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Two-dimensional ZIF-L derived dual Fe/FeNx sites for synergistic efficient oxygen reduction in alkaline and acid
Jun-Fei Gu1, Jichao Wang2, Caixia Wang3
1State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 122 Luoshi Road, Wuhan 430070 China.
Abstract:
Fe-N-C catalysts have emerged as the most promising alternatives to commercial Pt/C catalysts for oxygen reduction reaction (ORR) due to their cost-effectiveness and favorable activity. Herein, a dual-site Fe/FeNx-NC catalyst was synthesized via a green, in situ doping strategy using two-dimensional Fe-doped ZIF-L as a nitrogen-rich precursor. The catalyst integrated Fe nanoparticles (NPs) and FeNx sites anchored on carbon nanotubes, intertwined with nitrogen-doped porous carbon nanosheets, achieving a high active site density and graphitisation. Electrochemical tests revealed that the optimized Fe/FeNx-NC-1 exhibited significant ORR activity, with a half-wave potential of 0.92 V and 0.80 V for alkaline and acidic medium, respectively. Zn-air batteries employing Fe/FeNx-NC-1 delivered a peak power density of 168 mW·cm-2 and a specific capacity of 790 mAh·g-1, outperforming those of Pt-based catalysts. Density functional theory calculations demonstrated a reduced free energy barrier for the rate-determining step (0.48 eV) compared to single-site Fe-N4 models (0.79 eV). The synergy between Fe NPs and FeNx optimized ORR intermediate adsorption and facilitated charge/mass transfer. This study offers valuable insights for the development of advanced energy conversion systems.
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