Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 15, Issue 41, Pages 48179-48184Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.3c10055
Keywords
electrochemistry; single-atomcatalyst; electrode/electrolyteinterface; oxygen reduction; noncovalent interactions
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This study investigates the effect of noncovalent interactions on the performance of oxygen reduction reaction (ORR) using a synthesized Fe-N-C single-atom catalyst. It is found that TEA(+) plays a positive role in tuning the outer Helmholtz plane, improving oxygen diffusion coefficient, and increasing double-layer capacitance, enhancing the activity, selectivity, and stability of the catalyst towards ORR.
Highly efficient electrochemical interfaces are significant for the oxygen reduction reaction (ORR). However, previous efforts have been mainly paid to design catalytic sites with high intrinsic activity and neglect the electrode/electrolyte interfaces, especially the noncovalent interactions in the outer Helmholtz plane (OHP). Herein, an Fe-N-C single-atom catalyst is synthesized and acts as the model catalyst to demonstrate the effect of noncovalent interactions on the ORR performance. Two specific molecules of THA(+) and TEA(+) with different structures and functional groups have been selected to tune the OHP through noncovalent interactions. TEA(+) can adjust the OHP, improve the oxygen diffusion coefficient, and increase the double-layer capacitance. Therefore, TEA(+) enhances the activity, selectivity, and stability of Fe-N-C single-atom catalysts toward the ORR. This provides a new approach to finding new directions in designing electrochemical interfaces beyond the intrinsic catalytic sites in acidic electrolytes.
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