@article{Zhang2025, 
author = {Yang Zhang and Bingbing Gong and Benji Zhou and Zhibo Liu and Nengneng Xu and Yongxia Wang and Xiaoqian Xu and Qing Cao and Daniil I. Kolokolov and Haitao Huang and Shuaifeng Lou and Guicheng Liu and Woochul Yang and Jinli Qiao},
title = {Hydrophobicity engineering of hierarchically ordered SiO2/Fe-N-C catalyst with optimized triple-phase boundary for boosting oxygen reduction reaction},
year = {2025},
journal = {Nano Research Energy},
volume = {4},
pages = {e9120180},
keywords = {Fe-Nx site, a space-confinement strategy, oxygen reduction reaction (ORR), zinc-air batteries, proton exchange membrane fuel cells},
url = {https://www.sciopen.com/article/10.26599/NRE.2025.9120180},
doi = {10.26599/NRE.2025.9120180},
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.}
}