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, JasonScott
• 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: 2015
• 资助国家: 加拿大
• 起止时间: 2015-01-01 至 2016-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=588367
• 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度，但在过程中本身并不被消耗。它们的工作原理是通过增加步骤为反应提供一种替代途径，所有这些步骤都比非催化反应快，并最终再次再生催化剂。在所有规模的重要工业反应中，有很大一部分使用催化剂；它们经常使原本不可能发生的转化成为可能；它们使反应更清洁、更快；它们产生的废物显著减少(它们的“原子经济性”，即最终形成产品的起始材料中原子的比例通常非常高)。现代催化剂通常是非常有效的，极少量的催化剂可以产生大量的产品。虽然这种效率无疑是一件好事，但它也带来了一个问题--当只有少量混合物令人感兴趣时，我们如何研究相关条件下的催化反应？ 我们开发了一种新的方法来研究催化反应，使用的技术主要是研究蛋白质等大生物分子的科学家的专利：电喷雾电离质谱仪(ESI-MS)。我们将用它来研究催化中的困难问题，用它来检测中间体的同一性和丰度，同时使用能够检测溶液中丰富的物种(主要是原料和产品的数量)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打开了机会。虽然许多其他研究小组都被类似的问题所吸引，但我们的方法将为我们提供相当大的竞争优势：通过使用一套工具来测量主要组分(反应物、产品，通常是摩尔浓度)，同时使用ESI-MS探测次要组分(催化中间体、静止状态，通常是毫摩尔浓度到微摩尔浓度)，我们将能够在六个数量级或更大的动态范围内运行。通过这样做，我们将对反应进行的方式获得前所未有的洞察，我们将利用我们的理解合理地改进催化剂，并开发更清洁、更快、更高效地转化化学品的新方法。