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Updated: May 13, 2026
Surface Functionalization of Metal-Organic Frameworks for Improved Moisture Resistance
Published on: September 5, 2018
Dual modulation of the FeN4 electronic structure by axial F-coordination and second-shell P-doping for enhanced
Qingmeng Guo1, Lili Fan1, Zhanning Liu2
1Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, PR China.
Abstract:
Atomically dispersed Fe-N-C materials are promising catalysts for the oxygen reduction reaction (ORR), yet their performance is limited by the symmetric electron distribution inherent to the planar coordination structure. Herein, we propose a dual modulation strategy via simultaneous axial F-coordination and second-shell P doping within the FeN4 motif to enhance the ORR performance. The synthesized catalyst (Fe-NPFC) demonstrates exceptional ORR activity in alkaline electrolyte, featuring a half-wave potential of 0.927 V vs. RHE and robust stability, outperforming commercial 20 wt% Pt/C. Its superior activity has also been verified when used as a cathode in zinc-air batteries, delivering higher power density and cycling stability than the Pt/C counterpart under identical conditions. Density functional theory calculations suggest that the axial fluorine and second-shell phosphorus synergistically optimize the electronic structure of the Fe center, allowing for more efficient adsorption and desorption of oxygenated intermediates, thus enhancing the overall reaction kinetics. This strategy would be a viable route for developing high-performance single-atom catalysts.
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