Speakers
Description
The industrial and societal transformation towards carbon neutrality requires the development of mitigating strategies to significantly reduce the greenhouse gas emissions. In this framework, CO$_{2}$ electrocatalytic reduction (CO$_{2}$RR) is an elegant and promising approach to convert excess electrical energy and store it in the chemical bonds of multicarbon (C$_{2+}$) products such as alcohols and hydrocarbons using anthropogenic CO$_{2}$.$^{1}$ Cu is up to now the only class of materials which can lead to significant yields of ethanol and ethylene, especially under pulsed CO$_{2}$RR conditions.$^{1-4}$ However, it is crucial to comprehensively understand the (near-surface) structural adaptation as well as the surface coverage with adsorbates under (pulsed) CO$_{2}$RR conditions to allow knowledge-driven catalysts optimization.
In this work, we apply operando time-resolved X-ray diffraction as well as operando surface-enhanced Raman spectroscopy to investigate the active state formation and CO adsorbates under potentiostatic and pulsed CO$_{2}$RR electrochemical conditions. We chose Cu$_{2}$O nanocubes as shape-selected electrocatalysts that can be prepared by a facile, wet-chemical ligand-free approach and show promising catalytic activity.$^{5}$ From our studies, we gain structural insight during initial CO$_{2}$RR conditioning and present how the Cu lattice expands/contracts and the near-surface restructures under oxidizing/reducing conditions. We also gained insight into the link between the surface coverage / binding configuration of the CO and the catalytic function. Furthermore, DFT calculations on the Cu surface strain during selected degrees of charging and adsorbate coverage allowed us to better disentangle the structural influence of electron accumulation and adsorbate coverage.
Thereby, we present fundamental insights to better understand the implications of catalyst structure and (potentiodynamic) CO$_{2+}$RR conditions on the C$_{2+}$ production under industrially-viable conditions.
| Abstract Number (department-wise) | ISC 01 |
|---|---|
| Department | ISC (Roldán) |
