磷酸根促进涉水电氧化反应的去质子化和质子转移过程

doi:10.1016/S1872-2067(26)65234-5

催化学报 ›› 2026, Vol. 91: 341-350.DOI: 10.1016/S1872-2067(26)65234-5

磷酸根促进涉水电氧化反应的去质子化和质子转移过程

姚君尉^,¹, 程传祺^,¹, 李瑞, 高莹^*(), 张兵

天津大学理学院化学系，天津 300072

收稿日期:2026-03-16 接受日期:2026-05-15 出版日期:2026-12-18 发布日期:2026-10-13
通讯作者: ^*电子信箱: gaoying01@tju.edu.cn (高莹).
作者简介:¹共同第一作者.
基金资助:
国家重点研发计划(2024YFA1510100);国家重点研发计划(2023YFA1507400);国家自然科学基金(22504098);中国博士后科学基金(BX20250099);天津大学2024年研究生文理拔尖创新奖励计划项目(B2-2024-004)

Phosphate anions accelerated deprotonation and proton transfer for water-involved electrooxidation

Junwei Yao^,¹, Chuanqi Cheng^,¹, Rui Li, Ying Gao^*(), Bin Zhang

Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China

Received:2026-03-16 Accepted:2026-05-15 Online:2026-12-18 Published:2026-10-13
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2024YFA1510100);National Key Research and Development Program of China(2023YFA1507400);Na-tional Natural Science Foundation of China(22504098);China Postdoctoral Science Foundation(BX20250099);Tianjin University 2024 Postgraduate Education Special Fund(B2-2024-004)

摘要/Abstract

摘要：

涉水电氧化反应在能源转换与合成化学领域展现出巨大潜力. 作为电氧化体系的核心组成部分, 阳极电催化剂在决定整体性能方面发挥着关键作用. 目前, 非贵金属氢氧化物, 尤其是镍、钴、铁基的层状双氢氧化物, 已成为该类反应中极具前景的催化材料. 在一定的氧化电位下, 生成的相应的羟基氧化物是关键活性物种, 其催化活性与氧化电位下的去质子化行为密切相关. 然而, 去质子化过程中, 界面处质子的局部积累会导致局部酸化, 进而引发催化剂腐蚀, 影响其稳定性与活性. 因此, 促进电催化剂和反应物的去质子化过程以及后续的质子转移, 对于提升涉水氧化反应的电催化性能具有重要意义.
本文设计了磷酸根离子插层的NiFe LDH催化剂, 通过协同促进催化剂与反应物的去质子化过程以及界面质子转移, 桥连界面氢键网络恢复其连续性, 从而提升涉水电氧化反应性能. 原位拉曼光谱和电化学阻抗谱结果表明, 具有强夺质子能力的磷酸根加速了氢氧化物向NiOOH以及反应物向活性中间体的去质子化过程, 提高活性中心Ni⁴⁺位点的数量, 并增强本征电氧化活性. 密度泛函理论计算进一步揭示, 磷酸根插层后的NiFe LDH具有更低的去质子化能和更直接的质子迁移路径, 热力学上更有利于电氧化过程. 此外, 从头算分子动力学模拟和原位衰减全反射-傅里叶变换红外光谱表明, 磷酸根可桥接界面氢键网络, 改善网络连续性, 进而促进质子转移和反应动力学. 该策略不仅适用于析氧反应, 还可拓展到多种醇的电氧化反应, 其法拉第效率和反应速率均显著提高. 此外, 本工作构建了一种级联电合成系统, 可将环己醇转化为环己酮并在阴极进一步合成环己酮肟, 在100 mA cm⁻²下实现了1.04 mmol h⁻¹的环己酮肟产率.
综上, 本工作阐明了磷酸根插层增强去质子化热力学和质子转移动力学的机制, 实现了一系列涉水电氧化反应性能的提升, 提出一种改善电氧化催化性能的普适策略, 为设计和合成高效催化剂提供了新思路.

关键词: 电催化, 电氧化, 质子转移, 氢键, 镍铁层状双氢氧化物

Abstract:

Phosphate anions (Pi)-modified layered double hydroxides (LDH) have long been regarded as promising anodic electrocatalysts, but the effect by which Pi enhances electrooxidative activity remains unclear. Here, we prepare a Pi-intercalated NiFe LDH (Pi-NiFe LDH) to investigate the role of Pi intercalation in electrooxidation processes. Pi anchored at Fe sites facilitates the deprotonation of adjacent hydroxyl groups at Ni sites to form the active NiOOH phase while promoting the deprotonation of reactants to initiate electrooxidation processes. These dual effects collectively lower the thermodynamic energy. Moreover, Pi bridges the interfacial hydrogen-bond (H-bond) network to restore its continuity, ensuring efficient proton transfer and accelerating reaction kinetics. Therefore, Pi-NiFe LDH delivers enhanced activity for both the oxygen evolution reaction and the electrooxidation of various alcohols with reduced overpotentials and elevated yield rates. This study offers mechanistic insights into how anions modulate deprotonation and proton transfer processes, guiding the design of electrooxidation catalysts.

Key words: Electrocatalysis, Electrooxidation, Proton transfer, Hydrogen-bond, NiFe LDH

姚君尉, 程传祺, 李瑞, 高莹, 张兵. 磷酸根促进涉水电氧化反应的去质子化和质子转移过程[J]. 催化学报, 2026, 91: 341-350.

Junwei Yao, Chuanqi Cheng, Rui Li, Ying Gao, Bin Zhang. Phosphate anions accelerated deprotonation and proton transfer for water-involved electrooxidation[J]. Chinese Journal of Catalysis, 2026, 91: 341-350.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65234-5

https://www.cjcatal.com/CN/Y2026/V91/I12/341

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Fig. 1. Proposed Pi-intercalation strategy for facilitating deprotonation and proton transfer. (a) Process analysis of electrooxidation reactions. (b) The proposed Pi-intercalation strategy.

Fig. 2. Characterization of the Pi-NiFe LDH. Raman spectra (a), Ni 2p XPS spectra (b), Fe 2p XPS spectra (c), Ni K-edge XANES spectra (d), Fe K-edge XANES spectra (e), and O K-edge XANES spectra (f) of NiFe LDH and Pi-NiFe LDH.

Fig. 3. Origin of facilitated deprotonation. (a) CV curves measured in 1 mol L-1 KOH with or without 0.1 mol L-1 CHA at a scan rate of 10 mV s-1. (b) Potential-dependent yield rates and FEs for the CHN of NiFe LDH and Pi-NiFe LDH. Potential-dependent in situ Raman spectra measured in 1 mol L-1 KOH with 0.1 mol L-1 CHA over NiFe LDH (c) and Pi-NiFe LDH (d). Proton transfer barriers of hydroxides to anions (e) and anions to anions (f). Potential-dependent Bode plots measured in 1 mol L-1 KOH with 0.1 mol L-1 CHA over NiFe LDH (g) and Pi-NiFe LDH (h). (i) Free energy diagram for CHA oxidation.

Fig. 4. Origin of facilitated proton transfer. Potential-dependent ATR-FTIR spectra of Pi-NiFe LDH (a) and NiFe LDH (b). (c) Corresponding wavenumbers of the O-H stretching vibration under different potentials. (d) Representative snapshot of the interfacial H-bond networks adjacent to NiFe LDH and Pi-NiFe LDH. (e) Statistical distribution of the intensity of H-bonds. (f) Proton transfer barriers at the interfaces of NiFe LDH and Pi-NiFe LDH. Inset: calculated energy barriers for proton transfer. (g) CHA deprotonation energy barriers at the interfaces of NiFe LDH and Pi-NiFe LDH. Inset: calculated energy barriers for CHA deprotonation. (h) Ea for the CHA electrooxidation of NiFe LDH and Pi-NiFe LDH.

Fig. 5. Universality and utility of Pi-NiFe LDH. FEs of electrooxidation of isopropanol (a), ethylene glycol (b), and glycerol electrooxidation (c) at a current density of 100 mA cm-2 over NiFe LDH and Pi-NiFe LDH. (d) Schematic diagram of the cascade system for cyclohexanone oxime electrosynthesis. (e) FE and full-cell voltage of anodic CHN electrosynthesis and cathodic cyclohexanone oxime electrosynthesis. (f) 1H NMR spectra of the obtained cyclohexanone oxime.

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磷酸根促进涉水电氧化反应的去质子化和质子转移过程

Phosphate anions accelerated deprotonation and proton transfer for water-involved electrooxidation

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