构建锐钛矿-金红石TiO2异质结构调控竞争吸附以缓解Ru在碱性氢氧化反应中的羟基毒化效应

doi:10.1016/S1872-2067(25)64853-4

催化学报 ›› 2026, Vol. 82: 74-83.DOI: 10.1016/S1872-2067(25)64853-4

构建锐钛矿-金红石TiO₂异质结构调控竞争吸附以缓解Ru在碱性氢氧化反应中的羟基毒化效应

高杰^a, 刘静^a^,^*(), 王梦迪^a, 孙诺^a, 胡皓^a, 崔学晶^a, 周新^b^,^c^,^*(), 姜鲁华^a^,^*()

^a青岛科技大学材料科学与工程学院, 山东青岛 266042
^b辽宁师范大学生物与化学交叉学科研究中心, 辽宁大连 116029
^c大连大学环境与化学工程学院, 辽宁大连 116622

收稿日期:2025-07-19 接受日期:2025-09-03 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: liuj955@qust.edu.cn (刘静),zhouxin@dlu.edu.cn (周新),luhuajiang@qust.edu.cn (姜鲁华).
基金资助:
国家自然科学基金(22279067);山东省自然科学基金重大基础研究计划项目(ZR2022ZD10)

Alleviating hydroxyl poisoning on Ru through competitive adsorption regulation using anatase-rutile TiO₂ heterostructures in alkaline hydrogen oxidation reaction

Jie Gao^a, Jing Liu^a^,^*(), Mengdi Wang^a, Nuo Sun^a, Hao Hu^a, Xuejing Cui^a, Xin Zhou^b^,^c^,^*(), Luhua Jiang^a^,^*()

^aCollege of Materials Science & Engineering, Qingdao University of Science & Technology, Qingdao 266042, Shandong, China
^bInterdisciplinary Research Center for Biology and Chemistry, Liaoning Normal University, Dalian 116029, Liaoning, China
^cCollege of Environment and Chemical Engineering, Dalian University, Dalian 116622, Liaoning, China

Received:2025-07-19 Accepted:2025-09-03 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: liuj955@qust.edu.cn (J. Liu),zhouxin@dlu.edu.cn (X. Zhou),luhuajiang@qust.edu.cn (L. Jiang).
Supported by:
National Natural Science Foundation of China(22279067);Major Funda mental Research Program of Natural Science Foundation of Shandong Province(ZR2022ZD10)

摘要/Abstract

摘要：

阴离子交换膜燃料电池(AEMFCs)凭借其经济性与高能量密度, 成为极具应用前景的能源转换装置. 然而, 碱性条件下氢氧化反应(HOR)速率显著低于酸性体系, 严重制约了AEMFC技术的发展, 亟需高活性、高稳定性的非铂催化剂. 钌(Ru)因具有适宜的氢结合能和较低成本, 被认为是碱性HOR中极具潜力的铂(Pt)替代催化剂, 但其在高电位(>0.1 V vs. RHE)下, 易因吸附态羟基(OH)吸附中毒, 导致活性位点被阻塞, 限制了实际应用.

近年来研究集中于引入亲氧性载体(如过渡金属氧化物等)以调控OH吸附行为, 进而调节中间体结合能并提升催化剂稳定性. 然而, 多数Ru-氧化物型催化剂在高电位下仍面临稳定性不足的问题, 其根本原因在于载体与Ru之间对OH的竞争性吸附. 基于此, 本文提出通过调控Ru与载体对OH的竞争吸附, 实现Ru表面OH覆盖度的降低, 并提高其催化活性. 锐钛矿(A-TiO₂)和金红石(R-TiO₂)作为典型的金属氧化物载体, 因晶体结构和缺陷特性不同, 可通过与Ru的强金属-载体相互作用(SMSI)调控Ru的电子结构和吸附性能, 从而影响催化反应中间体的吸附和脱附行为. 本文设计了一种三相异质结构催化剂(Ru-P25-TiO₂), 该催化剂由Ru与金红石(R-)和锐钛矿(A-)两相TiO₂复合组成. 该催化剂展现出卓越的HOR活性, 达到0.82 mA μg_Ru^-1, 并在高达0.9 V vs. RHE的电位下表现出优异的电化学稳定性, 成为当前HOR领域的先进电催化剂. 进一步结合程序升温脱附、原位红外光谱及理论计算研究发现, 该性能提升归因于强金属-载体相互作用带来的优化电子分布和Ru表面定制化的d带结构, 从而削弱了氢和羟基的结合能. 高度亲氧性的P25-TiO₂有助于羟基在其表面吸附, 并在催化剂/电解质界面建立连续的氢键网络, 促进OH^-的传输, 有效缓解了Ru表面的OH竞争性吸附与毒化. 锐钛矿与金红石两相TiO₂的协同作用, 使Ru同时具备优异的活性和出色的电化学稳定性.

综上, 本研究揭示了双相TiO₂在调控Ru电催化性能中的本征作用, 证实了异质结构设计在缓解催化剂中毒、协同提升活性与稳定性中的有效性, 为开发高效稳定的电催化剂提供了一种可推广的协同异质结构设计策略.

关键词: 锐钛矿TiO₂, 金红石TiO₂, 钌, 协同效应, 氢氧化反应

Abstract:

Ruthenium (Ru) is a promising electrocatalyst for the alkaline hydrogen oxidation reaction (HOR), yet it suffers from deactivation at higher potentials due to excessive oxophilicity, which leads to hydroxyl adsorption poisoning. Here, we report a tri-phase heterostructured catalyst (Ru-P25-TiO₂) comprising Ru with anatase (A-) and rutile (R-)TiO₂. This catalyst exhibits remarkable HOR activity, delivering 0.82 mA μg_Ru^-1 along with superior electrochemical stability up to 0.9 V vs. RHE, positioning it as the state-of-the-art electrocatalyst for HOR. This enhanced performance is attributed to the optimized electron distribution and a tailored d band structure at the Ru surface, enabled by strong metal and support interaction, which weakens both hydrogen binding energy and hydroxyl binding energy. The highly oxyphilic P25-TiO₂ facilitates hydroxyl adsorption and establishes a continuous hydrogen-bond network at the catalyst/electrolyte interface, thereby promoting OH⁻ transport and alleviating competitive OH adsorption on the Ru surface. The synergistic interplay between anatase and rutile TiO₂ ideally endows Ru with both superior activity and excellent electrochemical stability. This work not only unravels the intrinsic role of biphasic TiO₂ in tailoring Ru electrocatalysis but also provides a generalizable synergistic heterostructure design strategy for developing efficient and durable electrocatalysts.

Key words: Anatase TiO₂, Rutile TiO₂Ruthenium, Synergistic interplay, Hydrogen oxidation reaction

高杰, 刘静, 王梦迪, 孙诺, 胡皓, 崔学晶, 周新, 姜鲁华. 构建锐钛矿-金红石TiO₂异质结构调控竞争吸附以缓解Ru在碱性氢氧化反应中的羟基毒化效应[J]. 催化学报, 2026, 82: 74-83.

Jie Gao, Jing Liu, Mengdi Wang, Nuo Sun, Hao Hu, Xuejing Cui, Xin Zhou, Luhua Jiang. Alleviating hydroxyl poisoning on Ru through competitive adsorption regulation using anatase-rutile TiO₂ heterostructures in alkaline hydrogen oxidation reaction[J]. Chinese Journal of Catalysis, 2026, 82: 74-83.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64853-4

https://www.cjcatal.com/CN/Y2026/V82/I3/74

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Fig. 1. (a) Schematic diagram of the design strategy of Ru-TiO2. (b) AC HAADF-STEM image of Ru-P25-TiO2. (c) Elemental mapping images of Ru-P25-TiO2. TEM images of Ru-P25-TiO2 (d), Ru-R-TiO2 (e), and Ru-A-TiO2 (f). The insert is the histogram for Ru particle size distribution. (g) AC HRTEM image of Ru-P25-TiO2. g1 and g2 are the enlarged images of the smaller box region. (h) HRTEM image of Ru-R-TiO2. h1 and h2 are the enlarged images of the smaller box region. (i) HRTEM image of Ru-A-TiO2. i1 and i2 are the enlarged images of the smaller box region.

Fig. 2. Chemical state and atomic coordination environment of Ru-P25-TiO2, Ru-A-TiO2, and Ru-R-TiO2. C 1s, Ru 3d (a) and Ti 2p, Ru 3p (b) XPS spectra of Ru-P25-TiO2, Ru-A-TiO2, and Ru-R-TiO2. (c) Valance band XPS spectra of Ru-P25-TiO2, Ru-A-TiO2, and Ru-R-TiO2. Normalized Ru K-edge XANES spectra (d) and Ru K-edge FT-EXAFS spectra (e) of Ru-P25-TiO2, Ru-R-TiO2, Ru foil, and RuO2. (f) The wavelet transform EXAFS contour plots of Ru-P25-TiO2, Ru-R-TiO2, Ru foil, and RuO2. Normalized Ti K-edge XANES spectra (g) and Ti K-edge FT-EXAFS spectra (h) of Ru-P25-TiO2, Ru-R-TiO2, Ti foil, TiO2-A, and TiO2-R.

Fig. 3. Electrocatalytic HOR performances. (a) HOR polarization curves in H2-saturated 0.1 mol L-1 KOH at a scan rate of 10 mV s-1 of Ru-P25-TiO2, Ru-R-TiO2, Ru-A-TiO2, and Ru/C. Tafel plots (b) and comparison of j0,s and jk,m (c) of Ru-P25-TiO2, Ru-R-TiO2, Ru-A-TiO2, and Ru/C. (d) HOR polarization curves of Ru-P25-TiO2 before and after 5k, 10k cycles of ADT. (e) Chronoamperometry curves of Ru-P25-TiO2 and Ru-R-TiO2 at 0.9 V vs. RHE in H2-saturated 0.1 mol L-1 KOH at 400 rpm. (f) Deactivation potentials and mass activities of Ru-based nonprecious metal electrocatalysts for the alkaline HOR.

Fig. 4. In-situ SEIRAS spectra recorded at potentials from 0.35 to -0.05 V of Ru-P25-TiO2 (a,c) and Ru-R-TiO2 (b,d) electrocatalyst in 0.1 mol L-1 NaOH. Deconvolution of the O-H stretching vibration features of in-situ SEIRAS spectra recorded at 0.15 V (e) and 0.35 V (f) for Ru-P25-TiO2 and Ru-R-TiO2.

Fig. 5. DFT results of the model catalysts. The projected d-band states in Ru-A-TiO2 (a) and Ru-R-TiO2 (b). (c) The hydroxide binding energy of Ru-A-TiO2 and Ru-R-TiO2 on Ru and Ti sites. (d) The hydrogen binding energy of Ru-A-TiO2 and Ru-R-TiO2. (e) Free energy profiles of HOR over Ru-A-TiO2 and Ru-R-TiO2.

Fig. 6. Schematic illustration of the mechanism for the enhanced HOR activities of Ru-P25-TiO2.

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构建锐钛矿-金红石TiO₂异质结构调控竞争吸附以缓解Ru在碱性氢氧化反应中的羟基毒化效应

Alleviating hydroxyl poisoning on Ru through competitive adsorption regulation using anatase-rutile TiO₂ heterostructures in alkaline hydrogen oxidation reaction

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