通过界面电荷操控强化氢键连通性以加速析氧反应

doi:10.1016/S1872-2067(26)65070-X

催化学报 ›› 2026, Vol. 86: 290-301.DOI: 10.1016/S1872-2067(26)65070-X

通过界面电荷操控强化氢键连通性以加速析氧反应

柯俊^a, 张嘉熙^b^,^*(), 张龙海^a, 钟承志^a, 宋慧宇^a, 杜丽^a, 张玉微^b, 崔志明^a^,^*()

^a 华南理工大学化学与化工学院, 广东广州 510641
^b 华南师范大学化学学院, 广东广州 510006

收稿日期:2026-01-12 接受日期:2026-03-10 出版日期:2026-07-05 发布日期:2026-06-12
通讯作者: ^*电子信箱: jxzhang@scnu.edu.cn (张嘉熙),
zmcui@scut.edu.cn (崔志明).
基金资助:
国家自然科学基金(22572062);国家自然科学基金(22302071);国家自然科学基金(22372062);广东省科学技术厅(2024A1515240043);广州市青年科技人才托举工程项目(QT-2025-009)

Interfacial charge manipulation enhancing H-bond connectivity for promoted oxygen evolution

Jun Ke^a, Jiaxi Zhang^b^,^*(), Longhai Zhang^a, Chengzhi Zhong^a, Huiyu Song^a, Li Du^a, Yuwei Zhang^b, Zhiming Cui^a^,^*()

^a Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology Guangzhou 510641, Guangdong, China
^b School of Chemistry, South China Normal University, Guangzhou 510006, Guangdong, China

Received:2026-01-12 Accepted:2026-03-10 Online:2026-07-05 Published:2026-06-12
Supported by:
National Natural Science Foundation of China(22572062);National Natural Science Foundation of China(22302071);National Natural Science Foundation of China(22372062);Guangdong Provincial Department of Science and Technology(2024A1515240043);Young Talent Support Project of Guangzhou Association for Science and Technology(QT-2025-009)

摘要/Abstract

摘要：

在电催化析氧反应中, 界面反应动力学是决定催化活性的关键因素. 传统研究多聚焦于催化剂本体的组成调控、电子结构优化及活性位构筑, 而对电极/电解液界面中双电层微观溶剂结构的作用关注不足. 近年来, 双电层内界面水分子的氢键连通性被认为会显著影响质子耦合电子转移、界面去质子化以及反应中间体转化的动力学, 但其与析氧动力学之间的定量关联仍缺乏系统研究, 也缺少可普适实施的调控策略. 因此, 发展一种能够在分子尺度上精准操控界面氢键网络的新方法, 对于揭示碱性析氧反应本质并指导高效催化剂设计具有重要科学意义.

针对上述问题, 本文提出了一种界面电荷操控策略, 即通过在催化剂表面引入不同电荷密度的阴离子化学吸附层, 改变界面局域电场与水分子排列方式, 从而调节双电层中的氢键连通性并促进析氧反应动力学. 以Ni₃FeN为模型催化剂, 系统考察了NO₃^-, SO₄^2-和PO₄^3-三种代表性阴离子对界面结构与催化行为的影响, 并将该策略进一步拓展至RuO₂, Ni(OH)₂, Co(OH)₂, FeNi LDH和FeCo LDH等典型析氧催化剂体系, 以验证其普适性. 电化学测试结果表明, 经过NO₃^-, SO₄^2-和PO₄^3-修饰后, Ni₃FeN在1.5-1.6 V vs. RHE电位区间的析氧活性相较原始样品分别提升约1.1倍、1.4倍和2.3倍, 表现出催化性能随阴离子所带电荷增加而逐步增强的明确趋势. 结合原位拉曼表征结果可以看出, 不同阴离子吸附不是改变活性位点数量, 而是显著影响了界面水分子的配位状态与氢键网络重构行为. 进一步通过AIMD模拟发现, 高价阴离子能够提升界面四氢键配位水分子的比例, 增强氢键网络的连续性和稳定性, 进而为去质子化步骤提供更高效的质子传输通道, 降低反应决速步的能垒. 研究表明, 界面局域电荷密度、氢键连通性以及析氧动力学之间存在清晰的正相关关系, 揭示了阴离子修饰促进OER并非仅源于传统电子结构调控或表面吸附能优化, 更关键在于其对电双层溶剂化环境和质子传递过程的深层调控.

综上, 界面氢键网络的精准调控有望成为突破高效电催化瓶颈的关键方向. 本文提出的界面电荷操控策略不仅为析氧催化剂设计提供了新范式, 也为其他涉及质子转移和溶剂重组的电催化反应提供了通用界面工程思路.

关键词: 析氧反应, 电双层, 界面电荷调控, 氢键连通性, 镍铁氮化物, 阴离子

Abstract:

Interfacial hydrogen bond connectivity (HBC) of electrical double layer (EDL) has been identified as a critical factor for many electrocatalytic reactions, However, there is a lack of systematic investigation on the correlation between HBC and oxygen evolution reaction (OER) kinetics, and the advanced strategies to rationally manipulate HBC. Herein, we proposed an interfacial charge manipulation (ICM) methodology to engineer HBC and enhance OER kinetic of various electrocatalysts including Ni3FeN and the benchmark oxides (RuO₂, Ni(OH)₂, Co(OH)₂, FeNi LDH, and FeCo LDH). With Ni₃FeN as a model catalyst, we systematically studied the influence of different anion chemisorption (NO₃^-, SO₄^2-, and PO₄^3-) on HBC and establishing a positive correlation between OER activity and the charge of anions. Electrochemical tests show that the modified Ni₃FeN catalysts with NO₃^-, SO₄^2-, and PO₄^3- exhibit 1.1-, 1.4-, and 2.3-fold activity enhancements at 1.5-1.6 V vs. RHE relative to the raw Ni₃FeN, respectively. The in-situ spectroscopy and AIMD reveal that high anion charges increase four-hydrogen-bonded water populations, strengthening HBC to promote proton transfer across the EDL during deprotonations step and lower energy obstacle of the rate-determining step. This work has offered a new paradigm to regulate the interfacial HBC at molecular scale for promoting OER.

Key words: Oxygen evolution reaction, Electrical double layer, Interfacial charge manipulation, Hydrogen bond connectivity, Ni₃FeN, Anions

柯俊, 张嘉熙, 张龙海, 钟承志, 宋慧宇, 杜丽, 张玉微, 崔志明. 通过界面电荷操控强化氢键连通性以加速析氧反应[J]. 催化学报, 2026, 86: 290-301.

Jun Ke, Jiaxi Zhang, Longhai Zhang, Chengzhi Zhong, Huiyu Song, Li Du, Yuwei Zhang, Zhiming Cui. Interfacial charge manipulation enhancing H-bond connectivity for promoted oxygen evolution[J]. Chinese Journal of Catalysis, 2026, 86: 290-301.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65070-X

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图/表 5

Fig. 1. Structure characterization. (A) A schematic illustration of surface reconstruction happened over Ni3FeN. (B) SEM image of Ni3FeN. (C) N 1s XPS spectra of Ni3FeN before and after NO3- modification. (D) S 2p XPS spectra of Ni3FeN before and after SO42- modification. (E) P 2p XPS spectra of Ni3FeN before and after PO43- modification. In-situ Raman spectra of Ni3FeN modified with PO43- (F) and without modification (G) (corresponding raw Raman spectra are provided in Fig. S12). (H) Concentration of PO43- in electrolytes before and after the modification.

Fig. 2. OER evaluation. (A) Difference in OER activity (Δjgeo = jgeo(anion) - jgeo(OH-)) of Ni3FeN in the presence and absence of 5 mmol L-1 anions salts at varying potential. EIS results (B) and Tafel slope (C) for Ni3FeN in 1 mol L-1 KOH with three different anion salts (5 mmol L-1 KNO3, 5 mmol L-1 Na2SO4, and 5 mmol L-1 K3PO4). (D) Difference in specific OER activity (Δjs = js(anion) - js(OH-)) of Ni3FeN with and without 5 mmol L-1 of anions salt at different applied potential. (E) Difference in specific OER activity (Δjs = js(anion) - js(OH-)) of Ni3FeN at 1.6 V vs. RHE in 1 mol L-1 KOH with different concentrations of anion salts. (F) Rate of specific activity for Ni3FeN in 1 mol L-1 KOH with and without 5 mmol L-1 anion salt as a function of potential. (G) Stability test of Ni3FeN in 1 mol L-1 KOH with 5 mmol L-1 K3PO4.

Fig. 3. Anion-mediated proton transfer mechanism. (A) A schematic illustration of the proposed mechanism for anion effects on catalyst’s activity and proton transfer process. (B) Gibbs free energy change diagrams for Ni3FeN with different absorbed anions. (C) Kinetic isotope effect of Ni3FeN with different absorbed anions. (D) Equivalent circuit model used for EIS fitting of Ni3FeN. (E) Correlation between the equivalent charge capacity of adsorbed anions (CA) and concentration of anions in the electrolyte. (F) Relationship between the valence charge of anions and specific activity and anion charge capacity. (G) Relationship between specific activity and capacity of anion.

Fig. 4. The role of ICM in HBC. (A) In-situ Raman spectra of PO43- modified Ni3FeN with different interfacial waters (4HB-H2O, 2HB-H2O, and free-H2O) distribution at different potentials vs. Ag/AgCl. (The Ag/AgCl reference was recalibrated against RHE before/after Raman measurements, and its drift in 1.0 mol L-1 KOH was verified to be < 3 mV over 12 h (Fig. S86)) (B,C) Potential-dependent populations of interfacial-water components extracted from Raman peak deconvolution. Data are reported as mean ± s.d. from three independent measurements (n = 3). Deconvolution quality metrics (residuals and RMSE/NRMSE) are provided in Figs. S87-S90.” (Notes: The number indicates difference between maximum and minimum population values). (D) Relationship between the valence charge of anions and the specific activity (at 1.6 V vs. RHE), as well as the population of 4HB-H2O (at 1.55 V vs. RHE) in the corresponding anion-containing electrolytes. (E) Relationship between specific activity and population of 4HB-H2O in corresponding anion electrolytes. (F) Interfacial pH swing calculated from OCP decay transient at different current densities. (G) Total number of H bond obtained from AIMD calculation. Representative snapshots of the EDL structure on NiFeOOH without (H) and with (I) PO43-, along with the corresponding hydrogen distribution profiles and the number of H bonds along the surface normal direction.

Fig. 5. Universality of anion effect. Difference in OER activity (Δjgeo = jgeo(anion) - jgeo(OH-)) of RuO2 (A), Ni(OH)2 (B), Co(OH)2 (C), FeNi LDH (D), and FeCo LDH (E) at 1.65 V vs. RHE in 1 mol L-1 KOH with different concentrations of anion salts. Difference in specific OER activity (Δjs = js(anion) - js(OH-)) of RuO2 (F), Ni(OH)2 (G), OH)2 (H), FeNi LDH (I), and FeCo LDH (J) with and without 5 mmol L-1 of anions salt at different applied potential. Relationship of RuO2 (K), Ni(OH)2 (L), Co(OH)2 (M), FeNi LDH (N), and FeCo LDH (O) between the specific activity (Δjs = js(anion) - js(OH-)) and anion charge capacity (ΔCa = Ca (anion) - Ca (OH-)).

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通过界面电荷操控强化氢键连通性以加速析氧反应

Interfacial charge manipulation enhancing H-bond connectivity for promoted oxygen evolution

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