Fe and Co bimetallic single-atoms coordinated by N and Te as bifunctional oxygen reduction/evolution catalysts for high-performance zinc-air battery

doi:10.1016/S1872-2067(25)64875-3

Abstract

Abstract:

Zinc air batteries (ZABs) are a low-cost, high-energy density, and green sustainable energy storage device. At present, the main challenge in achieving large-scale application of ZABs is to develop low-cost and high-performance bifunctional catalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Compared with monometallic single-atom catalyst, the bimetallic single-atoms catalyst can effectively improve ORR/OER bifunctional activity, realize rapid charge transfer, and play a significant role in regulating the adsorption of oxygen intermediates. In this study, we design the novel Fe and Co bimetallic single-atoms coordinated by Te and N anchoring on N-doped carbon (NC) (denoted as FeN_xTe_y/CoN_xTe_y@NC) for the first time, serving as a bifunctional catalyst for ZABs. This innovative catalyst exhibits excellent bifunctional ORR/OER catalytic performance under alkaline conditions, achieving a high half-wave potential of 0.912 V for ORR and a low overpotential of 305 mV for OER at 10 mA cm^-2. The FeN_xTe_y/CoN_xTe_y@NC-based ZABs realizes a high peak power density of 306.1 mW cm^-2 and a large specific energy density of 773.2 mAh g^-1. The experimental data show that the N-doped can achieve precise regulation of the structure and high-density distribution of atomic active sites in FeN_xTe_y/CoN_xTe_y@NC (idealized theoretical model is FeCoN₆Te). The density functional theory calculations show that when the FeN₄/CoN₄ models (the synthesized catalyst denoted as FeN_x/CoN_x@NC) transforms into FeCoN₆Te models, Te atoms regulate the local charge densities of Fe and Co on FeCoN₆Te models and further promote the charge transfer between Fe and Co on FeCoN₆Te models, which optimizes the adsorption energies of ORR/OER intermediates. The findings in this study will pave the way for the development of high-performance bimetallic single-atom catalysts for practical energy conversion applications.

Key words: Bimetallic single-atoms, Te coordination, N-doped Carbon, Oxygen reduction reaction, Oxygen evolution reaction, Zinc-air battery

Hui-Min Xu, Xiao-Qi Gong, Kai-Hang Yue, Chen-Jin Huang, Hong-Rui Zhu, Lian-Jie Song, Gao-Ren Li. Fe and Co bimetallic single-atoms coordinated by N and Te as bifunctional oxygen reduction/evolution catalysts for high-performance zinc-air battery[J]. Chinese Journal of Catalysis, 2026, 81: 319-332.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64875-3

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Figures/Tables 7

Fig. 1. Design and synthesis of SACs. (a) Geometric structures of single atom, dual atoms, and FeCoN6Te bimetallic single-atoms catalysts. (b) Calculated theoretical overpotential of rate-determining of ORR volcano plot with ΔGOH as descriptors and Free energy distribution of RDS for ORR and OER of different theoretical models.

Fig. 2. Schematic diagram of preparation and the structure of FeNxTey/CoNxTey@NC.

Fig. 3. (a) SEM image of FeNxTey/CoNxTey@NC. (b) AC-TEM image of FeNxTey/CoNxTey@NC. (c) 3D and 2D resolution mappings obtained from area 1 of AC-TEM image of FeNxTey/CoNxTey@NC in (b). (d) Interatomic distances measured in the AC-TEM image of FeNxTey/CoNxTey@NC in (b). (e−k) HAADF-STEM image and EDS mappings of FeNxTey/CoNxTey@NC ((k) is the superposition of (h) and (i)).

Fig. 4. XANES curves of FeNxTey/CoNxTey@NC and references at Fe K-edge (a) and Co K-edge (b). Fourier-transform EXAFS curves of FeNxTey/CoNxTey@NC and references at Fe K-edge (c) and Co K-edge (d). R-space (e) and k-space (f) of Co K-edge EXAFS (points) and the fitting curve (red line) of FeNxTey/CoNxTey@NC.

Fig. 5. LSVs (a) and Tafel plots (b) of FeNxTey/CoNxTey@NC, FeNx/CoNx@NC, Pt/C + RuO2, Fe SA@NC, and NC of ORR in O2-saturated 0.1 mol L−1 KOH electrolyte. (c) Comparison of E1/2, Eonset, and JK (at 0.85 V vs. RHE) of FeNxTey/CoNxTey@NC, FeNx/CoNx@NC, Pt/C + RuO2, Fe SA@NC, and NC. (d) LSVs of FeNxTey/CoNxTey@NC at the different rotation speeds, ranging from 400 to 2025 rpm (inset: electron transfer number of FeNxTey/CoNxTey@NC). (e) Methanol tolerance tests of FeNxTey/CoNxTey@NC and Pt/C + RuO2. (f) Constant voltage stability tests of FeNxTey/CoNxTey@NC and Pt/C + RuO2.

Fig. 6. In-situ Raman spectra of the ORR at FeNxTey/CoNxTey@NC (a) and FeNx/CoNx@NC (b) electrode surface in a 0.1 mol L−1 KOH solution. (c) Theoretical schematic diagram of OH adsorption on Fe sites in FeN4 and FeCoN6Te models and schematic diagram of Fe d and O p orbital hybridization. (d) Schematic diagram of four-electron process of ORR at Fe site of FeCoN6Te model. (e) Gibbs free energy diagrams of ORR at Fe site of FeN4 and Fe, Co sites of FeCoN6Te models. (f) Gibbs free energy diagrams of OER at Fe site of FeN4 and Fe, Co sites of FeCoN6Te models.

Fig. 7. (a) The model diagram of ZAB. (b) Charge-discharge polarization curves and corresponding power density curve of FeNxTey/CoNxTey@NC-based ZAB and Pt/C + RuO2-based ZAB. (c) Constant current discharge curves at different current densities. (d) Step discharge curves of FeNxTey/CoNxTey@NC-based ZAB and Pt/C + RuO2-based ZAB at different current densities. (e) Cyclic charge-discharge diagram at a current density of 10 mA cm−2 (insets: the cycle curves of the first 5 h and 48th 5 h of charge and discharge). (f) Schematic diagram of flexible FeNxTey/CoNxTey@NC-based soft pack ZAB with different bending angles. (g) Discharge curve and power density curve of flexible FeNxTey/CoNxTey@NC-based soft pack ZAB and flexible Pt/C+RuO2-based soft pack ZAB. (h) Step discharge curves at the different current densities of flexible FeNxTey/CoNxTey@NC-based soft pack ZAB.

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