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Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical
Sander D de Vos1, Maartje Otten1, Tim Wissink2
1Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The, Netherlands.
This study compares cobalt catalysts for hydrogen evolution. The novel [Co(HBMIMPh2 )2 ](BF4 )2 catalyst showed strong performance, indicating molecular design influences electrocatalytic activity.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Molecular cobalt complexes are promising for electrocatalytic hydrogen evolution.
- Understanding the relationship between molecular structure and catalytic deposit formation is crucial for optimizing performance.
Purpose of the Study:
- To investigate the electrocatalytic hydrogen evolution reaction (HER) performance of [Co(HBMIMPh2 )2 ](BF4 )2 (1).
- To benchmark catalyst 1 against other molecular cobalt HER electrocatalysts.
- To analyze the composition and properties of electrode deposits formed during electrolysis.
Main Methods:
- Voltammetry and controlled potential/current electrolysis (CPE/CCE) in DMF.
- In-line product detection setup for electrolysis.
- X-ray photoelectron spectroscopy (XPS) for deposit analysis.
- Electrode deposit rinse tests.
Main Results:
- Catalyst 1 demonstrated competitive H2 evolution during CPE and superior overpotential and Faradaic efficiency during CCE compared to benchmarks.
- Electrolysis of all cobalt complexes resulted in electrode deposits.
- XPS analysis of deposits from catalyst 1 showed minimal cobalt content, primarily Co2+.
- Rinse tests indicated that the catalytic activity of deposits from catalysts 1 and 2 was partly retained.
Conclusions:
- The molecular design of cobalt complexes significantly influences the characteristics of the electrocatalytic deposit.
- These deposit features, in turn, dictate the observed hydrogen evolution activity.
- Catalyst 1 represents a promising molecular design for efficient electrocatalytic hydrogen production.
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