B-SURF: Triggering the energy release from MOST compounds at interfaces – Fundamental mechanisms, kinetics, reversibility

在未来基于MOST的存储技术中，控制能量的随意释放将是必不可少的。该项目将为固/液界面高效、可控的能量释放奠定科学基础。我们将探索催化和电化学触发的途径以及相关的新策略，如电位控制催化过程。我们将侧重于在知识驱动的基础上开发未来能源释放技术所需的基本理解。为此，我们将从研究理想表面科学条件下的能量释放机制开始(工作包1)，并继续进行有势控制和无势控制的固/液界面的现场研究(工作包2和3)。我们将探索理想原子定义的模型界面上的能量释放反应，重点放在三类材料上，即金属系统、氧化物和分子系统。对于每一类，我们将从简单的模型系统开始，依次增加具有纳米结构和孤立位置的界面的复杂性。作为该项目的一个独特功能，我们将在所有环境中使用相同的原子定义的模型接口，从而促进工作包之间的信息传输。该项目将针对三个主要研究问题：(I)触发能量释放的基本化学机制是什么，限制其活性和选择性的关键因素是什么？(Ii)哪些基本材料概念能够使关键材料结合最高的活性、选择性和在延长的运行时间内的稳定性方面具有最高的效率？(Iii)在未来的MOST技术中实现可控性和可切换性以及最高的可逆性、能量密度和太阳能效率的基本操作概念是什么？在每个工作包中，我们将结合两种互补的原位方法，即扫描探针显微镜跟踪界面的原子结构和振动光谱来探索机制、动力学和选择性。通过在表面科学研究和(带电的)液/固界面研究中使用等效方法，我们将能够在这些世界之间传递科学见解。我们的重点将放在先进的光化学现场实验上，我们将在当前最先进的基础上进一步发展。我们的项目将通过提供基本的知识基础来指导分子设计策略，设计催化过程，并在本研究单位的合作项目中在设备中实施新颖的MOST系统，从而在MOST中发挥关键作用。探索定制界面的功能和基本操作原理，该项目将推动未来MOST技术的集成分子/材料概念达到前所未有的效率、稳定性、可逆性和可控性。

In future MOST-based storage technology, it will be essential to control the energy release at will. This project will lay the scientific foundations for efficient and controllable energy release at the solid/liquid interface. We will explore catalytically and electrochemically triggered pathways as well as new interrelated strategies such as potential-controlled catalytic processes. We will focus on the fundamental understanding required to develop future energy release technologies at a knowledge driven basis. To this aim, we will start from studies of the energy release mechanisms under ideal surface science conditions (work package 1) and proceed to in-situ studies of the solid/liquid interface with and without potential control (work packages 2 and 3). We will explore energy release reactions at ideal atomically defined model interfaces, focusing on three materials classes, i.e. metallic systems, oxides, and molecular systems. For each class, we will start from simple model systems and successively increase the complexity towards interfaces featuring nanostructures and isolated sites. As a unique feature of the project, we will use identical atomically defined model interfaces in all environments, thus facilitating the information transfer between the work packages. The project will target three main research questions: (i) What are the fundamental chemical mechanisms of triggered energy release and what are the key factors that limit the activity and selectivity? (ii) What are the fundamental materials concepts that enable highest efficiency in terms of critical materials combined with highest activity, selectivity, and stability over extended operation periods? (iii) What are the fundamental operation concepts to implement controllability and switchability in future MOST technology along with highest reversibility, energy density, and solar efficiency? In each work package, we will combine two complementary types of in-situ methods, i.e. scanning probe microscopy to follow the atomic structure of the interface and vibrational spectroscopy to explore the mechanisms, kinetics, and selectivity. By using equivalent methods in surface science studies and in studies of (electrified) liquid/solid interfaces, we will be able to transfer the scientific insights between these worlds. Our focus will be on advanced photochemical in-situ experiments which we will further develop beyond the current state-of-the-art. Our project will play a key role in FOR MOST by providing the fundamental knowledge basis to guide molecular design strategies, to design catalytic processes, and to implement novel MOST systems in devices within the partner projects of this Research Unit. Exploring the functionality of tailored interfaces and fundamental operation principles, this project will push forward integrated molecular/materials concepts for future MOST technology to unprecedented efficiency, stability, reversibility, and controllability.