单原子镧系元素掺杂增强界面自由水供应以促进高效酸性电解水析氧

doi:10.1016/S1872-2067(26)65111-X

催化学报 ›› 2026, Vol. 89: 196-206.DOI: 10.1016/S1872-2067(26)65111-X

单原子镧系元素掺杂增强界面自由水供应以促进高效酸性电解水析氧

郝晓珊^,¹, 卢珊珊^,¹(), 程传祺^,¹, 阮青青, 张兵^*(), 史艳梅^*()

天津大学分子+研究院,理学院化学系,天津 300072

收稿日期:2025-12-19 接受日期:2026-02-21 出版日期:2026-10-18 发布日期:2026-09-01
通讯作者: *电子信箱: lss133@tju.edu.cn (卢珊珊),
yanmeishi@tju.edu.cn (史艳梅),
bzhang@tju.edu.cn (张兵).
作者简介:
¹共同第一作者.
基金资助:
国家重点研发计划(2025YFA1511000);国家自然科学基金(22275134);国家自然科学基金(22579125);国家自然科学基金(22505175);全国博士后创新人才支持计划(BX20250114)

Promoting interfacial free water supply through the hydration of single-atom lanthanide doping for acidic water oxidation

Xiaoshan Hao^,¹, Shanshan Lu^,¹(), Chuanqi Cheng^,¹, Qingqing Ruan, Bin Zhang^*(), Yanmei Shi^*()

Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, Tianjin 300072,China

Received:2025-12-19 Accepted:2026-02-21 Online:2026-10-18 Published:2026-09-01
Contact: *E-mail: lss133@tju.edu.cn (S. Lu),yanmeishi@tju.edu.cn (Y. Shi),bzhang@tju.edu.cn (B. Zhang).
About author:
¹ Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2025YFA1511000);National Natural Science Foundation of China(22275134);National Natural Science Foundation of China(22579125);National Natural Science Foundation of China(22505175);China National Postdoctoral Program for Innovative Talents(BX20250114)

摘要/Abstract

摘要：

质子交换膜水电解(PEMWE)是绿色制氢的核心技术, 其发展主要受阳极电催化材料制约. 阳极的析氧反应(OER)为四电子转移过程, 动力学缓慢; 并且PEMWE的酸性强氧化环境易导致阳极催化材料因氧化溶解和结构坍塌而失活, 严重制约了PEMWE的稳定性. 目前商业化的IrO₂和RuO₂等贵金属阳极催化材料成本高昂，亟需开发低成本、高活性、长寿命的酸性非贵金属OER催化剂. Co₃O₄因其资源丰富和高本征活性被视为有潜力的替代材料, 但其在酸性条件下晶格氧易参与反应(即LOM机制), 导致Co-O键断裂, 稳定性差. 此外, 近期研究发现, 界面水结构对水参与的电催化反应性能具有显著影响, 其中无氢键束缚的界面自由水最容易解离, 因此增加界面自由水的供给是提升水分解效率的新思路.

本研究提出了一种通过掺杂单原子镧系金属元素来调控Co₃O₄电子结构与界面水环境, 从而同步提升酸性OER活性和稳定性的新策略. 以镧(La)为例, 首先利用理论计算预测了La掺杂能够提高界面自由水含量, 增强Co-O键稳定性, 促进OER活性. 随后, 通过温和的电化学插层法成功制备了单原子La掺杂的Co₃O₄(记为La-Co₃O₄). X-射线衍射、球差校正扫描透射电镜及X射线吸收精细结构谱等结构表征证实, La-Co₃O₄中的La以单原子形式均匀分散于Co₃O₄基体中, 并有效调控了Co的电子结构. 电化学测试表明, La-Co₃O₄在0.5 mol L^‒1 H₂SO₄溶液中表现出优异的OER活性和稳定性. 活性方面, La-Co₃O₄的质量活性和本征活性均提升显著, 在10 mA cm^‒2电流密度下仅产生288 mV的过电位. 稳定性方面, Co在酸性溶液中长时间测试导致的溶出得到了有效抑制, 样品能够在10 mA cm^‒2电流密度下稳定运行230 h. 借助原位拉曼、原位红外、差分电化学质谱等手段开展机理分析, 证实单原子La掺杂通过双重协同作用提升催化性能. 一方面单原子La通过强化Co-O键, 有效抑制了LOM机制, 显著提升了催化剂的电化学稳定性; 另一方面是由于镧系离子高的电荷密度和水合能, 掺杂在Co₃O₄表面的La原子能通过强水合作用自发从电解液中捕获水分子, 原位增加电极表面自由水的供给, 加速水分解动力学. 此外, 本研究还证明除La外, 其他镧系元素(如Pr和Sm)掺杂对Co₃O₄催化酸性OER活性和稳定性亦具有类似的促进作用.

综上, 本研究不仅开发了一种高效、稳定的酸性OER催化剂, 还提出了一种通过单原子镧系金属掺杂调控界面水结构来促进电催化性能的普适性策略, 为设计下一代高效能源材料提供了新思路.

关键词: 酸性析氧反应, 界面水结构, 掺杂, 镧系金属, 晶格氧

Abstract:

Interfacial free water plays a vital role in accelerating electrocatalytic water splitting. However, the low proportion of free water at the interface significantly limits the reaction rate. Herein, we demonstrate a new strategy to increase the interfacial free water supply by doping single lanthanide atoms into Co₃O₄ for acidic oxygen evolution (OER). Taking La as an example, the doped La at the surface of Co₃O₄ spontaneously captures water molecules from the electrolyte through hydration, providing a sufficient free water supply for the OER. In addition, La doping strengthens Co-O bonding, affording strong structural stability. As a result, La-doped Co₃O₄ has a small overpotential of 288 mV at a current density of 10 mA cm^-2 and can remain stable for 230 h. Except for La, other lanthanide elements, such as Sm and Pr, also have similar effects on the OER. Our work not only develops efficient electrocatalysts for the acidic OER but also provides a universal strategy to increase the interfacial free water supply.

Key words: Acidic oxygen evolution reaction, Structure of interfacial water, Doping, Lanthanides, Lattice oxygen

郝晓珊, 卢珊珊, 程传祺, 阮青青, 张兵, 史艳梅. 单原子镧系元素掺杂增强界面自由水供应以促进高效酸性电解水析氧[J]. 催化学报, 2026, 89: 196-206.

Xiaoshan Hao, Shanshan Lu, Chuanqi Cheng, Qingqing Ruan, Bin Zhang, Yanmei Shi. Promoting interfacial free water supply through the hydration of single-atom lanthanide doping for acidic water oxidation[J]. Chinese Journal of Catalysis, 2026, 89: 196-206.

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图/表 6

Fig. 1. Theoretical predictions of La doping into Co3O4. (a) Calculation models of La-Co3O4 for different OER steps. The red, dark blue, pink, and green balls represent O, Co, H, and La, respectively. The O and H in the OER intermediates are highlighted in cyan and light blue, respectively. (b) Calculated density of H2O (top) and O species (bottom) at the surface of Co3O4 and La-Co3O4. (c) Free energy diagrams of the OER over Co3O4 and La-Co3O4 at a bias of 0 V. (d) -pCOHP analysis of Co3O4 and La-Co3O4.

Fig. 2. Preparation and morphology of La-Co3O4. (a) Illustration of the preparation of La-Co3O4. (b) LSV curves of Co3O4 scanning in electrolytes with different La3+ concentrations. (c) XRD patterns of Co3O4 and La-Co3O4. Peaks labeled by asterisk (*) arise from Ti as the substrate. (d) Magnified view of the marked region in (c). (e) TEM image of La-Co3O4. (f) Aberration-corrected HAADF-STEM image of La-Co3O4. (g) HAADF-STEM and corresponding elemental distributing mapping images of La-Co3O4.

Fig. 3. Spectroscopic characterizations of La-Co3O4. (a) Co 2p XPS spectra of Co3O4 and La-Co3O4. (b) La 3d5/2 spectrum of La-Co3O4. (c) Raman spectra of Co3O4 and La-Co3O4. (d) Co K-edge XANES spectra of Co3O4 and La-Co3O4. The Co foil and CoO data are shown for comparison. The inset is the corresponding pre-edge region in (d). (e) Co K-edge EXAFS spectra of Co3O4 and La-Co3O4. (f) O K-edge soft X-ray absorption spectra of Co3O4 and La-Co3O4.

Fig. 4. Electrocatalytic OER performance and reaction mechanism. (a) LSV curves of Co3O4, La-Co3O4, and RuO2. (b) Tafel plots of Co3O4 and La-Co3O4. (c) Nyquist plots of Co3O4 and La-Co3O4 at 1.6 V vs. RHE. (d) I-t curves of Co3O4, La-Co3O4, and RuO2 at 10 mA cm-2. (e) Co 2p XPS spectra of the counter electrode used for Co3O4 and La-Co3O4. (f) Current densities of Co3O4 and La-Co3O4 at 1.7 V as a function of pH. (g) Proportion of 34O2 and 36O2 generated from 18O-labeled Co3O4 and La-Co3O4 tested in H216O. (h) Raman spectra of Co3O4 and La-Co3O4 with the addition of TMA+ at the OCP and 1.7 V.

Fig. 5. In-situ investigations of the effect of La doping. In-situ Raman spectra of Co3O4 (a) and La-Co3O4 (b) in the range of 550-770 cm-1. (c) Corresponding Raman shifts of F2g at different potentials for Co3O4 and La-Co3O4. In-situ Raman spectra of Co3O4 (d) and La-Co3O4 (e) in the range of 2800-4000 cm-1. Corresponding proportion (f) and Raman shift (g) of free water for Co3O4 and La-Co3O4.

Fig. 6. Universality of the performance promotion through other lanthanide-element doping. (a) LSV curves of Co3O4, Sm-Co3O4, and Pr-Co3O4. (b) I-t curves of Co3O4, Sm-Co3O4, and Pr-Co3O4 at 10 mA cm-2. In-situ Raman spectra of Sm-Co3O4 (c) and Pr-Co3O4 (d) in the range of 2800-4000 cm-1. Corresponding proportion (e) and Raman shift (f) of free water for Sm-Co3O4 and Pr-Co3O4.

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单原子镧系元素掺杂增强界面自由水供应以促进高效酸性电解水析氧

Promoting interfacial free water supply through the hydration of single-atom lanthanide doping for acidic water oxidation

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