Towards an understanding of the surface photocatalytic decomposition of H2O: Electronic structure and femtosecond electron dynamics

了解 H2O 的表面光催化分解：电子结构和飞秒电子动力学

• 批准号: 5261112
• 负责人: Professor Dr. Martin Wolf
• 金额: --
• 依托单位: Lehrstuhl für Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2000
• 资助国家: 德国
• 起止时间: 1999-12-31 至 2002-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/5261112?language=en
• 关键词: Towards; understanding; surface; photocatalytic; decomposition

This project aims towards a fundamental understanding of the photostimulated decomposition of water adsorbed on ruthenium and Ru-oxide surfaces, which is of key relevance for development of renewable energy sources by conversion of water to hydrogen using sunlight. In collaboration with the groups in Leiden, Cambridge and London we will use femtosecond time-resolved spectroscopic techniques and theoretical modeling to investigate the dynamics and mechanism of this process. In particular, we will focus on the electronic structure and the charge transfer dynamics of both the bare surface and the water/substrate interface. Our goal is to identify the relevant energy levels that initiate the photocatalytic decomposition of water and characterize the excited lifetimes and the competing electron relaxation dynamics at the adsorbate-substrate interface. The complexity of the surface will be varied in a controlled and systematic way using of water adsorbed on a single crystal Ru(001) surface, on a fully oxygen-covered (1x1)O/Ru(001) surface and on thin Ru-oxide layers as well as co-adsorbed alkali atoms. As experimental techniques we will use ultraviolet photoelectron spectroscopy (UPS) and femtosecond time-resolved two-photoemission (2PPE), which allows to study both the energetics and the dynamics of the excited state.

该项目旨在从根本上了解钌和钌氧化物表面吸附水的光刺激分解，这对于利用阳光将水转化为氢气来开发可再生能源具有重要意义。我们将与莱顿、剑桥和伦敦的研究小组合作，利用飞秒时间分辨光谱技术和理论建模来研究这一过程的动力学和机制。特别是，我们将重点关注裸露表面和水/基底界面的电子结构和电荷转移动力学。我们的目标是确定引发水光催化分解的相关能级，并表征吸附物-基质界面处的激发寿命和竞争电子弛豫动力学。利用吸附在单晶 Ru(001) 表面、完全氧覆盖的 (1x1)O/Ru(001) 表面、薄 Ru 氧化物层以及共吸附碱原子上的水，表面的复杂性将以受控和系统的方式变化。作为实验技术，我们将使用紫外光电子能谱（UPS）和飞秒时间分辨双光电子发射（2PPE），它可以研究激发态的能量学和动力学。