Journal
ACS CATALYSIS
Volume -, Issue -, Pages 7862-7876Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01654
Keywords
carbon dioxide reduction; heterogeneous electrocatalysts; pyridine catalysts; silver electrocatalyst; electrografting
Categories
Funding
- European Union [85144]
- NWO
- NSERC [RGPIN-2020-04960]
- Canada Research Chair [950-23288]
- FRQNT New Researchers Fund [2021-NC-283234]
- Calcul Quebec
- Compute Canada
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The researchers combined silver and pyridine catalysts through a one-pot and irreversible electrografting process, which resulted in the enhanced conversion of carbon dioxide. By tailoring the pyridine carbon chain length, a higher onset potential was achieved. It was demonstrated that the integration of two different catalytic structures can lead to a cocatalytic effect.
The electrochemical reduction of carbon dioxide (CO2) to value-added materials has received considerable attention. Both bulk transition-metal catalysts and molecular catalysts affixed to conductive noncatalytic solid supports represent a promising approach toward the electroreduction of CO2. Here, we report a combined silver (Ag) and pyridine catalyst through a one-pot and irreversible electrografting process, which demonstrates the enhanced CO2 conversion versus individual counterparts. We find that by tailoring the pyridine carbon chain length, a 200 mV shift in the onset potential is obtainable compared to the bare silver electrode. A 10-fold activity enhancement at -0.7 V vs reversible hydrogen electrode (RHE) is then observed with demonstratable higher partial current densities for CO, indicating that a cocatalytic effect is attainable through the integration of the two different catalytic structures. We extended the performance to a flow cell operating at 150 mA/cm(2), demonstrating the approach's potential for substantial adaptation with various transition metals as supports and electrografted molecular cocatalysts.
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