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Carbon-Vacancy-Induced Fe Coordination Modulation in FeZn Dual-Atom Sites for Enhanced Bifunctional Oxygen
Yu Bai1, Yingbi Chen1, Yuchao Wang1
1State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, P. R. China.
Abstract:
Precisely modulating the coordination structure of neighboring metal atomic sites is urgently required yet remains technically challenging. Herein, we report a carbon-vacancy-induced Fe coordination environment modulation in FeZn dual-atom sites (FeZnN6-VC) to boost bifunctional oxygen electrocatalysis. Finite element simulation and electronic structure characterization reveal that carbon vacancies promote electron transfer from Fe-N4 to neighboring Zn-N4 sites, establishing favorable electronic interactions. In situ Raman spectroscopy further identifies the key O-O- intermediate (corresponding to OOH*) and the FeOOH active phase during oxygen evolution reaction (OER), both showing significantly lowered onset potentials. Compared with conventional FeZn dual-atom catalysts, FeZnN6-VC achieves a 174 mV decrease in OER overpotential at 10 mA cm-2 and exhibits improved oxygen reduction reaction performance in alkaline media. The corresponding quasi-solid-state Zn-air battery delivers a long cycling life of 82.3 h at 50 mA cm-2. This work offers a versatile carbon-vacancy strategy to tune the local coordination of dual-atomic sites for advanced electrocatalysis.
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