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Nano-carbon supported B/N-coordinated Fe single atoms with a tuned electronic structure for long lifespan zinc–iodine batteries

Li, Yong; Zhu, Aoyang; Peng, Guodong; He, Jun; Li, Hongqiang; Jia, Dedong; He, Guanjie; ... He, Xiaojun; + view all (2025) Nano-carbon supported B/N-coordinated Fe single atoms with a tuned electronic structure for long lifespan zinc–iodine batteries. Energy and Environmental Sciences 10.1039/d5ee00809c. (In press).

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Abstract

Single-atom catalysts (SACs) have great potential to boost the sluggish iodine redox kinetics and alleviate the polyiodide shuttle in aqueous zinc–iodine (Zn–I2) batteries. Nevertheless, it is a big challenge to improve the catalytic activity of traditional metal nitrogen (M–N4) SACs by adjusting the microenvironment to enhance iodine redox kinetics. Herein, asymmetric B/N-coordinated Fe single atoms (Fe–B2N2) immobilized on carbon nanotube forests (denoted as Fe-SAs@BNCF) are prepared by a one-pot calcination method and used as the iodine host in Zn–I2 batteries. Theoretical calculation results have revealed that the B sites function to increase the electron density by disrupting the symmetrical electron distribution around the Fe sites compared to traditional Fe–N4. Correspondingly, the as-synthesized Fe–B2N2 SACs significantly improve polyiodide adsorption and electrocatalytic activities in Zn–I2 batteries. Moreover, carbon nanotube forests provide more adsorption sites for polyiodides. Consequently, the Zn–I2 batteries with Fe-SAs@BNCF as a host enable a superb long lifespan (78% retention over 60 000 cycles at 5 A g−1) and a high rate capability (147 mA h g−1 at 10 A g−1). This work provides a promising strategy for designing advanced I2 cathodes with asymmetric single atoms for long-life Zn–I2 batteries.

Type: Article
Title: Nano-carbon supported B/N-coordinated Fe single atoms with a tuned electronic structure for long lifespan zinc–iodine batteries
DOI: 10.1039/d5ee00809c
Publisher version: https://doi.org/10.1039/d5ee00809c
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10210601
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