质子交换膜电解槽中铱基催化剂的活性-稳定性协同提升

doi:10.1016/S1872-2067(26)64962-5

催化学报 ›› 2026, Vol. 85: 193-203.DOI: 10.1016/S1872-2067(26)64962-5

质子交换膜电解槽中铱基催化剂的活性-稳定性协同提升

张凯杨^a, 李惠惠^b, 王叔豪^b, 姚瑞^a, 李晋平^a^,^c(), 赵川^b(), 刘光^a()

^a 太原理工大学化学与化工学院, 气体能源高效清洁利用山西省重点实验室, 山西太原 030024, 中国
^b 新南威尔士大学化学学院, 悉尼, 澳大利亚
^c 怀柔实验室山西研究院, 山西太原 030031, 中国

收稿日期:2025-09-16 接受日期:2025-10-27 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: liuguang@tyut.edu.cn (刘光),
chuan.zhao@unsw.edu.au (赵川),
jpli211@hotmail.com (李晋平).
基金资助:
国家自然科学基金(U22A20418);国家自然科学基金(22578302);澳大利亚研究委员会基金(IC200100023);澳大利亚研究委员会基金(DP250101509);澳大利亚研究委员会基金(FL250100099)

Breaking the activity-stability trade-off of iridium-based catalysts for proton exchange membrane water electrolyzers

Kaiyang Zhang^a, Huihui Li^b, Shuhao Wang^b, Rui Yao^a, Jinping Li^a^,^c(), Chuan Zhao^b(), Guang Liu^a()

^a College of Chemistry and Chemical Engineering, Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^b School of Chemistry, The University of New South Wales, Sydney, New South Wales 2052, Australia
^c Shanxi Research Institute of Huairou Laboratory, Taiyuan 030031, Shanxi, China

Received:2025-09-16 Accepted:2025-10-27 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: liuguang@tyut.edu.cn (G. Liu),
chuan.zhao@unsw.edu.au (C. Zhao),
jpli211@hotmail.com (J. Li).
Supported by:
National Natural Science Foundation of China(U22A20418);National Natural Science Foundation of China(22578302);support from Australian Research Council(IC200100023);support from Australian Research Council(DP250101509);support from Australian Research Council(FL250100099)

摘要/Abstract

摘要：

质子交换膜电解槽(PEMWEs)制氢技术具备快速响应、高电流密度与高纯度产气等优势, 是极具前景的绿氢制取方式. 然而, 其广泛应用受限于缓慢的阳极析氧反应(酸性OER)动力学及苛刻的反应环境, 因此亟需开发高效稳定的催化剂. 铱(Ir)基催化剂仍是当前应用于酸性OER最具前景的催化材料, 但其面临着活性低、稳定性差及成本高等问题. 当前, 对于Ir基催化剂的设计面临着平衡活性-稳定性的问题, 单一的改性方法难以无法打破该限制.因此, 本文旨在通过钴(Co)掺杂与钨(W)载体引入的双重改性策略, 在低Ir载量的情况下实现催化剂活性与稳定性的综合提升.

基于Co掺杂可实现Ir位点的化学环境调控以及变价金属W具有“电子缓冲效应”的设计思路, 本文通过磁控溅射和单极脉冲电沉积成功制备了W负载的Co掺杂氧化铱(Co-IrO_x/W)催化剂. 该催化剂在三电极体系, 0.5 mol L^-1 H₂SO₄的模拟测试环境下, 其酸性OER过程达到10 mA cm^-2的电流密度仅需209 mV, 并且在400 mA cm^-2的极高电流密度下可实现50 h以上的稳定性测试. 在Ir负载量为0.262 mg cm^-2的条件下, 使用Co-IrO_x/W||Pt/C膜电极(MEA)用于PEMWEs测试时, 达到1 A cm^-2的电流密度所需的槽压为1.86 V. 此外, 该MEA装配的PEMWEs可实现1000 h的长期稳定测试, 并表现出6.8 µV h^-1的极低衰减率, 展现出了优异的工业化应用潜力. 电化学测试分析发现, Co-IrO_x/W在降低活化能、加速去质子化及电荷快速转移方面表现出更强的能力, 进而实现优异的酸性OER活性. 物理表征分析及密度泛函理论计算表明, Co-IrO_x/W的活性提升归因于Co掺杂改善了Ir位点的化学环境, 引起Ir位点的d带中心上移, 强化了反应过程中催化活性中心与含氧中间体的吸附能力, 进而加速了OER动力学. 此外, 在稳定性方面, 对电化学测试后的Co-IrO_x/W结构分析发现, W载体构建的W-O-Ir界面配位可实现电子重分布动态抑制Ir位点的过度氧化, 维持催化剂的结构完整性, 从而增强Co-IrO_x/W的抗衰减能力.

综上, 本研究采用一种双重改性策略, 以打破单一方法制备Ir基催化剂在平衡活性与稳定性方面的固有局限. 这种原子掺杂-载体工程的协同作用, 在Ru基及非贵金属Co基酸性析氧催化剂体系中有望展现出巨大的拓展潜力, 有望实现Ru基及Co基催化剂在PEMWEs中实现高效持久运行.

关键词: 质子交换膜电解槽, 析氧反应, 铱基催化剂, 掺杂, 载体

Abstract:

Achieving both high activity and stability remains a key bottleneck for Ir-based catalysts in the acidic oxygen evolution reaction (OER) for proton exchange membrane water electrolyzers (PEMWEs). Herein, we present a cobalt-doped iridium oxide catalyst coated on tungsten substrate (Co-IrO_x/W) fabricated via a synergistic magnetron sputtering and unipolar pulse electrodeposition strategy. The optimized catalyst demonstrates exceptional acidic OER activity with an ultralow overpotential of 209 mV at 10 mA cm^-2 in 0.5 mol L^-1 H₂SO₄, and a Ir loading only of 0.262 mg cm^-2 in PEMWEs to achieve over 1000 h of stable operation at 1 A cm^-2 with a degradation rate only of 6.8 µV h^-1. Integrated characterization reveals enhanced catalytic capacity of Co-IrO_x/W in activation energy, deprotonation, and charge transfer stemmed from Co doping induced Ir d-band upward, strengthening oxygen-intermediate adsorption and accelerates OER kinetics. Moreover, the W substrate creates a W-O-Ir interfacial coordination that dynamically suppresses over-oxidation of Ir sites via electronic redistribution, thereby enhancing the stability of iridium oxide catalyst. This work offers design insights for OER catalysts to simultaneously overcome activity-stability limitations through rational electronic-structure engineering and support interactions dual design principles, opening avenues for industrial hydrogen production.

Key words: Proton exchange membrane water electrolyzers, Oxygen evolution reaction, Ir-based catalysts, Doping, Support

张凯杨, 李惠惠, 王叔豪, 姚瑞, 李晋平, 赵川, 刘光. 质子交换膜电解槽中铱基催化剂的活性-稳定性协同提升[J]. 催化学报, 2026, 85: 193-203.

Kaiyang Zhang, Huihui Li, Shuhao Wang, Rui Yao, Jinping Li, Chuan Zhao, Guang Liu. Breaking the activity-stability trade-off of iridium-based catalysts for proton exchange membrane water electrolyzers[J]. Chinese Journal of Catalysis, 2026, 85: 193-203.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64962-5

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图/表 6

Fig. 1. (a) Schematic illustration of the synthesis process of Co-IrOx/W. SEM image (b), TEM image (c), HR-TEM image (d), SAED image (e), HAADF-STEM image (f), and corresponding EDS mappings (g) of Co-IrOx/W.

Fig. 2. Raman spectra (a) and High-resolution XPS spectra of Ir 4f (b) of Co-IrOx/W, Co-IrOx, and IrOx/W. (c) Analysis of Ir chemical states in Co-IrO?/W, Co-IrO?, and IrO?/W via Ir 4f XPS spectra. (d) High-resolution XPS spectra of W 4f of Co-IrOx/W and IrOx/W. Ir L3-edge XANES regions (e) and Fourier-transforms of k3-weight Ir L3-edge EXAFS spectra (f) of Co-IrOx/W, Ir foil, and IrO2. W L3-edge XANES regions (g) and Fourier-transforms of k3-weight W L3-edge EXAFS spectra (h) of Co-IrOx/W, W foil, and WO3. (i) Wavelet transforms for the k3-weighted Ir L3-edge and W L3-edge EXAFS signals of Co-IrOx/W.

Fig. 3. LSV curves (a), Overpotential at 10 mA cm-2 and mass activity 1.45 V (b), and Tafel slopes (c) of Co-IrOx/W, Co-IrOx, IrOx/W, and IrO2. (d) TOF values at 250 and 300 mV overpotential of Co-IrOx/W, Co-IrOx, and IrOx/W. (e) CP measurement for Co-IrOx/W and Co-IrOx at different current densities.

Fig. 4. (a) pH dependence of Co-IrOx/W and IrOx/W. (b) Polarization curves of Co-IrOx/W and IrOx/W in the presence or absence of TMAOH in H2SO4 electrolytes. (c) AEM pathways in acidic OER process for Co-IrOx. (d) The comparison of integrated -COHP values for Ir-O hybridization for Co-IrOx and IrOx. (e) Gibbs free-energy and (f) computed DOS diagrams of Co-IrOx and IrOx. (g) Arrhenius plots, (h) Phase peak angles and (i) Linear stored charge versus potential relationships for Co-IrOx/W and IrOx/W.

Fig. 5. (a) CP measurement for Co-IrOx/W and Co-IrOx at 400 mA cm-2, the inset displays the calculated S-number from produced O2/dissolved Ir. (b) Variation of Ir dissolution with time at 400 mA cm-2 for Co-IrOx/W and Co-IrOx. High-resolution XPS spectra of (c) Ir 4f and (d) Co 2p (d) were obtained for Co-IrOx/W and Co-IrOx after electrochemical measurement. (e) High-resolution XPS spectra of O 1s were obtained for Co-IrOx/W before and after electrochemical measurement.

Fig. 6. (a) Schematic diagram of PEMWEs. (b) Polarization curves of PEMWEs using Co-IrOx/W||Pt/C, IrOx/W||Pt/C, and IrO2||Pt/C, inset displays a digital photograph of the PEMWEs device. (c) Nyquist plots of Co-IrOx/W||Pt/C and IrO2||Pt/C at 1.7 V. (d) Breakdown of ohmic, transport, and kinetic losses for Co-IrOx/W||Pt/C. (e) The comparison of ohmic, transport, and kinetic losses for PEMWEs using Co-IrOx/W||Pt/C and IrO2||Pt/C. (f) Chronopotentiometry curve of PEMWEs using Co-IrOx/W||Pt/C and Co-IrOx||Pt/C at 1 A cm-2 current density. (g) Comparison of Co-IrO?/W with reported catalysts in terms of Ir loading and stability.

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质子交换膜电解槽中铱基催化剂的活性-稳定性协同提升

Breaking the activity-stability trade-off of iridium-based catalysts for proton exchange membrane water electrolyzers

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