WO2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池

doi:10.1016/S1872-2067(26)65066-8

催化学报 ›› 2026, Vol. 86: 302-314.DOI: 10.1016/S1872-2067(26)65066-8

WO_2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池

余旭^a^,^b^,¹, 田汉^a^,¹, 于子怡^a, 孔繁涛^a, 王敏^a, 申如香^a, 崔香枝^a^,^b^,^c^,^*(), 施剑林^a^,^b

^a 中国科学院上海硅酸盐研究所, 上海 200050
^b 中国科学院大学材料科学与光电技术中心, 北京 100049
^c 中国科学院大学杭州高等研究院化学与材料科学学院, 浙江杭州 310024

收稿日期:2025-10-28 接受日期:2025-12-16 出版日期:2026-07-05 发布日期:2026-06-12
通讯作者: ^*电子信箱: cuixz@mail.sic.ac.cn (崔香枝).
作者简介:第一联系人：¹共同第一作者.
基金资助:
国家自然科学基金(52172110);上海“科技创新行动计划”国际科技合作项目(23520710600);东方英才计划拔尖(E51SQ61601);“科技创新行动计划”自然科学基金(24ZR1475700)

WO_2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells

Xu Yu^a^,^b^,¹, Han Tian^a^,¹, Ziyi Yu^a, Fantao Kong^a, Min Wang^a, Ruxiang Shen^a, Xiangzhi Cui^a^,^b^,^c^,^*(), Jianlin Shi^a^,^b

^a Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
^b Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
^c School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, Zhejiang, China

Received:2025-10-28 Accepted:2025-12-16 Online:2026-07-05 Published:2026-06-12
About author:First author contact:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(52172110);Shanghai “Science and Technology Innovation Action Plan” intergovernmental international science and technology cooperation project(23520710600);Eastern Talent Plan Leading Project(E51SQ61601);Shanghai “Science and Technology Innovation Action Plan” Natural Science Foundation(24ZR1475700)

摘要/Abstract

摘要：

碱性阴离子交换膜燃料电池(AEMFCs)因其在氢能转换领域的应用潜力而备受关注, 其关键优势在于可使用非贵金属氧还原催化剂及廉价电池组件, 有望超越高铂载量的质子交换膜燃料电池性能. 然而, 碱性环境下的氢氧化反应(HOR)动力学比酸性环境中慢约2-3个数量级, 严重制约了AEMFCs的性能发展. 同时, 开发具有优异CO耐受性的阳极催化剂, 被视为利用低成本粗氢、提升AEMFCs经济可行性的关键. 在碱性HOR过程中, 涉及吸附的氢中间体(H_ad)和羟基中间体(OH_ad)吸附的Volmer步骤通常是决速步, 因此除了氢结合能(HBE), 羟基结合能(OHBE)也成为描述催化性能的关键指标. 钌因其类铂的催化特性及更低的成本, 被视为有前景的铂替代品, 但其仍存在OH_ad吸附位点不足、抗CO中毒能力弱等问题, 且在AEMFCs中的实际性能常不及商用Pt-C催化剂. 因此, 亟需设计新型高效、耐CO的钌基碱性HOR电催化剂.

本研究提出一种双位点协同催化机制, 旨在通过优化OHBE来提升催化剂碱性HOR性能. 具体而言, 在氮掺杂碳载体上构建了由高亲氧性WO_2.72团簇修饰的超细Ru纳米团簇催化剂(记为Ru-WO_2.72-NC). 该设计思路的创新性在于: WO_2.72团簇能特异性吸附OH_ad物种, 而Ru位点则负责吸附和解离氢气产生活性H_ad, 两者协同作用共同促进Volmer决速步骤的进行, 从而显著加速碱性HOR动力学. 研究结果表明, 所构建的Ru-WO_2.72-NC催化剂展现出优异的HOR活性, 其质量活性约为商用Pt-C的8倍. 更重要的是, 基于该催化剂的AEMFCs在纯H₂燃料下表现出高达1.193 W cm^-2的峰值功率密度, 即使在含50 ppm CO的H₂混合气中, 峰值功率密度仍能维持在1 W cm^-2以上, 显著优于未修饰的Ru-NC催化剂, 体现了卓越的活性和CO耐受性. 原位拉曼光谱等实验结果证实了其高性能源于Ru与WO_2.72之间的双位点协同效应:^-WO_2.72位点吸附的OH_ad能有效与Ru位点上的H_ad结合生成水, 促进Volmer步骤; 同时, 这些OH_ad也能与Ru上吸附的有毒CO物种反应, 实现CO分子的及时清除, 从而获得快速的HOR动力学和有效的CO解毒能力. 该工作不仅成功制备了一种高性能、高CO耐受性的碱性HOR阳极催化剂, 而且从机理上明确了双位点协同催化对优化OHBE和反应路径的关键作用.

综上, 本文通过构建Ru-WO_2.72-NC双位点协同催化体系, 为设计和研究高活性、高CO耐受性的碱性HOR催化剂提供了新的思路和理论依据. 该策略对于推动AEMFCs阳极催化剂的成本降低和性能提升具有重要价值, 也为深入理解碱性HOR反应机理与催化剂构效关系开辟了新的途径.

关键词: 阴离子交换膜燃料电池, 碱性氢气氧化反应, CO耐受性, 氧化钨, 协同催化

Abstract:

A dual-site synergistic catalytic mechanism is proposed to optimize the OHad binding energy (OHBE) by constructing ultrafine Ru nanoclusters modified with highly oxygenophilic WO_2.72 clusters in nitrogen-doped carbon carriers, which can optimize the adsorptions of OH_ad and active hydrogen species, respectively, resulting in a marked increase in hydrogen oxidation reaction (HOR) activity. The constructed Ru-WO_2.72-NC shows a HOR mass activity about 8 times that of Pt-C, and the corresponding alkaline exchange membrane fuel cells demonstrate rather higher peak power densities than Ru-NC with 1.193 W cm^-2 and more than 1 W cm^-2 in H₂ fuel and CO/H₂ mixtures, respectively. The excellent alkaline HOR performance of Ru-WO_2.72-NC is attributed to the adsorption of OH_ad species by WO_2.72 clusters, which synergizes with the adsorption and dissociation of hydrogen on Ru to facilitate the Volmer step. The success in constructing dual-site synergistic catalysis of Ru-WO_2.72-NC anode provides valuable insight and new guidelines for designing and studying high-activity alkaline HOR catalysts.

Key words: Anion exchange membrane fuel cells, Alkaline hydrogen oxidation reaction, CO resistance, Tungsten oxide, Synergistic catalysis

余旭, 田汉, 于子怡, 孔繁涛, 王敏, 申如香, 崔香枝, 施剑林. WO_2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池[J]. 催化学报, 2026, 86: 302-314.

Xu Yu, Han Tian, Ziyi Yu, Fantao Kong, Min Wang, Ruxiang Shen, Xiangzhi Cui, Jianlin Shi. WO_2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells[J]. Chinese Journal of Catalysis, 2026, 86: 302-314.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65066-8

https://www.cjcatal.com/CN/Y2026/V86/I7/302

图/表 6

Scheme 1. Scheme of the Ru-WO2.72-NC design strategy for efficient HOR and high CO-tolerance.

Fig. 1. Synthetic schematic (a), TEM (b), HRTEM (c), SAED (d), HAADF-STEM (e), andTEM-EDS elemental mappings (f) images of Ru-WO2.72-NC.

Fig. 2. XRD (a), Raman (b), and UV-vis-NIR (c) spectra of Ru-WO2.72-NC. High-resolution XPS spectra of Ru 3p (d), W 4f (e), and O 1s (f) of Ru-NC, WO2.72-NC and Ru-WO2.72-NC. (g) EPR spectra of the as-prepared samples. Ru K-edge XANES (h), EXAFS (i), and WT-EXAFS (j) spectra of the samples.

Fig. 3. HOR polarization curves (a), Tafel plots (b), and LSV curves (c) at varying rotating speeds (inset: K-L plots) for as-prepared catalysts and Pt-C. (d) Comparisons of E1/2, current densities and mass-normalized performance of Ru-WO2.72-NC (red), Ru-NC (blue) and Pt-C (green). (e) Relative current-time chronoamperometry curves of different catalysts at 0.1 V. (f) LSV curves of Ru-WO2.72-NC and Pt-C before and after ADT. (g) Polarization and power density curves of AEMFCs. (h) Mass current density and cost accounting of the catalysts in AEMFCs.

Fig. 4. LSV curves in pure H2, CO/H2 and after ADT in CO/H2 of Ru-WO2.72-NC (a) and Pt-C (b). (c) i-t curves of different catalysts in CO/H2 atmosphere. Polarization and power density curves of AEMFCs in 50 ppm CO/H2 anodic atmosphere (d) and corresponding PPD decay histograms (e). (g) CO-TPD of the samples. (h)Background-corrected VB spectra of Ru-WO2.72-NC and Pt-C. (i) CO-stripping voltammograms of Ru-WO2.72-NC and Pt-C.

Fig. 5. H2-TPD spectra (a) and zeta potential (b) of as-prepared catalysts. In-situ electrochemical Raman spectra on Ru-WO2.72-NC surfaces during HOR in the range of 1000-1800 cm-1 (c) and 3000-3800 cm-1 (d). (e) The reaction pathways of Ru-WO2.72-NC and Ru for alkaline HOR. (f) Schematic representation of the alkaline HOR mechanism for the proposed Ru-WO2.72-NC catalyst.

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WO_2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池

WO_2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells

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WO2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池

WO2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells

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WO_2.72调控的Ru团簇增强双位点吸附用于高效抗CO阴离子交换膜燃料电池

WO_2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells