an ability to catalyse multistep reaction process.Recent work in the Taylor group at Durham University has shown that zinc oxide (ZnO) supported on zeolites gives rise to very stable ethanol dehydrogenation catalysts (over 120 hours), which is the first step in the ethanol to butanol reaction cascade. This project aims to modify these ZnO/Zeolite catalysts further, with additional active sites to complete the full ethanol to butanol cascade pathway. This will include earth abundant, extra framework metal sites, as well as framework Lewis acid sites. The project will determine how the nature and location of the differing catalytic components affects overall catalytic function, which will provide structure function models for future catalyst design. The location of the different catalytic functionalities will be controlled via a variety of different synthetic approaches. The multistep conversion of ethanol to butanol will be explored using flow reactors coupled with online analysis, and mechanistic pathways will be probed by in-situ infrared spectroscopy.This project spans multiple EPSRC research areas including bioenergy, catalysis, chemical reaction dynamics and mechanisms, and functional ceramics and inorganics. The research falls under the themes of Energy and Manufacturing the Future, with the primary goal being development of catalysts for biofuel production.

自2015年以来，全球每年以生物质为原料生产的生物乙醇已超过250亿加仑。化学工业对化石燃料的依赖对环境产生了负面影响，这意味着利用可再生能源的压力越来越大。因此，将生物乙醇升级为更高价值的化学品和燃料是学术界和工业界的极大兴趣。生物乙醇主要用作汽油的可再生燃料添加剂。不幸的是，生物乙醇对大多数发动机都有腐蚀性，所以如果不对发动机进行适当的改造，只能在汽油中添加低含量（10%）的生物乙醇。此外，生物乙醇的能量密度比汽油低（70%），并且与水混溶，这可能会导致储罐中分离和稀释的问题。相比之下，从生物乙醇中提取的生物丁醇是一种更好的汽油发动机可再生添加剂；它的能量密度是汽油的90%，无腐蚀性，与水的混溶性有限，因此它可以在更高的浓度下混合，甚至可以作为独立的生物燃料使用。目前，贵金属催化剂通常用于将乙醇转化为丁醇。然而，这些催化剂对于生物丁醇的工业生产是不可持续的，它们的生产和处置被认为是环境和经济上的问题。因此，从地球上丰富的、无毒的材料中开发有效的催化剂将克服这一过程商业化的一个主要障碍。沸石是一种微孔铝硅酸盐材料，在催化裂化等一系列工业过程中用作可持续催化剂。它们高度稳定的笼状结构允许形状选择性催化，并且它们可以进行结构修改以适应许多不同的活性位点，从而能够催化多步反应过程。杜伦大学泰勒小组最近的研究表明，在沸石上负载氧化锌（ZnO）可以产生非常稳定的乙醇脱氢催化剂（超过120小时），这是乙醇到丁醇反应级联的第一步。本项目旨在进一步修饰这些ZnO/沸石催化剂，增加活性位点以完成乙醇到丁醇的全级联途径。这将包括地球丰富，额外的框架金属站点，以及框架刘易斯酸站点。该项目将确定不同催化组分的性质和位置如何影响整体催化功能，这将为未来催化剂设计提供结构功能模型。不同的催化功能的位置将通过各种不同的合成方法来控制。利用流动反应器与在线分析相结合的方法，探索乙醇多步转化为丁醇的过程，并利用原位红外光谱技术探索其机理。该项目涵盖了EPSRC的多个研究领域，包括生物能源、催化、化学反应动力学和机理、功能陶瓷和无机物。这项研究属于未来能源和制造业的主题，主要目标是开发生物燃料生产的催化剂。