[1Group 1subproject/Sang-Jae Kim] Rational Design of Atomically Immobilized Fe‐N4 Sites via Acid‐Amine Chemistry: Leveraging Metal Ionic Assistance for Precise Morphology Control

5 Jan 2026
Views 31
Author
Arunprasath Sathyaseelan, Vijayakumar Elumalai, Muthukumar Perumalsamy, Swapnil Shital Nardekar, Arul Saravanan Raaju Sundhar, SC Karthikeyan, Dong Jin Yoo, Sang‐Jae Kim
JournalSusMat
Pagee260
Year2025
Linkhttps://doi.org/10.1002/sus2.260


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ABSTRACT


Tailoring atomically dispersed single-atom catalyst (Fe-SAC) holding well-defined coordination structure (Fe-N4) along with precise control over morphology is a critical challenge. Herein, we propose a novel acid-amine coupling reaction between metal-chelated ionic liquid ([1-(3-aminopropyl) 3-methylimidazolium tetrachloroferrate(III)] [APIM]+[FeCl4]−) and carboxylic groups of carbon allotropes (C = GO, CNT, CNF, and vX-72) to precisely immobilize Fe-Nx sites. Out of designed single-atom catalyst (IL-Fe-SAC-C), Fe-N4 on graphene (IL-Fe-SAC-Gr) delivered superior oxygen reduction reaction (ORR) activity by holding higher halfwave potential of 0.882 V versus RHE in 1.0 M KOH akin to Pt/C (0.878 V vs. RHE) and surpassing recently reported M–N–C catalysts with superior ethanol tolerance. Thanks to higher graphitization degree, enhanced surface characteristics, and richness in high-density Fe-N4 sites of IL-Fe-SAC-Gr confirmed by XPS, X-ray absorption spectroscopy (XAS), and HAADF analysis. The IL-Fe-SAC-Gr catalyst-coated cathode on testing in flexible direct ethanol fuel cells (f-DEFC) delivered higher peak power density of 18 mW cm−2 by outperforming Pt/C-based cathode by 3.5 times as a result of excellent ethanol tolerance. Further, the developed f-DEFC successfully powered the Internet of Things (IoT)-based health monitoring system. This method demonstrates novel strategy to tailor high-performance single-atom (Fe-SAC-C) sites on desired morphologies to meet specific application requirements with feasibility and versatility.

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Jeju National University Green Hydrogen Glocal Leading Research Center 

TEL. 064-754-4446  | E-MAIL. gh2rlrc@gmail.com

LOCATION. D208, Engineering Building 4, 102 Jejudaehak-ro, Jeju-si, 

Jeju Special Self-Governing Province, Jeju National University (Arail-dong), Republic of Korea

Where Jeju’s nature meets technology shaping

a sustainable future.


Copyright ⓒ Jeju National University Green Hydrogen Glocal Leading Research Center. All right reserved.