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Potent Charge-Trapping for Boosted Electrocatalytic Oxygen Reduction

Li, Z; Cheng, H; Lu, Y; Wang, T; Li, Y; Zhang, W; He, G; (2023) Potent Charge-Trapping for Boosted Electrocatalytic Oxygen Reduction. Advanced Energy Materials , Article 2203963. 10.1002/aenm.202203963. (In press). Green open access

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Abstract

Metal-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 OO. 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.

Type: Article
Title: Potent Charge-Trapping for Boosted Electrocatalytic Oxygen Reduction
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/aenm.202203963
Publisher version: https://doi.org/10.1002/aenm.202203963
Language: English
Additional information: © 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/).
Keywords: d–p orbital hybridization, electron-enriched carbon, metal–air batteries, N regulation, oxygen reduction reaction
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10167775
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