Optimal Addition Profiles to Control Reactivity and Selectivity of Catalytic Reactions

化学反应的最终结果取决于几个参数，如温度，溶剂以及反应物和催化剂的浓度。通过改变初始反应条件来常规筛选这些参数以获得最佳反应结果。然而，这些参数中的一些，例如反应物和活性催化剂的浓度，在反应过程中发生变化。因此，这些浓度的最佳值也在反应过程中变化。我们可以通过在反应过程中连续添加反应物和催化剂来校正反应物和催化剂的浓度。不幸的是，寻找每次反应的最佳添加速率比寻找反应开始时的最佳浓度要复杂得多。该项目将阐明三种不同类型的至关重要的催化反应的最佳试剂添加速率。我们计划通过应用不同的策略来做到这一点，然后这些策略可能最终应用于其他反应。其中一些策略将使用从机理研究中获得的知识来确定最影响反应最终结果的浓度及其最佳值。在可能的情况下，我们将使用现代原位反应监测工具的信息来即时调节添加速率，这将使我们能够非常快速地找到最佳添加速率。对于更具挑战性的反应，我们提出了一种更保守的方法，通过截面分析反应的行为。这种近似方法比较费力，需要大量的实验，但它可以普遍应用于任何反应，而不管其内在的复杂性。每个反应的最后阶段研究的目的是分析在大规模反应中使用最佳加成曲线的可能性。为了实现这一目标，我们将测试最佳添加曲线对不同参数（如添加速度的准确性、反应规模或搅拌速度）的稳定性。最终，该项目将把学术界开发的不适合工业用途的尖端催化工艺转化为生产药物和先进材料等产品的有用工艺。

The final outcome of a chemical reaction depends on several parameters such as the temperature, the solvent and the concentration of reactants and catalyst. These parameters are routinely screened by modifying the initial reaction conditions to obtain the best outcome of the reaction. However, some of these parameters, for example the concentration of reactants and active catalyst, change during the course of the reaction. Thus, the optimal values for these concentrations also change during the course of the reaction. We can correct the concentration of reactants and catalysts by adding them continuously during the reaction. Unfortunately, finding the optimal rate of addition for each time of the reaction is much more complicated than finding the optimal concentration at the beginning of the reaction.This project will elucidate the best rate of addition of reagents for three different kinds of crucially important catalytic reactions. We plan to do this by applying different strategies, which then may be ultimately applied to other reactions. Some of these strategies will use the knowledge derived from mechanistic studies to identify the concentrations that most affect the final result of the reaction and their optimal values. When possible, we will use the information of modern in situ reaction monitoring tools to instantaneously modulate the rate of addition, which will allow us to find the best rate of addition very quickly. For more challenging reactions, we have proposed a more conservative approach that analyses the behaviour of the reaction by sections. This approximation is more laborious and requires a larger number of experiments, but it can be generally applied to any reaction regardless of its intrinsic complications.The final stage of study for each reaction aims to analyse the possibility of using the best addition profiles on large scale reactions. To do this, we will test how robust are the optimal addition profiles to the variation of different parameters such as the accuracy in the rate of the addition, the scale of the reaction or the stirring rate.Ultimately, this project will convert cutting-edge catalytic processes developed in academia, which are unfit for industrial purposes, to useful processes for the manufacture of products such as pharmaceuticals and advanced materials.