Real-time analysis of catalytic reactions

催化剂提高了化学反应的速率，但在反应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另一种途径，所有这些步骤都比未催化的反应快，并最终使催化剂再次再生。工业上各种规模的重要反应中有很大一部分都使用催化剂。它们经常使原本不可能的转化成为可能，它们使反应更清洁、更快，而且它们产生的废物显著减少（它们的“原子经济性”，即最终进入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，少量就能产生大量的产物。虽然这种效率无疑是一件好事，但它也带来了一个问题——当只有少量的混合物是有趣的时，我们如何在相关条件下研究催化反应？我们开发了一种新的方法来研究催化反应，这种技术主要是科学家研究大型生物分子（如蛋白质）的范围：电喷雾电离质谱（ESI-MS）。我们已经将它与其他实时技术结合使用，研究了5个数量级浓度差异的反应动力学。现在，我们将利用机器人技术帮助我们将ESI-MS与传统的离线方法配对，并部署我们的新型离子迁移率质谱仪，通过形状和成分实时表征离子。我们的新三重四极杆仪器通常用于化学家的超痕量分析，将针对其他方法因缺乏灵敏度而无法检测的短寿命中间体。我们将收集的大量数据将需要现代工具来解释，我们计划编写和部署算法，以识别进化反应中最有趣的组件的动态行为特征，并将其标记出来供人类检查。我们将利用现代工具处理大数据，并根据我们独特的应用开发所需的方法。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力。我们将利用我们的认识，合理改进催化剂，开发更清洁、更快、更有效的方式，将化学品增值为更高价值的材料。研究结果将对制造聚合物、燃料、药品、农用化学品和商品化学品的化学家产生影响：任何依赖于催化的合成过程，只要有改进的空间，都将受益于对该过程更详细的了解。

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 methods to study catalytic reactions using a technique that was principally the purview of scientists studying large biomolecules such as proteins: electrospray ionization mass spectrometry (ESI-MS). We have used it in conjunction with other real-time techniques to study the dynamics of reactions across 5 orders of magnitude differences in concentration. Now, we'll use robotics to help us pair ESI-MS with traditional off-line methods, and deploy our new ion mobility mass spectrometer to characterize ions by both shape and composition in real time. Our new triple-quadrupole instrument, typically used by chemists in ultra-trace analyses, will be targeted at short-lived intermediates for which other methods have not been able to detect for lack of sensitivity. The vast amounts of data we will gather will need modern tools for interpretation, and we plan to write and deploy algorithms that will identify dynamic behavior characteristic of the most interesting components of an evolving reaction and flag them for human inspection. We will utilize modern tools for processing big data and will develop methodologies as required for our unique applications. In doing so, we will obtain unprecedented insight into the way in which reactions proceed. We will use our understanding to rationally improve catalysts and to develop cleaner, faster and more efficient ways of adding value to chemicals into higher value materials. The results will have impact on chemists who make polymers, fuels, pharmaceuticals, agrochemicals, commodity chemicals: any synthetic process relying on catalysis that still has room for improvement stands to benefit from a more detailed understanding of that process.