异质原子掺杂与表面工程协同调控普鲁士蓝衍生物的电子结构为高效水裂解

doi:10.1016/S1872-2067(26)65222-9

催化学报 ›› 2027, Vol. 92: 170-181.DOI: 10.1016/S1872-2067(26)65222-9

异质原子掺杂与表面工程协同调控普鲁士蓝衍生物的电子结构为高效水裂解

刘玉婵^a, 高文婧^a^,^b, 黄沁彤^a, 刘晓雄^c^,^*(), 欧阳慧欢^a, 叶融凯^a, 李旻鸶^d^,^*(), 胡建强^a^,^*()

^a 华南理工大学化学与化工学院, 广东省燃料电池技术重点实验室, 广东省功能分子工程重点实验室, 广东广州 510641
^b 河南省科学院智慧创制研究所, 河南郑州 451162
^c 南方科技大学理学院物理系, 广东深圳 518055
^d 宁波工程学院微纳研究院, 浙江宁波 315211

收稿日期:2026-01-12 接受日期:2026-04-21 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: jqhusc@scut.edu.cn (胡建强),
liuxx@sustech.edu.cn (刘晓雄),
tjminsi@nbut.edu.cn (李旻鸶).
基金资助:
国家自然科学基金(22272058);国家自然科学基金青年科学基金项目(52502271)

Heteroatom doping and surface engineering co-modulated electronic structure of prussian blue analogs for efficient overall water splitting

Yuchan Liu^a, Wenjing Gao^a^,^b, Qintong Huang^a, Xiaoxiong Liu^c^,^*(), Huihuan Ouyang^a, Rongkai Ye^a, Minsi Li^d^,^*(), Jianqiang Hu^a^,^*()

^a Key Laboratory of Fuel Cell Technology of Guangdong Province, Key Laboratory of Functional Molecular Engineering of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China
^b Institute of Intelligent Innovation, Henan Academy of Sciences, Zhengzhou 451162, Henan, China
^c Department of Physics, Southern University of Science and Technology (SUSTech), Shenzhen 518055, Guangdong, China
^d Institute of Micro/Nano Materials and Devices, Ningbo University of Technology, Ningbo 315211, Zhejiang, China

Received:2026-01-12 Accepted:2026-04-21 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: jqhusc@scut.edu.cn (J. Hu),
liuxx@sustech.edu.cn (X. Liu),
tjminsi@nbut.edu.cn (M. Li).
About author:First author contact:CRediT authorship contribution statement
Yuchan Liu: Investigation, Methodology, Data curation, Writing-original draft, Writing-review & editing. Wenjing Gao: Data curation. Qintong Huang: Investigation. Huihuan Ouyang: Data curation. Rongkai Ye: Investigation. Xiaoxiong Liu: Writing-review & editing. Minsi Li: Writing-review & editing. Jianqiang Hu: Conceptualization, Funding acquisition, Writing-review & editing, Project administration, Supervision.
Supported by:
National Natural Science Foundation of China(22272058);Young Scientists Fund of the National Natural Science Foundation of China(52502271)

摘要/Abstract

摘要：

氢能作为清洁高效的能源载体, 是实现能源低碳转型的重要途径. 电解水制氢因原料丰富、产物纯度高且过程无碳排放而成为发展潜力大的制氢策略. 然而, 电解水析氢反应(HER)和析氧反应(OER)的动力学缓慢, 通常需高的过电位, 制约了其能量转换效率. 贵金属催化剂(如Pt/C和RuO₂)在HER和OER中虽有优异的催化活性, 但其资源稀缺且成本高昂. 因此, 开发高效、稳定且低成本的非贵金属电催化剂具有重要的意义. 普鲁士蓝衍生物(PBAs)因其三维框架结构、可调构型、合成工艺简单以及在电催化分解水领域的应用而被广泛关注. 但其实际应用常受结构不稳和活性位点少等不足的限制.

本文采用杂原子掺杂与表面工程协同的策略, 通过两步水热法在泡沫镍(NF)上原位生长V掺杂的镍铁三金属PBAs前驱体(V-NiFe PBAs/NF), 再经低温磷化成功制备了具有优秀稳定性和催化性能的V-NiFeP PBAs/NF立方体纳米材料(NCs)预催化剂. 利用V, Fe和Ni三金属间的协同效应, 通过优化V-NiFeP PBAs/NF NCs的电子结构和重构其活性羟基氧化物, 该V-NiFeP PBAs/NF NCs预催化剂在碱性电解质溶液中表现出优异的双功能催化活性和稳定性. 在OER测试中, V-NiFeP PBAs/NF NCs预催化剂在100 mA·cm^-2电流密度下, 仅需~257 mV的过电位, 比商业RuO₂(~443 mV)降低约42%; 其Tafel斜率为~50.43 mV·dec^-1, 表明V-NiFeP PBAs/NF NCs具有较快的反应动力学和较低的电荷转移阻力(约1.35 Ω); 其有相对较大的电化学活性面积(对应C_dl约为4.3 mF·cm^-2)和暴露更多活性位点, 且在50 mA·cm^-2下能稳定运行超500 h, 说明其有很强的电化学活性和高的稳定性. X-射线光电子能谱和X-射线吸收精细结构结果表明, V掺杂优化了V-NiFeP PBAs/NF NCs催化剂中的金属活性位点Ni和Fe的d带中心, 使反应过程中的决速步能垒降低, 从而提升了其OER催化活性. pH依赖实验和化学探针实验表明, V-NiFeP PBAs/NF NCs遵循晶格氧介导机制. 密度泛函理论计算进一步揭示, 与传统的吸附演化机制相比, V掺杂能够改善电化学重构后真实活性物种对含氧中间体的吸附能力, 明显降低速率控制步骤的能垒, 这也是其OER性能优异的原因. 此外, 得益于V-NiFeP PBAs/NF NCs催化剂的独特结构和组成, 该预催化剂在HER中也表现出良好的活性, 在20 mA·cm^-2下过电位约为170 mV, 在全水裂解中在10 mA·cm^-2电流密度下其可实现约1.59 V的驱动电压.

综上, 本文为理解多元金属磷化物的表面重构提供了实验依据, 揭示了V掺杂与预磷化协同策略可实现催化活性与稳定性兼顾. 该策略有望扩展至Co, Mn等非贵金属体系, 为开发高效稳定的双功能催化剂和高电流密度长寿命水分解催化剂提供设计依据.

关键词: 过渡金属磷化物, 钒掺杂, 表面重构, 氧析出反应, 全水裂解, 晶格氧机制

Abstract:

Overall water splitting based on Prussian blue analogues (PBAs) electrocatalysts has attracted increasing attention due to its tunable structures, facile synthesis, reducing costs and promoting green energy applications. However, it is usually hindered by structural instability and limited active sites of electrocatalysts. Herein, we have constructed vanadium-doped and surface-phosphated NiFeP PBAs/Ni foam (V-NiFeP PBAs/NF) nanocubes (NCs) with excellent stability and catalytic performance by heteroatom doping and surface engineering strategy. Benefiting from optimized electronic structures and reconstructed active oxyhydroxides, the V-NiFeP PBAs/NF NCs as pre-catalysts exhibited exceptional oxygen evolution reaction (OER) activity in alkaline media (~257 mV at 100 mA·cm^-2), which was ~42% lower than commercial RuO₂ (~443 mV) and excellent stability (500 h at 50 mA·cm^-2). Experimental and theoretical results indicated that the V-doping of the V-NiFeP PBAs/NF NCs could effectively modulate its electronic configuration by upward-shifting d-band center of Ni and Fe, thereby increasing its conductivity and active sites. The V-NiFeP PBAs/NF NCs had lower reaction energy barrier for lattice oxygen mechanism pathway than that for adsorption evolution mechanism pathway. The V-NiFeP PBAs/NF NCs had excellent hydrogen evolution (~170 mV at 20 mA·cm^-2) and overall water splitting performance (~1.59 V at 10 mA·cm^-2). This work provides a synthetic paradigm for in-situ growth of surface-engineered PBAs on conductive substrates and offers fundamental insights for designing high-performance OER catalysts.

Key words: Transition metal phosphide, V-doping, Surface reconstruction, Oxygen evolution reaction, Overall water splitting, Lattice oxygen mechanism

刘玉婵, 高文婧, 黄沁彤, 刘晓雄, 欧阳慧欢, 叶融凯, 李旻鸶, 胡建强. 异质原子掺杂与表面工程协同调控普鲁士蓝衍生物的电子结构为高效水裂解[J]. 催化学报, 2027, 92: 170-181.

Yuchan Liu, Wenjing Gao, Qintong Huang, Xiaoxiong Liu, Huihuan Ouyang, Rongkai Ye, Minsi Li, Jianqiang Hu. Heteroatom doping and surface engineering co-modulated electronic structure of prussian blue analogs for efficient overall water splitting[J]. Chinese Journal of Catalysis, 2027, 92: 170-181.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65222-9

https://www.cjcatal.com/CN/Y2027/V92/I1/170

图/表 6

Fig. 1. Schematic illustration of the V-NiFeP PBAs/NF nanocubes fabricated by the present study.

Fig. 2. SEM images of NiV LDHs (a), V-NiFe PBAs/NF (b), NiFe PBAs/NF (c) and V-NiFeP PBAs/NF NCs (d). (e,f) HRTEM images of the V-NiFeP PBAs/NF NCs. (g-l) STEM and EDS elemental mappings of the V-NiFeP PBAs/NF NCs.

Fig. 3. High-resolution XPS spectra of Ni 2p (a), Fe 2p (b) and V 2p (c) of NiFe PBAs/NF, V-NiFe PBAs/NF and V-NiFeP PBAs/NF NCs. XANES spectra at Ni K-edge (d) and Fe K-edge (e) of NiFe PBAs/NF, V-NiFe PBAs/NF and V-NiFeP PBAs/NF NCs, in which the inset plots are enlarged plots of selected area. (f,g) Fourier-transformed EXAFS spectra of NiFe PBAs/NF, V-NiFe PBAs/NF, V-NiFeP PBAs/NF NCs and references (Ni and Fe foils). (h,i) Wavelet transforms of k3-weighted Ni K-edge and Fe K-edge EXAFS signals of V-NiFeP PBAs/NF NCs.

Fig. 4. OER performance of the NiFe PBAs/NF, V-NiFe PBAs/NF, V-NiFeP PBAs/NF, RuO2/NF and blank NF. LSV curves (a), overpotential at the current density of 50 and 100 mA·cm-2 (b), Tafel plots (c), EIS plots (d), and Cdl versus scan rates (e). (f) Chronopotentiometry curve of the V-NiFeP PBAs/NF NCs at 50 mA·cm-2 for 500 h (inset: LSV of V-NiFeP PBAs/NF NCs before and after OER stability test).

Fig. 5. HER performance of NiFe PBAs/NF, V-NiFe PBAs/NF, V-NiFeP PBAs/NF NCs, Pt/NF and blank NF. LSV curves (a), overpotential at the current density of 20 mA·cm-2 (b), Tafel plots (c), and EIS plots (d) of water-splitting performance of the electrolyzer assembled with V-NiFeP PBAs/NF ||V-NiFeP PBAs/NF. LSV curves (e) and stability test (f) at the current density of 50 mA·cm-2 of the V-NiFeP PBAs/NF ||V-NiFeP PBAs/NF electrolyzer in 1 M KOH, inset shows the photograph of the assembled electrolyzer.

Fig. 6. (a) LSV curves of V-NiFeP PBAs/NF NCs in KOH electrolyte with different pH values. (b) LSV curves of V-NiFeP PBAs NCs in different electrolytes. Gibbs free energy diagrams of NiFeOOH/NF and V-NiFeOOH/NF at U = 1.23 V for LOM (c) and AEM (d) pathways. (e) PDOS of NiFeOOH/NF and V-NiFeOOH/NF. (f) Charge density difference of the V-NiFeOOH/NF, in which the yellow and blue regions represent electron accumulation and depletion, respectively. Schematic plot of OER pathway for LOM (g) and AEM (h) based on Fe sites in the optimized model of the V-NiFeOOH/NF with different reaction intermediates.

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异质原子掺杂与表面工程协同调控普鲁士蓝衍生物的电子结构为高效水裂解

Heteroatom doping and surface engineering co-modulated electronic structure of prussian blue analogs for efficient overall water splitting

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[2]	Jegon Lee, Do-Hyun Kim, Seulgi Ji, Sangmoon Yoon, Seung Hyun Nam, Jucheol Park, Jin Young Oh, Seung Gyo Jeong, Jong-Seong Bae, Sang A. Lee, Heechae Choi, Woo Seok Choi. 激活BaRuO₃薄膜催化活性表面以促进碱性析氢反应[J]. 催化学报, 2026, 83(4): 341-350.
[3]	Hyunseok Yoon, Hee Jo Song, Yumin Park, Andi Haryanto, Dohun Kim, Kyuri Cho, Chanyeon Kim, Wooyul Kim, Chan Woo Lee, Dong-Wan Kim. 通过铜诱导的表面重构动态调节钌催化剂中酸性析氧反应途径[J]. 催化学报, 2026, 83(4): 363-375.
[4]	孙欣然, 霍孟田, 孙健航, 梁宇, 秦愷池, 张浩杨, 邢子豪, 常进法. 金属硫化物前驱体的牺牲转化生成活性羟基氧化物催化剂以增强析氧反应[J]. 催化学报, 2026, 82(3): 84-91.
[5]	唐宇, 陈阳, 陈柯润, Edmund Qi, 刘晓旸, 陆海彦, 高宇. 铜钼协同掺杂金属有机框架双壳空心纳米球: 表面重构激活吸附物演化和晶格氧机制[J]. 催化学报, 2026, 81(2): 159-171.
[6]	钟海红, 徐芊牵, 杨玮婷, ALONSO-VANTE Nicolas, 冯拥军. 铁族过渡金属硫属化合物组成调控以增强氧电极电催化性能[J]. 催化学报, 2026, 81(2): 37-68.
[7]	肖娟, 黄婷婷, 刘夏, 冯玉莹, 许贯诚, 张丽. 磷空位工程化的Ru,P_v-CoP作为氢溢流催化剂以增强工业碱性水电解[J]. 催化学报, 2026, 91(12): 192-209.
[8]	陈阳, 唐宇, 韩雷云, 刘佳颜, 华英杰, 赵旭东, 刘晓旸. 双壳层空心纳米球NiCo₂S₄@CoS₂/MoS₂: 通过协同效应增强析氧催化活性用于水分解[J]. 催化学报, 2025, 74(7): 394-410.
[9]	唐江渔, 王啸, 王云发, 石敏, 霍彭, 吴建祥, 李巧霞, 徐群杰. 活性非键合氧介导NiFe₂O₄晶格氧氧化以实现高效稳定水氧化[J]. 催化学报, 2025, 72(5): 164-175.
[10]	张朋祥, 王佳雯, 杨天宇, 王瑞哲, 沈若凡, 彭智昆, 刘艳艳, 武现丽, 蒋剑春, 李保军. 揭示复杂性: 析氧反应机理研究进展[J]. 催化学报, 2025, 72(5): 48-83.
[11]	郭昊天, 赵路路, 刘欣宇, 李晶, 王鹏飞, 柳宗琳, 王琳琳, 舒杰, 伊廷锋. 静电纺丝技术与MOFs结合: 推动高性能锌空气电池发展[J]. 催化学报, 2025, 79(12): 32-67.
[12]	赵婷, 巩兵兵, 许贯诚, 姜佳慧, 张丽. 异质结构Ni₂P/CoP/FeP₄纳米线网络催化剂的原位表面重构实现大电流密度下全水分解[J]. 催化学报, 2024, 61(6): 269-280.
[13]	欧阳, 李松达, 王飞, 段心怡, 袁文涛, 杨杭生, 张泽, 王勇. 二氧化钛负载的铂纳米颗粒在CO和O₂环境下表面平台位点和台阶位点的可逆转变[J]. 催化学报, 2022, 43(8): 2026-2033.
[14]	齐静, 陈明星, 张伟, 曹睿. 不对称配位磷酸钴铵增强电催化水氧化反应性能[J]. 催化学报, 2022, 43(7): 1955-1962.
[15]	沈巍, 靳晶, 胡阳, 侯亦超, 殷杰, 马振辉, 赵永青, 席聘贤. 表面氯掺杂钙钛矿型钴酸镧催化水氧化[J]. 催化学报, 2022, 43(6): 1485-1492.