Molecular stopwatch measurements of dynamics in catalysts, battery electrolytes and ionic liquids in situ

“清洁增长”和“未来移动”是英国政府产业战略中的两大挑战。这些挑战要求物理科学在分子水平上对催化、电池和燃料电池科学有更好的理解、更好的预测和新颖的想法。在这些领域仍有许多基本但未解决的问题。分子筛催化剂的孔隙中分子是如何反应的？水是如何在催化剂表面反应生成氢和氧的？离子液体中质子传导的机理是什么？在解决这些问题的许多实验方法中，没有一种可以轻易地报告分子运动的最快时间尺度（飞秒），或者在多相催化剂中足够快地启动反应以分离出最早的步骤。该提案概述了UKRI未来领导者奖学金的愿景，通过集中开发和应用新的，尖端的超快红外原位方法来解决催化，离子液体和燃料电池电解质中的这些关键分子动力学问题，从而改变这一现状。提出的实验将揭示所涉及的关键分子的运动和化学转化的最快时间尺度——目前该领域的研究人员无法获得这些信息。这些信息将i)揭示这些复杂分子系统行为的新方面，ii)提供可以指导和验证分子动力学模拟的信息（化学科学家可用的最佳预测工具之一），iii)作为经验比较不同催化剂或电解质行为的有力手段。

'Clean growth' and 'Future of mobility' are two challenges in the UK government's industrial strategy. From these challenges are a call for the physical sciences to respond with a better understanding, better predictions and novel ideas in catalysis, battery and fuel cell science at the molecular level. There are many basic, but unanswered questions remaining in these fields. How do molecules react in the pores of Zeolite Catalysts? How does water react at the surface of catalysts to form Hydrogen and Oxygen? What is the mechanism of proton conduction in ionic liquids? Of the many experimental methods available to address these questions, none can easily report on the fastest timescales of molecular motion (femtoseconds), or initiate a reaction fast enough in a heterogeneous catalyst to separate out the earliest steps. This proposal outlines a vision for a UKRI future leaders fellowship to change this by centering on developing and applying new, cutting edge ultrafast IR methods in-situ to answer these key molecular dynamical questions in catalysis, ionic liquids and fuel cell electrolytes. The experiments proposed will reach out to reveal the fastest timescales of the motions and chemical transformations of the key molecules involved - information currently inaccessible to researchers in the field. This information will i) reveal new aspects of the behaviour of these complex molecular systems, ii) provide information that can guide and verify molecular dynamics simulations (one of the best predictive tools available to chemical scientists) and iii) be used as a powerful means of empirically comparing the behavior of different catalysts or electrolytes.