N,Te配位Fe-Co双金属位点作为高效氧电催化剂用于高性能锌空电池

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

催化学报 ›› 2026, Vol. 81: 319-332.DOI: 10.1016/S1872-2067(25)64875-3

N,Te配位Fe-Co双金属位点作为高效氧电催化剂用于高性能锌空电池

徐慧民^a^,¹, 宫萧琪^b^,¹, 岳楷航^c^,¹, 黄陈金^a, 朱鸿睿^a, 宋联杰^d, 李高仁^a()

^a 四川大学材料科学与工程学院, 四川成都 610065
^b 中山大学化学学院, 广东广州 510275
^c 中国科学院上海硅酸盐研究所, 能源转换材料重点实验室, 上海 200050
^d 中国十九冶集团有限公司, 四川成都 610031

收稿日期:2025-06-25 接受日期:2025-09-11 出版日期:2026-02-18 发布日期:2025-12-26
通讯作者: *电子信箱: ligaoren@scu.edu.cn (李高仁).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(52373215);四川省自然科学基金(2023NSFSC0086);高校基本业务费(YJ2021156)

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

Hui-Min Xu^a^,¹, Xiao-Qi Gong^b^,¹, Kai-Hang Yue^c^,¹, Chen-Jin Huang^a, Hong-Rui Zhu^a, Lian-Jie Song^d, Gao-Ren Li^a()

^a College of Materials Science and Engineering, Sichuan University, Chengdu 610065, Sichuan, China
^b School of Chemistry, Sun Yat-sen University, Guangzhou 510275, Guangdong, China
^c CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences (SICCAS), Shanghai 200050, China
^d China 19th Metallurgical Group Corporation Limited, Chengdu 610031, Sichuan, China

Received:2025-06-25 Accepted:2025-09-11 Online:2026-02-18 Published:2025-12-26
Contact: *E-mail: ligaoren@scu.edu.cn (G.-R. Li).
About author:¹ Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(52373215);Sichuan Science and Technology Program(2023NSFSC0086);Fundamental Research Funds for the Central Universities(YJ2021156)

摘要/Abstract

摘要：

锌空气电池(ZABs)因其低成本、高理论能量密度(1086 Wh kg⁻¹)及环境友好特性, 被视为极具前景的可持续储能技术. 然而, 其大规模应用受限于空气电极动力学缓慢的双功能氧催化过程—析氧反应(OER)与氧还原反应(ORR). 开发兼具高活性、低成本及稳定性的双功能催化剂是突破该瓶颈的核心挑战. 单金属单原子催化剂的性能受限于其单一活性位点的催化活性. 而双金属单原子体系利用金属协同效应, 可同时优化电荷转移效率与氧中间体(OOH, O, *OH)的吸附能垒, 从而为提升双功能催化性能开辟了新途径.

本研究使用具有独特的三角锥形结构的TeO₃²⁺作为金属阳离子的配体, 与Fe³⁺和Co²⁺形成桥接配位模式, 形成[M1-(TeO)-M2]的局部结构单元. 与简单的单齿配体(如氯离子、硝酸根离子)或小尺寸的多齿配体不同, TeO₃²⁺具有一定的空间尺寸, 有助于限制簇的大小, 并防止形成更大的金属聚合物. 在随后的热解过程中, 各种形式的碲(如TeO₃²⁺, TeO₂, Te等)会经历复杂的转变(还原、挥发和掺杂), 最终形成具有N, Te共配位的铁钴双金属单原子催化剂(记为FeNxTey/CoNxTey@NC), 将其用作ZABs双功能催化剂. 该FeN_xTe_y/CoN_xTe_y@NC催化剂在碱性条件下表现出卓越的ORR/OER双功能催化性能: ORR半波电位高达0.912 V, 在10 mA cm⁻²电流密度下的OER过电位低至305 mV. 基于该催化剂的ZABs实现了306.1 mW cm⁻²的峰值功率密度和773.2 mAh g⁻¹的高比能量密度. 实验数据表明, Te掺杂可实现FeN_xTe_y/CoN_xTe_y@NC中原子活性位点结构(理想化理论模型为FeCoN₆Te)的高密度分布与精准调控. 密度泛函理论计算揭示, 当FeN₄/CoN₄模型(对应合成催化剂FeN_x/CoN_x@NC)转变为FeCoN₆Te模型时, Te原子通过调控FeCoN₆Te模型中Fe/Co位点的局部电荷密度, 促进双金属间的电荷转移, 进而优化ORR/OER反应中间体的吸附能.

综上, 本文成功研制出一种氮/碲(N/Te)共配位型双金属单原子催化剂, 其创新性在于: 一方面, 通过构建FeCoN₆Te理论模型揭示了双功能催化的构效关系; 另一方面, 采用铁、钴等非贵金属元素显著降低锌空气电池的电极材料成本. 该工作为开发面向实际应用的高性能双原子催化剂提供了新的策略.

关键词: 双金属单原子, 碲配位, 氮掺杂碳, 氧还原反应, 析氧反应, 锌空气电池

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

徐慧民, 宫萧琪, 岳楷航, 黄陈金, 朱鸿睿, 宋联杰, 李高仁. N,Te配位Fe-Co双金属位点作为高效氧电催化剂用于高性能锌空电池[J]. 催化学报, 2026, 81: 319-332.

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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https://www.cjcatal.com/CN/Y2026/V81/I2/319

图/表 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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N,Te配位Fe-Co双金属位点作为高效氧电催化剂用于高性能锌空电池

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

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