Affiliation:
1. School of Metallurgy and Environment Central South University Changsha 410083 P. R. China
2. Christopher Ingold Laboratory Department of Chemistry University College London 20 Gordon Street London WC1H 0AJ UK
Abstract
AbstractMetal‐free carbon‐based materials are considered to be one of the most promising alternatives to precious metal Pt‐based electrocatalysts. However, the electrocatalytic activity of heteroatom‐modulated carbon rarely reaches the level of metal‐based electrocatalysts. Here, electron‐rich carbon and abundant pyridinic‐N adjacent to C vacancies decorated with carbon nanosheets (E‐NC‐V) are synthesized and used as the host for boosting efficient oxygen reduction reaction. Rich pyridinic‐N structures adjacent to C vacancies work in synergy with electron‐rich carbon, which promotes the sharp decrease of |ΔGO*|, resulting in the balanced adsorption and dissociation of oxygen intermediates, and thus activating OO. This can be attributed to the abundant vacancies and d–p orbital hybridization between Zn and N/C. The E‐NC‐V catalyst drives the oxygen reduction reaction (ORR) via a 4e− transfer‐dominated pathway with a half‐wave potential of 0.87 V versus RHE in the alkaline solution, even superior to Pt/C. The assembled Al–air battery exhibits a high peak power density of 113 mW cm−2. This promising strategy sheds light on the design and fabrication of robust, rich‐density, and high‐performance active sites for the ORR. The work is expected to inspire future work on the role of electronic structure modulation and defect engineering for enhanced reaction kinetics.
Funder
National Natural Science Foundation of China
Subject
General Materials Science,Renewable Energy, Sustainability and the Environment
Cited by
22 articles.
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