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Potential Dependent Reorientation Controlling Activity of a Molecular Electrocatalyst
Adrian M Gardner1,2, Gaia Neri1, Bhavin Siritanaratkul1
1Department of Chemistry and Stephenson Institute for Renewable Energy, University of Liverpool, Liverpool L69 7ZD, United Kingdom.
Journal of the American Chemical Society
|March 5, 2024
Summary
A study on CO2 reduction catalysts reveals that N-methyl-2-pyrrolidone (NMP) presence influences molecular electrocatalyst Mo(bpy)(CO)4 orientation. This reorientation enhances CO2 reduction yields at less negative potentials.
Area of Science:
- Electrochemistry
- Materials Science
- Surface Chemistry
Background:
- Molecular electrocatalyst activity is governed by complex interfacial interactions.
- Understanding these interactions is crucial for designing efficient catalysts.
- The role of electrolyte composition and electric fields is often overlooked.
Purpose of the Study:
- To investigate the solvent and potential-dependent activation of a CO2 reduction catalyst, Mo(bpy)(CO)4.
- To elucidate the influence of N-methyl-2-pyrrolidone (NMP) on catalyst behavior at the electrode surface.
- To correlate interfacial changes with catalytic performance for CO2 reduction.
Main Methods:
- Utilized surface-specific vibrational sum frequency generation (VSFG) spectroscopy.
- Studied the catalyst Mo(bpy)(CO)4 at a polycrystalline gold (Au) electrode.
- Varied electrolyte composition (presence of NMP) and applied electrode potential.
Main Results:
- Observed potential-dependent reorientation of the parent Mo(bpy)(CO)4 complex at the Au electrode surface.
- The presence of NMP was found to induce this reorientation.
- This pre-activation by NMP led to increased yields of the active CO2 reduction electrocatalyst.
Conclusions:
- Interfacial solvent effects significantly impact molecular electrocatalyst activation and performance.
- NMP acts as a crucial additive, promoting catalyst reorientation and enhancing CO2 reduction efficiency.
- VSFG spectroscopy is a powerful tool for probing interfacial phenomena in electrocatalysis.
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