Porous Liquids for Catalysis

用于催化的多孔液体

• 批准号: 2754360
• 金额: --
• 依托单位: Imperial College London
• 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-2754360
• 关键词: Porous; Liquids; Catalysis

Porous liquids (PLs) are an exciting new class of counterintuitive porous materials that combine the properties of a microporous solid with the mobility of a liquid. Like their solid counterparts, these liquids with holes have the capability to demonstrate gas uptake and release, and guest selectivity. However, unlike solid porous materials, they could also potentially have unique applications, such as the ability to be pumped around a continuous system facilitating guest loading/unloading steps, or being used as a gas-loaded reaction solvent. Despite this potential, the application of PLs in areas other than gas uptake and selectivity has not been investigated. Recently, we reported the formation of high cavity concentration PLs using porous organic cages (POCs) - discrete molecules containing permanent molecular cavities accessible through windows - and demonstrated their ability to exhibit increased uptake of a range of gases (e.g., CO2, CH4, Xe, SF6) over neat liquids (Nature, 2015, 527, 216; Chem. Sci., 2017, 8, 2640, ChemRxiv, 2021, DOI:10.26434/chemrxiv.14719503.v2). In addition, there have been reports of the use of solutions of cages for catalytic CO2 conversion into cyclic carbonates (Sustainable Energy Fuels, 2019, 3, 2567), and as nanoreactors (Chem. Soc. Rev., 2008, 37, 247). These systems differ from PLs, which are defined as having permanently empty pores that are accessible to guests, due to either guests being in competition with the solvent which occupies the cavities or guest binding being driven by a hydrophobic effect. In this project, we will build on these initial reports and explore different ways of applying PLs in the area of catalysis. This includes the use of gas-loaded PLs as a reusable and controllable external gas source in stoichiometric gas reactions, and as a solvent to carry out lower pressure gas reactions by 'simulating' high gas concentrations that are normally only achieved at higher pressures, and as nanoreactors to catalyse small molecule reactions by confinement. Once we have a thorough understanding of these different methodologies, we will then seek to translate this into a high-throughput workflow with the aim of being able to use PLs to rapidly screen a range of catalytic reactions involving the incorporation of a gas as a reagent.

多孔液体(Pls)是一类令人兴奋的新型反直觉多孔材料，它结合了微孔固体的性质和液体的流动性。与固体液体一样，这些带有孔洞的液体能够展示气体的吸收和释放以及客户的选择性。然而，与固体多孔材料不同的是，它们也可能具有独特的应用，例如能够在连续系统中泵送，方便客户装卸步骤，或用作气载反应溶剂。尽管有这种潜力，但除了气体吸收和选择性之外，pls在其他领域的应用还没有得到研究。最近，我们报道了使用多孔有机笼子(POCs)形成高空腔浓度的PL，POC是包含可通过窗口访问的永久性分子空腔的离散分子，并展示了它们在整洁液体上对一系列气体(例如，CO2、CH4、Xe、SF6)的吸收增加的能力(自然，2015,527,216；化学)。科学，2017年，8,2640，化学，2021年，DOI：10.26434/Chemrxiv.14719503.v2)。此外，有报告称，使用笼子溶液将二氧化碳催化转化为环状碳酸盐(可持续能源燃料，2019、3、2567)，并用作纳米反应器(化学。SoC。修订版，2008，37,247)。由于客体与占据空腔的溶剂竞争，或者客体结合由疏水效应驱动，这些系统不同于PLS，后者被定义为具有对客体可接近的永久空孔。在这个项目中，我们将在这些初步报告的基础上，探索在催化领域应用PLS的不同方法。这包括使用载气式pls作为化学计量气体反应中可重复使用和可控制的外部气体源，并作为溶剂通过模拟通常只有在较高压力下才能达到的高气体浓度来执行较低压力的气体反应，以及作为纳米反应器通过限制催化小分子反应。一旦我们对这些不同的方法有了透彻的了解，我们将寻求将其转化为高通量的工作流程，目的是能够使用pls来快速筛选涉及将气体作为试剂的一系列催化反应。