- Title
- Dual single-atomic Ni-N4 and Fe-N4 sites constructing Janus Hollow Graphene for selective oxygen electrocatalysis
- Creator
- Chen, Jiangyue; Li, Hao; Fan, Chuang; Meng, Qingwei; Tang, Yawen; Qiu, Xiaoyu; Fu, Gengtao; Ma, Tianyi
- Relation
- ARC.DE150101306 http://purl.org/au-research/grants/arc/DE150101306
- Relation
- Advanced Materials Vol. 32, Issue 30, no. 2003134
- Publisher Link
- http://dx.doi.org/10.1002/adma.202003134
- Publisher
- Wiley
- Resource Type
- journal article
- Date
- 2020
- Description
- Nitrogen-coordinated metal single atoms in carbon have aroused extensive interest recently and have been growing as an active research frontier in a wide range of key renewable energy reactions and devices. Herein, a step-by-step self-assembly strategy is developed to allocate nickel (Ni) and iron (Fe) single atoms respectively on the inner and outer walls of graphene hollow nanospheres (GHSs), realizing separate-sided different single-atom functionalization of hollow graphene. The Ni or Fe single atom is demonstrated to be coordinated with four N atoms via the formation of a Ni-N4 or Fe-N4 planar configuration. The developed Ni-N4/GHSs/Fe-N,4 Janus material exhibits excellent bifunctional electrocatalytic performance, in which the outer Fe-N4 clusters dominantly contribute to high activity toward the oxygen reduction reaction (ORR), while the inner Ni-N4 clusters are responsible for excellent activity toward the oxygen evolution reaction (OER). Density functional theory calculations demonstrate the structures and reactivities of Fe-N4 and Ni-N4 for the ORR and OER. The Ni-N4/GHSs/Fe-N4 endows a rechargeable Zn–air battery with excellent energy efficiency and cycling stability as an air-cathode, outperforming that of the benchmark Pt/C+RuO2 air-cathode. The current work paves a new avenue for precise control of single-atom sites on carbon surface for the high-performance and selective electrocatalysts.
- Subject
- bifunctional electrocatalysis; Janus catalysts; single atoms; Zn-air batteries; SDG 7; Sustainable Development Goals
- Identifier
- http://hdl.handle.net/1959.13/1458924
- Identifier
- uon:45543
- Identifier
- ISSN:0935-9648
- Language
- eng
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