Dissertation
Insights into the mechanism of electrocatalytic CO2 reduction and concomitant catalyst degradation pathways
This work describes several studies into the electroreduction of carbon dioxide (CO2RR), both regarding mechanistical aspects and catalyst stability considerations. Mechanistic insights into carbon-carbon bond formation on a silver catalyst are described in Ch 2, were we find an acetaldehyde-like surface adsorbate to be a key intermediate.
- Author
- Raaijman, S.J.
- Date
- 19 January 2022
- Links
- Thesis in Leiden Repository
This work describes several studies into the electroreduction of carbon dioxide (CO2RR), both regarding mechanistical aspects and catalyst stability considerations. Mechanistic insights into carbon-carbon bond formation on a silver catalyst are described in Ch 2, were we find an acetaldehyde-like surface adsorbate to be a key intermediate. Gold stability in alkaline environment under strongly reducing conditions and the effect of near-surface CO on said stability is reported on in Ch 3, showing catalyst degradation under reductive conditions which is furthermore exacerbated by CO adsorption. Chapter 4 details the voltammetric behavior of variously oriented copper surfaces when prepared via a non-standard methodology, showing good agreement with prior literature. The last chapter (Ch 5) contains investigations into the stability of copper under reductive conditions in near-neutral buffered electrolyte and in alkaline electrolyte, where it was observed that copper is morphologically stable under strongly alkaline conditions and neutral conditions in the presence of CO2 and buffer ions, so long as strictly reducing potentials are applied.