期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 126, 期 1, 页码 30-39出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c07691
关键词
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资金
- Natural Science Foundation of Jiangsu Province [BK20200873, BZ2020011]
- National Key R&D Program of China [2017YFA0204800]
- National Natural Science Foundation of China [22173067]
- Collaborative Innovation Center of Suzhou Nano Science Technology
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- 111 Project
- Joint International Research Laboratory of Carbon-Based Functional Materials and Devices
- Science and Technology Development Fund, Macau SAR (FDCT) [0052/2021/A]
Designing bifunctional electrocatalysts for the ORR and OER is crucial for improving performance in reversible oxygen/water redox cell systems. This study explores the effect of graphene edges on the activity of single-atom M-N-4 motifs, with Co-N-4 and Rh-N-4 motifs at the armchair edge predicted to be optimal catalytic sites for ORR/OER. Symmetry breaking around the edge may impact intermediates' adsorption and thermodynamics, providing theoretical guidance for designing bifunctional oxygen electrode materials.
Designing bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) holds a central position for performance improvement in reversible oxygen/water redox cell systems. Herein, taking the graphene-confining single-atom M-N-4 motif as an example, we explored the effect of a graphene edge (armchair and zigzag configurations) on their bifunctional ORR and OER activities. It is clarified that the symmetry breaking of the M-N-4 motif around the edge has a potential influence on the intermediates' adsorption and thermodynamic pictures. Based on the evaluation of the electrochemical step symmetry index (ESSI) and bifunctional index (BI), Co-N-4 and Rh-N-4 motifs at the armchair edge with BIs of 0.49 and 0.61 V are predicted as optimal bifunctional catalytic sites for the ORR/OER due to the d-band modulation from the edge environment. Our results unfold the effect of the graphene edge on the oxygen-involving electrocatalytic mechanism and provide a clear theoretical guidance for the design of bifunctional oxygen electrode materials in reversible fuel cells, electrolyzers, and rechargeable metal-air batteries.
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