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Research Article | Open Access | Online First

Hydrophobicity engineering of hierarchically ordered SiO2/Fe-N-C catalyst with optimized triple-phase boundary for boosting oxygen reduction reaction

Yang Zhang1, Bingbing Gong3, Benji Zhou1, Zhibo Liu6, Nengneng Xu1, Yongxia Wang1, Xiaoqian Xu1, Qing Cao1, Daniil I. Kolokolov4, Haitao Huang5, Shuaifeng Lou6, Guicheng Liu7, Woochul Yang8, Jinli Qiao1,2( )
State Key Laboratory of Advanced Fiber Materials, College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
School of Chemical Engineering and Technology, Xinjiang University, Urumqi 830017, China
Boreskov Institute of Catalysis, Siberian Branch of Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
Department of Applied Physics, Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hong Kong SAR 999077, China
State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China
Beijing Laboratory of New Energy Storage Technology, School of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China
Department of Physics, Dongguk University, Seoul 04620, Republic of Korea
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Graphical Abstract

Abstract

The Fe single-atom catalyst (Fe-N-C) with Fe-Nx active sites is considered a promising alternative to Pt-based catalysts for oxygen reduction reaction (ORR). However, the exposure and utilization efficiency of the Fe-Nx site in Fe-N-C lead to a certain competitive distance with Pt-based catalysts in the ORR process. Herein, a space-confinement strategy triggered by SiO2 templates to optimize the ORR triple-phase boundary of Fe-N-C, is reported. As expected, the optimized SiO2(4)/Fe-N-C exhibits excellent ORR activity with a half-wave potential of 0.886 V in 0.1 M KOH. More importantly, the E1/2 loss of SiO2(4)/Fe-N-C is merely 32 mV after 30,000 cycles. Density functional theory (DFT) calculations confirm SiO2-induced carbon defects critically modulate electronic configurations of FeN4 centers, optimizing adsorption energetics of oxygen intermediates. Remarkably, when utilized as air cathodes for zinc-air batteries (ZABs), the device based on SiO2(4)/Fe-N-C displays record-breaking power density (444.10 mW·cm–2) with superior long-term durability over 1013 h, outperforming most reported noble-metal-free electrocatalysts. This work provides a new route to optimize the triple-phase boundary of single-atom catalysts for energy storage applications.

Keywords

Fe-Nx sitea space-confinement strategyoxygen reduction reaction (ORR)zinc-air batteriesproton exchange membrane fuel cells

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Nano Research Energy
DOI: 10.26599/NRE.2025.9120180
Cite this article:
Zhang Y, Gong B, Zhou B, et al. Hydrophobicity engineering of hierarchically ordered SiO2/Fe-N-C catalyst with optimized triple-phase boundary for boosting oxygen reduction reaction. Nano Research Energy, 2025, https://doi.org/10.26599/NRE.2025.9120180

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Received: 31 March 2025
Revised: 08 May 2025
Accepted: 03 June 2025
Published: 20 June 2025
© The Author(s) 2025. Published by Tsinghua University Press.

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