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Cage-confinement of gas-phase ferrocene in zeolitic imidazolate frameworks to synthesize high-loading and atomically dispersed Fe?N codoped carbon for efficient oxygen reduction reaction

Ye, Guanying, He, Qian, Liu, Suqin, Zhao, Kuangmin, Su, Yuke, Zhu, Weiwei, Huang, Rongjiao and He, Zhen 2019. Cage-confinement of gas-phase ferrocene in zeolitic imidazolate frameworks to synthesize high-loading and atomically dispersed Fe?N codoped carbon for efficient oxygen reduction reaction. Journal of Materials Chemistry A 7 (27) , pp. 16508-16515. 10.1039/C9TA04954A
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Abstract

Fe–N codoped carbon (Fe–N/C) has emerged as one of the most promising non-precious electrocatalysts for the oxygen reduction reaction (ORR). However, the fabrication of Fe–N/C with high Fe and N loadings while maintaining atomic dispersion of the loaded Fe is still challenging. Herein, we present a cage-confinement synthesis strategy that utilizes zeolitic imidazolate framework-8 (ZIF-8) with an ordered microporous structure to uniformly adsorb gas-phase ferrocene (FeCp) molecules at mildly elevated temperatures followed by carbonization to fabricate Fe–N/C with a high content of atomically dispersed Fe and abundant N. The content of FeCp molecules adsorbed in the nanocavities of ZIF-8 could be precisely controlled by the adsorption temperature and time, and confining the adsorbed FeCp in the nanocavities of ZIF-8 could effectively prevent the Fe atoms from aggregating and/or forming Fe compounds during the carbonization process. The Fe–N/C fabricated under optimal conditions has a high iron loading of 5.86 wt% and abundant N content of 10.51 at%. The as-prepared Fe–N/C exhibits a remarkable ORR catalytic performance in 0.1 M KOH with a half-wave potential (E1/2) of 0.85 V (vs. RHE) and excellent long-term durability (less than 10 mV change of E1/2 after 10 000 cycles of the CV test and 11% current density decay after a 40 000 s long-term ORR test). This work provides a simple and controllable synthesis strategy for fabricating high-content atomically dispersed Fe and N codoped carbon catalysts, which might also shed light on the design and synthesis of other single-atom metal doped carbon materials for energy storage and conversion applications.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Royal Society of Chemistry
ISSN: 2050-7488
Date of First Compliant Deposit: 30 July 2019
Date of Acceptance: 16 June 2019
Last Modified: 18 Oct 2019 06:35
URI: http://orca-mwe.cf.ac.uk/id/eprint/124594

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