(Invited) Measuring the Temporal Evolution of Surface Intermediates in Electrocatalysis
Meeting abstracts(2023)
摘要
Ensemble measurements in electrocatalysis average over populations of single entities such as transient chemical intermediates and active sites. Ensemble-averaged empirical data provides general trends in reactivity but lost is a vast amount of information on how molecules interact and evolve on an electrocatalyst surface which could reveal over- or underperforming subpopulations within an ensemble. To validate and improve current theoretical predictions of reaction pathways, direct measurements of intermediates in electrocatalysis are required. Toward this goal, I will discuss our development of time-resolved surface-enhanced Raman scattering (SERS) microscopy as a tool to measure the evolution and dynamics of surface intermediates formed on metallic electrodes in CO 2 reduction. Combining diffraction-limited spatial resolution with µs temporal resolution, we observe the formation of surface-bound CO ca. 1 V below the ensemble onset potential. Further, our time-resolved spectroscopy reveals the timescales of surface intermediate accumulation on and evolution from electrode surfaces, providing insight into the residence times of intermediates. Time-resolved SERS microscopy reveals the action of surface intermediates previously hidden by spatially and temporally averaged ensemble measurements, providing new mechanistic insight to the CO 2 reduction reaction.
更多查看译文
关键词
surface intermediates,temporal evolution
AI 理解论文
溯源树
样例
生成溯源树,研究论文发展脉络
Chat Paper
正在生成论文摘要