Light Sparks for Plasmonic Catalysis: Colloidal-Based Cavities as Molecular Magnifying Glasses for Reactions on Pd

催化是一个真正的纳米级的过程，了解潜在的机制是未来发展的关键（光）催化剂。最近对结构化催化剂的推动，下至原子尺度，旨在实现重要的经济和生态目标。将等离子体纳米粒子用于催化是一个生动的研究领域，因为光限制可以在适度条件下决定反应路径，速率和选择性。在FLATCat等离子体激元项目中，我将开发基于等离子体激元的原子光学腔，从根本上研究它们的基础物理并利用它们的特性。通过将使用欠电位电化学沉积的2D原子平坦材料的无配体沉积与分子和等离子体纳米颗粒的高度限定的自下而上的自组装相结合，将在大面积上实现稳健的钯/金纳米腔。我的目标是使用这些（子）纳米级腔的快速拉曼振动散射作为分子放大镜的极端限制，暂时研究在单个原子的水平上由等离子体激元增强的化学反应。实现这一点将有力地使真正的纳米级等离子体催化剂的更系统的发展成为可能。我计划在剑桥大学的杰里米·鲍姆伯格教授的实验室里实现所提出的项目。他的跨学科小组一直处于纳米光子学研究的最前沿，特别是在物理和化学中率先使用等离子体腔。因此，它是实现该项目的理想和独特的位置。我将学习先进的纳米粒子的合成，原子钯的精确定位和时间和空间分辨的纳米表征需要遵循在原子尺度上的催化。该项目将使我获得经验，研究和领导技能，以及独立成功所需的强大的国际网络。

Catalysis is a truly nanoscale processes-understanding underlying mechanisms is key for the future development of (photo)catalysts. The recent push towards structuring catalysts, down to the atomic-scale, aims for vital economic and ecological goals. Incorporating plasmonic nanoparticles into catalysis is a vivid field of research, as the light confinement can dictate reaction paths, rates, and selectivity at modest conditions. In the FLATCat Plasmon project, I will develop bimetallic atomic optical cavities based on plasmonics to fundamentally study their underlying physics and exploit their properties in photocatalysis. Robust palladium/gold nanocavities will be achieved over large areas by combining ligand-free deposition of 2D atomic flatland materials using underpotential electrochemical deposition, with highly-defined, bottom-up self-assembly of molecules and plasmonic nanoparticles. I aim to use the extreme confinement of light inside these (sub)nanoscopic cavities for fast Raman vibrational scattering as molecular magnifying glasses to temporally study chemical reactions enhanced by plasmonic photocatalysis at the level of individual atoms. Achieving this will strongly enable a more systematic development of plasmonic catalysts at the true nanoscale. I plan to realize the proposed project in the lab of Prof Jeremy Baumberg at the University of Cambridge. His interdisciplinary group has been at the forefront of research in nanophotonics and, in particular, has been pioneering the use of plasmonic cavities in physics and chemistry. Therefore, it is the ideal and unique location to realise this project. I will learn synthesis of advanced nanoparticles, the precise positioning of atomic palladium and the time- and spatially resolved nanocharacterization required to follow catalysis at the atomic scale. The project will allow me gain the experience, research and leadership skills, as well as a robust international network that are needed to succeed independently.