Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.223
Publication date: 23rd September 2021
Catalytic mechanisms at electrode surfaces guide the development of electrochemically-controlled energy storing reactions and chemical synthesis. The intermediate steps of these mechanisms are challenging to identify experimentally, but are critical to understanding the speed, stability, and selectivity of product evolution. In the laboratory group, we employ photo-triggered vibrational and electronic spectroscopy to time-resolve the catalytic cycle at a surface, identifying meta-stable intermediates and critical transition states which connect one to another. The focus is on the highly selective water oxidation reaction at the semiconductor (SrTiO3)-aqueous interface, triggered by an ultrafast light pulse in an electrochemical cell. Here, I will summarize the work done to date by the group: the structure and kinetics of forming the initial intermediates that trap charge (Ti-OH*) through the next event at microseconds, suggested to be the formation of the first O-O bond of O2 evolution. There will be a focus on how time-resolving the intermediates leads to experimental identification of theoretical descriptors of oxygen evolution, one of which is the free energy difference to create the first meta-stable intermediate (DG1(OH*)). In so doing, reaction conditions that shift equilibria become an important, independent axis to the time & energy axes of the spectroscopy. While many open questions remain, these experiments provide and benchmark the opportunity to quantify intermediates at an electrode surface and follow a heterogeneous catalytic cycle in time.
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