CAREER: Characterizing Electrochemical and Photocatalytic Reaction Pathways via Nanostructured-Photoelectrodes

在这个由化学系化学测量和成像计划资助的项目中，莱斯大学的Isabell Thomann教授正在开发新的仪器，以跟踪通常复杂的、多步骤的多相光催化反应路径，这些反应路径与太阳能燃料发电、环境修复和一般的化学合成有关。飞秒时间分辨拉曼技术将被用来探测短寿命反应中间产物的化学特性。此外，还将通过电化学质谱学和核磁共振对反应产物进行相应的分析。利用这些技术，将研究高效二氧化碳光还原的新概念。等离子体光电极和介电光电极纳米结构都有潜力开辟独特的反应途径，克服有限的转化效率和产物选择性。在这项工作中获得的光催化反应的基础知识将有助于提高二氧化碳还原的选择性和效率。此外，这里开发的技术能力还将用于招聘、教育和培训高度跨学科研究领域的学生(包括本科生和研究生)。作为该奖项的一部分，正在制定一项外展计划，其中包括让K12教师和本科生有机会在托曼教授的实验室了解这项研究并为其做出贡献。

In this project funded by the Chemical Measurement and Imaging Program of the Chemistry Division, Professor Isabell Thomann of Rice University is developing novel instrumentation to follow the often complex, multi-step reaction pathways of heterogeneous photocatalytic reactions that are relevant for solar fuel generation, environmental remediation, and chemical synthesis in general. Femtosecond time-resolved Raman techniques will be developed to probe the chemical identities of short-lived reaction intermediates. These will be complemented by concomitant analyses of the reaction products via electrochemical mass spectrometry and nuclear magnetic resonance. Using these techniques, novel concepts for efficient carbon dioxide photoreduction will be investigated. Both plasmonic and dielectric photoelectrode nanostructures will be explored for their potential to open up distinctive reaction pathways and to overcome limited conversion efficiencies and product selectivities.The fundamental knowledge about photocatalytic reactions gained in this work will, among many other applications, aid in improving the selectivity and efficiency of CO2 reduction. The technological capabilities developed here will in addition serve to recruit, educate and train students (both undergraduate and graduate) in a highly interdisciplinary research field. As part of this award, an outreach program is being developed that includes opportunities for K12 teachers and undergraduates to learn about and contribute to this research in the Professor Thomann's lab.