Atomically dispersed Fe-Nx sites doped mesopore-dominated carbon nanodisks towards efficient oxygen reduction

• Published in: International journal of hydrogen energy 2022-09, Vol.47 (78), p.33308-33318
• Main Authors: Jiang, Xiaole, Yang, Yaoyue, Zhu, Chenglin, Zhou, Chong, Zhang, Rui, Wu, Feng, Wu, Haihua, Wang, Jing
• Format: Article
• Language: English
• Subjects: Fe-Nx active sites; Oxygen reduction reaction; Surface functionalization; Zeolitic imidazolate frameworks
• ISSN: 0360-3199; 1879-3487
• DOI: 10.1016/j.ijhydene.2022.07.209

Rational design and synthesis of carbon nanostructures doped with atomically dispersed metal sites is an effective method to improve electrocatalytic oxygen reduction reaction (ORR) performance. Introducing mesopores into substrate carbon materials would help expose more active sites and improve mass/charge transfer in the microenvironments near active sites, thus accelerating ORR. Nonetheless, it is still challenging to construct atomically dispersed metal-nitrogen-carbon with mesoporous structures. Herein, we propose a facile strategy to synthesize atomically dispersed Fe-Nx sites doped mesopore-dominated carbon nanodisks catalysts (Fe–N/CNDs) using functionalized zeolitic imidazole frameworks (ZIF-D). The Fe–N/CNDs-900 catalyst exhibits outstanding ORR activity (Eo = 1.03 V, E1/2 = 850 mV), as well as excellent long-term durability and methanol-tolerance, ascribed to synergistic effect of the Fe-Nx active sites and the surrounding mesoporous structures. This work presents a promising method to develop highly efficient metal-nitrogen-carbon ORR catalysts using functionalized MOFs. Herein, atomically dispersed Fe-Nx sites doped mesopore-dominated carbon nanodisks catalysts was synthesized by a facile strategy using functionalized zeolitic imidazole frameworks (ZIF-D). The as-prepared catalysts exhibited excellent ORR catalytic performance due to synergistic effect of atomically dispersed Fe-Nx active sites and the surrounding mesopore-dominated structures. [Display omitted] •The Fe–N/CNDs is synthesized by a facile strategy using functionalized ZIF-D.•The Fe-Nx active sites are atomically dispersed in the mesopore-dominated carbon.•The Fe–N/CNDs exhibits outstanding ORR activity compared with the commercial Pt/C.•The synergistic effect makes great contribution to the catalytic performance.