Mass spectrometry-led catalyst discovery

质谱主导的催化剂发现

• 批准号: RGPIN-2014-05363
• 负责人: McIndoe, Jason
• 金额: $ 6.12万
• 依托单位: University of Victoria
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2018
• 资助国家: 加拿大
• 起止时间: 2018-01-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=659297
• 关键词: Mass; spectrometry; led; catalyst; discovery

Catalysts increase the rate of chemical reactions, but are not themselves consumed in the process. They work by providing an alternative pathway for reaction through an increased number of steps, all of which are faster than the uncatalyzed reaction and that ultimately regenerate the catalyst again. A huge proportion of industrially-important reactions at all scales use catalysts; they frequently enable transformations that would otherwise be impossible; they make reactions cleaner and faster; and they generate significantly less waste (their "atom economy", or proportion of atoms in starting materials that end up in products, is often very high). Modern catalysts are often extraordinarily effective, with tiny quantities generating enormous amounts of product. While this efficiency is unquestionably a good thing, it also creates a problem - how do we study catalytic reactions under relevant conditions when only a tiny amount of the mixture is interesting?**We have developed novel methodologies to study catalytic reactions using a technique that was principally the preserve of scientists studying large biomolecules such as proteins: electrospray ionization mass spectrometry (ESI-MS). We will use it to study the difficult problems in catalysis by using it to inspect the identity and abundance of intermediates while simultaneously measuring the progress of reactions using complementary methods capable of examining the abundant species in solution (primarily the quantity of starting materials and products). The ability to probe intermediates directly also opens up opportunities for the discovery of new catalysts and new transformations. While numerous other research groups are captivated by similar problems, our approach will give us a considerable competitive advantage: by using one set of tools to measure the major components (reactants, products, typically at molar concentrations) while using ESI-MS to probe the minor components (catalytic intermediates, resting states, typically at milli- to micromolar concentrations), we will be able to operate across six orders of magnitude or more of dynamic range. In doing so, we will obtain unprecedented insight into the way in which reactions proceed, and we will use our understanding to rationally improve catalysts and to develop new ways of transforming chemicals that are cleaner, faster and more efficient.

催化剂增加了化学反应的速率，但本身并没有在过程中被消耗。它们的工作原理是通过增加步骤数量为反应提供替代途径，所有这些步骤都比未催化的反应更快，并且最终再次再生催化剂。在所有规模的工业重要反应中，很大一部分都使用催化剂;它们经常能够实现否则不可能实现的转化;它们使反应更清洁，更快;它们产生的废物显著减少（它们的“原子经济”，或最终形成产品的起始材料中的原子比例通常非常高）。现代催化剂通常非常有效，少量产生大量产物。虽然这种效率无疑是一件好事，但它也产生了一个问题-当只有少量混合物感兴趣时，我们如何在相关条件下研究催化反应？我们已经开发了新的方法来研究催化反应，使用的技术主要是研究大生物分子，如蛋白质的科学家的保留：电喷雾电离质谱（ESI-MS）。我们将使用它来研究催化中的难题，通过使用它来检查中间体的身份和丰度，同时使用能够检查溶液中丰富物种（主要是起始材料和产物的数量）的补充方法来测量反应的进展。直接探测中间体的能力也为发现新的催化剂和新的转化开辟了机会。虽然许多其他研究小组也被类似的问题所吸引，但我们的方法将为我们带来相当大的竞争优势：通过使用一套工具来测量（反应物，产物，通常在摩尔浓度下），同时使用ESI-MS探测次要组分（催化中间体，静止状态，通常在毫摩尔至微摩尔浓度下），我们将能够在六个数量级或更多的动态范围上操作。通过这样做，我们将获得对反应进行方式的前所未有的洞察力，我们将利用我们的理解来合理地改进催化剂，并开发更清洁，更快速和更有效的化学品转化新方法。