@article{Li2026, 
author = {Yang Li and Yuemei Liu and Yang Yuan and Xiaojun Lv and Junhong Ma and Chaoyun Ma and Hao Jiang},
title = {Synergizing the activity–stability trade-off in Fe–N–C electrocatalysts towards efficient and durable CO2-to-CO conversion},
year = {2026},
journal = {Nano Research},
volume = {19},
number = {7},
pages = {94908640},
keywords = {electrocatalysts, CO2 electroreduction, active sites, Zn-based batteries},
url = {https://www.sciopen.com/article/10.26599/NR.2026.94908640},
doi = {10.26599/NR.2026.94908640},
abstract = {Single-atom Fe–N–C electrocatalysts have demonstrated exceptional selectivity toward CO during CO2 reduction, yet their practical application is severely hindered by the intrinsic activity–stability trade-off. Herein, we report a straightforward in-situ sulfidation of Fe-doped zeolitic imidazolate frameworks to construct ZnS nanoparticle-modified S-doped Fe–N–C catalysts (ZnS@Fe–NSC). This approach causes the concurrent formation of Fe–N4 active sites, S doping, and ZnS nanoparticles. Operando characterizations and density functional theory (DFT) calculations reveal that ZnS nanoparticles donate electrons to Fe centers with a 0.5 eV negative shift in Fe 2p binding energy and strengthen Fe–N bonds with an increased integrated crystal orbital Hamiltonian population value from −0.94 to −1.30 eV. This electronic modulation accelerates the formation of the key *COOH intermediate and suppresses the hydrogen-induced Fe leaching by over 20-fold. The ZnS@Fe–NSC exhibits a CO Faradaic efficiency of 98.5% at −0.58 V versus reversible hydrogen electrode and maintains over 90% selectivity for 30 h. When integrated into a Zn–CO2 battery, it delivers a peak power density of 6.2 mW·cm−2 and operates stably for 125 h. This work opens an avenue for the rational design of robust single-atom electrocatalysts toward practical CO2 conversion and beyond.}
}