MOFs衍生的磷掺杂Co9S8增强氧析出和还原反应: 迈向高性能锌空气电池

doi:10.1016/S1872-2067(26)65028-0

催化学报 ›› 2026, Vol. 85: 204-215.DOI: 10.1016/S1872-2067(26)65028-0

MOFs衍生的磷掺杂Co₉S₈增强氧析出和还原反应: 迈向高性能锌空气电池

王翔^a^,^b^,¹(), 周敏^c^,¹, 廖小彬^c, 韩旭^b^,^d, 省聪聪^e^,^f, Bes René^g, Huotari Simo^g, Arbiol Jordi^d^,^h, Cabot Andreu^b^,^h()

^a 武汉工程大学化工与制药学院, 磷矿及其共伴生资源绿色高效开发利用全国重点实验室, 湖北武汉 430205, 中国
^b 西班牙加泰罗尼亚能源研究所(IREC), 巴塞罗那, 西班牙
^c 武汉理工大学材料科学与工程国际化示范学院, 硅酸盐科学与先进建材全国重点实验室, 湖北武汉 430070, 中国
^d 西班牙加泰罗尼亚纳米科学与纳米技术研究所(ICN2), 巴塞罗那, 西班牙
^e 浙江大学温州研究院, 浙江温州, 中国
^f 宾夕法尼亚州立大学材料科学与工程系, 费城, 美国
^g 赫尔辛基大学物理系, 赫尔辛基, 芬兰
^h 加泰罗尼亚高等研究院(ICREA), 巴塞罗那, 西班牙

收稿日期:2025-09-17 接受日期:2026-01-06 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: wangxiang@wit.edu.cn (王翔),
acabot@irec.cat (A. Cabot).
作者简介:
¹共同第一作者.
基金资助:
国家自然科学基金(22302151);国家自然科学基金(52502312);湖北省自然科学基金(2024AFB755)

Enhanced oxygen evolution and reduction by phosphorus-doped Co₉S₈ derived from MOFs: Toward high-performance zinc-air batteries

Xiang Wang^a^,^b^,¹(), Min Zhou^c^,¹, Xiaobin Liao^c, Xu Han^b^,^d, Congcong Xing^e^,^f, René Bes^g, Simo Huotari^g, Jordi Arbiol^d^,^h, Andreu Cabot^b^,^h()

^a State Key Laboratory of Green and Efficient Development of Phosphorus Resources, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, Hubei, China
^b Catalonia Institute for Energy Research (IREC), Sant Adrià de Besòs, 08930 Barcelona, Spain
^c State Key Laboratory of Silicate Materials for Architectures, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, Hubei, China
^d Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, 08193 Barcelona, Catalonia, Spain
^e Institute of Wenzhou, Zhejiang University, Wenzhou 325006, Zhejiang, China
^f Department of Materials Science and Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States
^g Department of Physics, University of Helsinki, P.O. Box 64, FI-00014 Helsinki, Finland
^h ICREA Pg. Lluis Companys, 08010 Barcelona, Catalonia, Spain

Received:2025-09-17 Accepted:2026-01-06 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: wangxiang@wit.edu.cn (X. Wang),
acabot@irec.cat (A. Cabot).
About author:
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22302151);National Natural Science Foundation of China(52502312);Natural Science Foundation of Hubei Province(2024AFB755)

摘要/Abstract

摘要：

近年来, 锌空气电池因其理论能量密度高, 安全性高、资源丰富等优势, 被认为是极具潜力的新型储能体系. 然而, 其性能受限于空气电极中氧还原(ORR)和氧析出(OER)反应动力学缓慢, 开发高效稳定的双功能电催化剂至关重要. 金属有机框架材料(MOFs)因结构可控、组成可调和孔道丰富, 成为理想的前驱体. 尤其是MOFs在热解或刻蚀过程中形成空腔与多级孔结构, 可显著提高比表面积与活性位点暴露量, 缩短传质路径, 增强电解液渗透, 缓冲电极材料充放电过程中的体积膨胀. 同时, 中空结构构筑的连续导电网络, 可加速电子传输. 通过调控前驱体组成与转化条件, 实现中空结构与非金属活性中心的协同优化, 有望显著提升氧电催化活性与循环稳定性, 为高性能锌空气电池的构筑提供重要结构设计思路.

本文报道了一种钴基金属有机框架材料ZIF-67衍生的高效双功能磷掺杂的硫化钴(P-Co₉S₈)中空纳米立方体电催化剂, 应用于可充电锌空气电池(ZABs)的ORR和OER. 扫描电镜、透射电镜和比表面积测试结果表明, P-Co₉S₈保持了结构规整的空心纳米立方体形貌, 具有互连的孔隙, 从而提供了高比表面积, 丰富的暴露活性位点以及缩短的电子/离子扩散路径. X射线光电子能谱及X射线吸收谱结果表明, 磷掺杂促进了P-Co键的形成, 并提高了钴活性位点周围的电子密度, 从而调控了P-Co₉S₈的催化性能, 增强了电导率, 并改善了表面润湿性, 获得了260 mV的OER过电位和0.899 V的高ORR半波电位. 当用作ZABs的空气阴极时, P-Co₉S₈的峰值功率密度为177 mW cm^-2, 比容量为775 mAh gZn^-1. 此外, ZIF-67衍生的P-Co₉S₈具有良好的机械强度和循环稳定性, 在连续循环900 h后仍保持稳定, 显著优于基准Pt/C + RuO₂催化剂. 密度泛函理论计算分析, 磷掺杂能够改变局部配位环境, 增强Co-S相互作用, 重新分布电荷密度, 并优化氧中间体形成和解吸的能垒. 此外, 磷的引入还使d带中心发生移动, 促进轨道杂化, 从而加速ORR和OER的动力学过程. 上述结果表明P-Co₉S₈具有作为可逆氧电化学的稳健双功能催化剂的潜力.

综上, 本工作展示了通过非金属杂原子掺杂结合MOF衍生的空心结构进行原子级微环境工程, 在实现高效, 耐用且经济的双功能电催化剂方面的有效性. 除了提升锌空气电池(ZABs)的性能外, 还为开发用于各种可持续能源转换和存储应用的下一代过渡金属硫族化合物催化剂提供了可推广的设计思路.

关键词: 金属有机框架材料, 磷掺杂, 硫化钴, 双功能催化剂, 析氧反应, 氧还原反应, 锌空气电池

Abstract:

Developing high-performance electrocatalysts for the oxygen evolution (OER) and reduction reactions (ORR) is key to further developing rechargeable zinc-air batteries (ZABs). In this work, we demonstrate phosphorus-doped hollow cobalt pentlandite (P-Co₉S₈) nanocubes, derived from ZIF-67, which combine MOF-inherited porosity with phosphorus-induced electronic modulation, as a bifunctional oxygen electrocatalyst. As a cathode catalyst, P-Co₉S₈ achieves a high power density of 177 mW cm^-1, a specific capacity of 775 mAh g_Zn^-1, and remarkable cycling stability over 900 h. Comprehensive experiments and density functional theory show that P doping tunes the local coordination environment, optimizes the d-band center, and lowers reaction energy barriers, enabling fast, durable, and selective oxygen electrocatalysis. This study establishes a generalizable strategy for designing advanced chalcogenide-based electrocatalysts for next-generation energy storage devices.

Key words: Metal-organic framework, Phosphorus doping, Cobalt sulfide, Bifunctional electrocatalyst, Oxygen evolution reaction, Oxygen reduction reaction, Zinc-air battery

王翔, 周敏, 廖小彬, 韩旭, 省聪聪, Bes René, Huotari Simo, Arbiol Jordi, Cabot Andreu. MOFs衍生的磷掺杂Co₉S₈增强氧析出和还原反应: 迈向高性能锌空气电池[J]. 催化学报, 2026, 85: 204-215.

Xiang Wang, Min Zhou, Xiaobin Liao, Xu Han, Congcong Xing, René Bes, Simo Huotari, Jordi Arbiol, Andreu Cabot. Enhanced oxygen evolution and reduction by phosphorus-doped Co₉S₈ derived from MOFs: Toward high-performance zinc-air batteries[J]. Chinese Journal of Catalysis, 2026, 85: 204-215.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65028-0

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Fig. 1. (a) Schematic illustration of the synthesis process for P-Co9S8. SEM images of ZIF-67 (b), Co9S8 (c), and P-Co9S8 (d). (e,f) TEM images of P-Co9S8. (g) HRTEM image and corresponding FFT spectrum (insert). The P-Co9S8 lattice fringe distances were measured to be 0.235, 0.288, and 0.296 nm, at 52.92° and 130.11°, which could be interpreted as the cubic Co9S8 phase, visualized along its [011] zone axis. (h,i) HAADF-STEM images and EELS chemical composition maps obtained from the red squared area of the STEM micrograph. Individual Co L2,3-edges at 779 eV (red), P L2,3-edges at 132 eV (green), S L2,3-edges at 165 eV (blue), and composites of Co-P, Co-S, Co-P-S.

Fig. 2. XRD patterns (a) and P 2p (b), S 2p (c), and Co 2p (d) high-resolution XPS spectra of Co9S8 and P-Co9S8. (e) Normalized XANES at the Co K-edge. (f) Calculated Co valence state from the XANES. Corresponding FT-EXAFS spectra (h) and Wavelet transform for the k2-weighted EXAFS signals (i) of Co for Co9S8 and P-Co9S8.

Fig. 3. (a) LSV polarization curves. (b) Corresponding Tafel plots. (c) Overpotential at 10 mA cm-2 and extracted Tafel slopes for the as-prepared catalysts. (d) Capacitive current density. (e) EIS Nyquist responses. (f) LSV curves of P-Co9S8 recorded before and after 5000 cycles. (g) Chronoamperometric stability of P-Co9S8 compared with IrO2. (h) Benchmarking of overpotential at 10 mA cm-2 and Tafel slopes against reported sulfide-based OER catalysts (Table S2).

Fig. 4. LSV polarization curves (a), Tafel plots (b), and Ehalf together with jk (0.85 V vs. RHE) (c) for Co9S8, P-Co9S8, P-Co3S4, and Pt/C measured in O2-saturated 0.1 mol L-1 KOH at 1600 rpm. RDE polarization curves of P-Co9S8 acquired at different rotation rates (d), with the corresponding K-L plots (e). (f) Electron-transfer number and H2O2 yield of P-Co9S8 (inset: RRDE LSV curves at 1600 rpm). (g) Chronoamperometric stability tests. (h) LSV curves of P-Co9S8 before and after 2000 CV cycles. (i) Methanol crossover tolerance at 0.7 V for P-Co9S8 and commercial Pt/C.

Fig. 5. (a) Atomic structure models of P-Co9S8 (b,c) PDOS and d band center of Co9S8 and P-Co9S8. Gibbs free energy evolution for OER of the different P-Co9S8 models at 1.23 V (d), and of Co9S8 and P-Co9S8 at different potentials (e).

Fig. 6. (a) Schematic diagram of an aqueous ZAB. Open circuit potentials (b), discharge polarization curves and corresponding peak powder density (c), specific capacities (d), and long-term charge-discharge cycling stabilities (e) of Pt/C +RuO2, Co9S8 and P-Co9S8 cells.

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MOFs衍生的磷掺杂Co₉S₈增强氧析出和还原反应: 迈向高性能锌空气电池

Enhanced oxygen evolution and reduction by phosphorus-doped Co₉S₈ derived from MOFs: Toward high-performance zinc-air batteries

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