原位制备水氧化铁基薄膜电极研究★

doi:10.6023/A26060188

研究通讯

原位制备水氧化铁基薄膜电极研究^★

徐昕^a,b, 廖芳杰^a,b, 佟振合^a,b, 吴骊珠^a,b,*

^a中国科学院理化技术研究所光化学转换与功能材料重点实验室中国科学院-香港大学新材料合成和检测联合实验室新基石科学实验室北京 100190;
^b中国科学院大学未来技术学院北京 100049

投稿日期:2026-06-08
作者简介:^★“纪念兰州大学化学学科创建80周年”专辑
基金资助:
国家重点研发计划(No. 2022YFA1502900 and 2022YFA0911900)、国家自然科学基金(No. 22588101 and 92356309)和新基石科学基金会资助项目.

In-situ Preparation of Iron-based Film Electrode for Water Oxidation

Xu Xin^a,b, Liao Fang-jie^a,b, Tung Chen-ho^a,b, Wu Li-zhu^a,b,*

^aKey Laboratory of Supramolecular Photochemistry and HKU-CAS Joint Laboratory on New Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190;
^bSchool of Future Technology, University of Chinese Academy of Sciences, Beijing 100049

Received:2026-06-08
Contact: ^*E-mail: lzwu@mail.ipc.ac.cn
Supported by:
National Key R&D Program of China (No. 2022YFA1502900 and 2022YFA0911900), the National Natural Science Foundation of China (No. 22588101 and 92356309), the Strategic Priority Research Program of the Chinese Academy of Science (No. XDB0960000), and New Cornerstone Science Foundation.

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摘要/Abstract

电催化分解水制氢是新能源开发的重要策略。其中,水氧化反应具有较高的能量势垒和缓慢的动力学,被视为该过程的瓶颈。因此迫切需要开发高效稳定的阳极电极以提高水分解效率。本文以铁（III）配合物[Fe(bpy-pma)]（bpy-pma=N¹-(2-([2,2'-bipyridin]-6-yl)propan-2-yl)-N²-methyloxalamide）为前体,在pH=9.0的BBS中通过电沉积法原位制备了氧化铁薄膜电极,能够在过电位540 mV下催化水氧化反应,电流密度为1 mA cm^-2,塔菲尔斜率为85 mV dec^-1。1.3 V电压下进行控制电位电解,电流密度可达到7.3 mA cm^-2,保持10小时以上未出现电流衰减。配体的引入,不仅影响薄膜形貌,还提高了薄膜中铁负载量及其电催化活性,克服了铁离子在中性到碱性条件下易形成沉淀析出,导致薄膜电极质量差、效率低、稳定性差等问题。

关键词: 水氧化, 电催化, 电沉积, 催化薄膜, 高稳定性

The depletion of petroleum reserves and imminent environmental problems has promoted the pursuit of clean and sustainable energy. Electrocatalytic water splitting to produce hydrogen represents a critical strategy in the field of new energy development. Water oxidation reaction is regarded as the bottleneck restricting the process due to the high energy demanding and slow kinetics process. Development of efficient and stable anode electrodes to enhance the efficiency of water splitting is essential. Here, Fe-based film electrode was in-situ prepared by electrodeposition directly from complex [Fe(bpy-pma)] (bpy-pma=N¹-(2-([2,2'-bipyridin]-6-yl)propan-2-yl)-N²-methyloxalamide) in BBS (pH=9.0). The morphology, composition, structure and catalytic activity of the catalytic film were characterized using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS) and electrochemical measurements. The results indicate that the surface of the Fe-cat electrode is covered with cubic Fe₂O₃ nanoparticles. Inductively coupled plasma (ICP) measurements showed that 1.8 μg cm^-2 of Fe was deposited on the Fe-cat electrode. The catalytic film exhibits an overpotential of 540 mV at 1 mA cm^-2 current density and a Tafel slop of 85 mV dec^-1for water oxidation in carbonate/bicarbonate solution (pH=9.75). A stable current density of 7.3 mA cm^-2 over 10 h was observed during controlled potential electrocatalysis (CPE) with an applied potential of 1.3 V. No current attenuation occurred in the longer-term CPE for 24 h. The electrolysis products, H₂ and O₂, were detected using gas chromatography (GC), yielding a calculated Faradaic efficiency of 99%. During the electrodeposition process, the slow dissociation of ligands effectively suppresses Fe(OH)₃ precipitation, yielding ultrathin nanomembranes with uniform density. Compared with FeCl₃ as a precursor, ligand coordination not only markedly modulates the film morphology but also greatly enhances the iron loading and electrocatalytic activity. This strategy overcame the problems of poor quality, low efficiency and poor stability of film electrode caused by the precipitation of iron ions under neutral to alkaline conditions.

Key words: water oxidation, electrocatalysis, electrodeposition, catalytic film, high stability

引用此文

徐昕, 廖芳杰, 佟振合, 吴骊珠. 原位制备水氧化铁基薄膜电极研究^★[J]. 化学学报, doi: 10.6023/A26060188.

Xu Xin, Liao Fang-jie, Tung Chen-ho, Wu Li-zhu. In-situ Preparation of Iron-based Film Electrode for Water Oxidation[J]. Acta Chimica Sinica, doi: 10.6023/A26060188.

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