TY - JOUR
T1 - CO2 Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts
AU - Abdinejad, Maryam
AU - Irtem, Erdem
AU - Farzi, Amirhossein
AU - Sassenburg, Mark
AU - Subramanian, Siddhartha
AU - Iglesias Van Montfort, Hugo Pieter
AU - Ripepi, Davide
AU - Li, Mengran
AU - Middelkoop, Joost
AU - Seifitokaldani, Ali
AU - Burdyny, Thomas
PY - 2022
Y1 - 2022
N2 - 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 CO2conversion 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/cm2, demonstrating the approach's potential for substantial adaptation with various transition metals as supports and electrografted molecular cocatalysts.
AB - 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 CO2conversion 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/cm2, demonstrating the approach's potential for substantial adaptation with various transition metals as supports and electrografted molecular cocatalysts.
KW - carbon dioxide reduction
KW - electrografting
KW - heterogeneous electrocatalysts
KW - pyridine catalysts
KW - silver electrocatalyst
UR - http://www.scopus.com/inward/record.url?scp=85134891811&partnerID=8YFLogxK
U2 - 10.1021/acscatal.2c01654
DO - 10.1021/acscatal.2c01654
M3 - Article
AN - SCOPUS:85134891811
SN - 2155-5435
VL - 12
SP - 7862
EP - 7876
JO - ACS Catalysis
JF - ACS Catalysis
IS - 13
ER -