Abstract
Transition-metal-nitrogen/carbon (TM-N/C) materials are promising alternatives to Pt-based oxygen reduction reaction (ORR) electrocatalysts of fuel cells. Identifying the highly active sites is the prerequisite for the design of high-performance electrocatalysts, in which the density functional theory (DFT) calculation is an important tool. However, the DFT simulation was usually conducted with a charge-neutral model, which is far away from the working condition, that is, under certain potentials. Herein, by using the DFT method with the explicit consideration of electrode potential, we systematically compared the activities of the Fe-N/C moieties previously proposed in the literature and identified the best one. This study not only demonstrates the significance of the electrode potential in computational electrochemistry but also suggests a feasible experimental strategy to increase the ORR performance of Fe-N/C electrocatalysts by creating edges defects and coordinating with the axial ligands on the Fe center, which is of practical significance for exploring the advanced non-precious-metal-based ORR electrocatalysts and related devices.
Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
