乙酸根介导的仿生质子穿梭机制构筑高效析氧催化剂

doi:10.1016/S1872-2067(26)65072-3

催化学报 ›› 2026, Vol. 87: 282-294.DOI: 10.1016/S1872-2067(26)65072-3

乙酸根介导的仿生质子穿梭机制构筑高效析氧催化剂

张建平^a^,^b, 张坤^a^,^*(), 翁应龙^b, 李楠楠^d, 黄婷婷^b, 路亦通^a, 孙庭宇^e, 韩晓彤^b^,^*(), 邱介山^c^,^*()

^a 东北电力大学化学工程学院, 吉林 132012, 中国
^b 重庆大学化学化工学院, 重庆 401331, 中国
^c 北京化工大学化学工程学院, 化工资源有效利用国家重点实验室, 北京 100029, 中国
^d 成均馆大学化学系, 基础科学研究院, 水原 16419, 韩国
^e 华南理工大学化学与化工学院, 广东广州 510641, 中国

收稿日期:2025-12-01 接受日期:2026-01-12 出版日期:2026-08-18 发布日期:2026-06-24
通讯作者: ^*电子信箱: zhangkun@neepu.edu.cn (张坤),
hanxiaotong@cqu.edu.cn (韩晓彤),
qiujs@mail.buct.edu.cn (邱介山).
基金资助:
吉林省自然科学基金(20260102125JC);国家自然科学基金(22208035);重庆市自然科学基金(CSTB2024NSCQ-MSX0728);重庆市留学人员回国创业创新支持计划(cx2024115)

Bioinspired acetate-mediated proton shuttling toward robust oxygen evolution

Jianping Zhang^a^,^b, Kun Zhang^a^,^*(), Yinglong Weng^b, Nannan Li^d, Tingting Huang^b, Yitong Lu^a, Tingyu Sun^e, Xiaotong Han^b^,^*(), Jieshan Qiu^c^,^*()

^a School of Chemical Engineering, Northeast Electric Power University, Jilin 132012, Jilin, China
^b School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331, China
^c College of Chemical Engineering, State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^d Department of Chemistry, Institute of Basic Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
^e School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China

Received:2025-12-01 Accepted:2026-01-12 Online:2026-08-18 Published:2026-06-24
Supported by:
Natural Science Foundation of Jilin Province(20260102125JC);National Natural Science Foundation of China(22208035);Natural Science Foundation of Chongqing(CSTB2024NSCQ-MSX0728);Support Plan for Overseas Students to Return to China for Entrepreneurship and Innovation(cx2024115)

摘要/Abstract

摘要：

在电解水制氢系统中, 阳极析氧反应(OER)催化剂的长期运行稳定性是制约其槽效率提升与成本降低的核心挑战之一. 催化剂性能衰减的根源在于OER过程中持续的脱质子化步骤, 导致质子(H⁺)在电极-电解液界面动态累积, 形成显著的局部酸性微环境. 这种界面酸化不仅直接侵蚀催化活性位点, 更会加速活性金属组分(如Ni,Fe)的溶出, 造成催化剂结构的不可逆破坏. 现有改善策略, 如在催化剂表面修饰路易斯酸性氧化物, 虽可通过捕获OH^-局部缓解传质限制, 但这类惰性覆盖层通常会遮蔽部分活性位点, 且无法在体相电解质与活性界面之间构建起高效、连续的离子传输通道. 因此, 发展一种能够在不牺牲活性位点的前提下, 定向调节界面离子传输、特别是促进OH^-快速供给以中和累积质子的新方法,成为突破当前稳定性瓶颈的关键所在.

本文以镍铁层状双氢氧化物为模型体系, 提出一种仿生策略, 通过引入具有路易斯碱性的乙酸根阴离子作为动态质子传导媒介, 实现对界面微环境的精准调控. 研究表明, 乙酸根可通过其-COO^-/-COOH基团的可逆质子化/去质子化循环, 构建高效的质子传递路径, 并协同增强界面氢键网络, 从而显著促进氢氧根离子向催化剂表面的传输. 同时, 乙酸根中的孤对电子可选择性配位于层状双氢氧化物骨架中的铁活性中心, 有效调控局部电子结构, 提升材料本征催化活性. 借助原位拉曼与红外光谱, 成功捕捉到反应过程中瞬态CH₃COOH物种的生成; 进一步通过差分电化学质谱检测到CH₃COOD信号, 直接证实乙酸根介导的质子穿梭机制. 理论计算表明, 乙酸根配位不仅有助于稳定催化活性位点, 还可显著降低OER反应的关键能垒. 得益于上述双功能协同效应, 乙酸根插层镍铁层状双氢氧化物表现出优异的OER性能, 在10 mA cm^-2电流密度下过电位仅为213 mV, 并在阴离子交换膜电解槽中实现了50 mA cm^-2条件下超过1200 h的持续稳定运行.

综上, 本文发展的乙酸根介导界面微环境调控策略及其在镍铁层状双氢氧化物体系中的成功应用, 为解决OER中因界面酸化导致的稳定性瓶颈问题提供了明确可行的新途径. 尽管实际电解水系统中仍面临复杂工况下的传质限制、长期运行下的阴离子流失以及膜电极集成工艺等挑战, 但随着对界面离子传输机制认识的深化, 以及原位表征与理论模拟技术的协同发展, 未来有望设计出更多具有动态自适应能力的智能催化界面. 本文不仅为开发高稳定性OER催化剂提供了创新的设计思路与实验依据, 也为理解并调控电催化反应中的界面微环境提供了重要的理论参考.

关键词: 层状双金属氢氧化物, 仿生催化, 质子穿梭, 质子迁移, 析氧反应

Abstract:

Persistent proton accumulation from extensive reactant deprotonation during oxygen evolution reaction (OER) induces severe local acidification at electrode-electrolyte interface, accelerating catalyst degradation and performance decay. Employing NiFe layered double hydroxide (NiFe-LDH) as a model, we present a bioinspired strategy wherein Lewis-basic acetate anion (CH₃COO^-, Ac^-) functions as dynamic proton shuttle to regulate interfacial microenvironment (Ac^--LDH). Ac^- undergoes reversible -COO^-/-COOH cycle upon protonation, promoting efficient proton transfer and reinforcing hydrogen-bond networks that expedite OH^- delivery to LDH surface. Simultaneously, Ac^- lone pairs selectively coordinate with Fe centers in LDH framework, tuning electronic structure and enhancing intrinsic activity. In-situ Raman and infrared spectroscopy capture transient CH₃COOH formation, while differential electrochemical mass spectrometry evidences proton shuttling via CH₃COOD detection. Theoretical calculations reveal that Ac^- coordination stabilizes active site and reduces OER energy barrier. Leveraging this dual functionality, Ac^--LDH exhibits superior activity with 213 mV overpotential at 10 mA cm^-2 and remarkable durability, maintaining 50 mA cm^-2 for over 1200 h in anion-exchange membrane electrolyzer. This work establishes bioinspired molecular shuttles for interfacial microenvironment engineering as versatile paradigm for developing OER catalysts with high activity and durability.

Key words: Layered double hydroxide, Biomimetic, Proton shuttling, Proton migration, Oxygen evolution reaction

张建平, 张坤, 翁应龙, 李楠楠, 黄婷婷, 路亦通, 孙庭宇, 韩晓彤, 邱介山. 乙酸根介导的仿生质子穿梭机制构筑高效析氧催化剂[J]. 催化学报, 2026, 87: 282-294.

Jianping Zhang, Kun Zhang, Yinglong Weng, Nannan Li, Tingting Huang, Yitong Lu, Tingyu Sun, Xiaotong Han, Jieshan Qiu. Bioinspired acetate-mediated proton shuttling toward robust oxygen evolution[J]. Chinese Journal of Catalysis, 2026, 87: 282-294.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65072-3

https://www.cjcatal.com/CN/Y2026/V87/I8/282

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Fig. 1. (a) Schematic of proton accumulation-induced NiFe-LDH dissolution. (b) Schematic of carrier proteins transporting ions and small molecules to maintain intracellular homeostasis (illustration created using Figdraw). (c) Schematic of Ac- and SO42- modulated NiFe-LDH.

Fig. 2. Structural characterization of Ac--LDH. XRD patterns (a) and FT-IR spectra (b) of Ac--LDH and SO42--LDH. (c) Contact-angle measurements for Ac--LDH and SO42--LDH. TEM (d) and HR-TEM (e) images of Ac--LDH (inset: SAED pattern). (f) HR-TEM image and corresponding 3D intensity map of Ac--LDH. (g) Elemental mapping of Ac--LDH.

Fig. 3. Local structure analysis of Ac--LDH and SO42--LDH. XPS spectra of Fe 2p (a) and Ni 2p (b) for Ac--LDH and SO42--LDH. (c) Content of specific species in Ac--LDH and SO42--LDH. (d) EPR spectra of Ac--LDH and SO42--LDH. Normalized XANES spectra at Fe (e) and Ni (f) K-edges. Fourier-transformed EXAFS spectra at Fe (g) and Ni (h) K-edges. Wavelet-transformed spectra at Fe (i) and Ni (j) K-edges for Ac--LDH. Wavelet-transformed spectra at Fe (k) and Ni (l) K-edges for SO42--LDH.

Fig. 4. OER activity evaluation of the catalysts. (a) CV curves of Ac--LDH and SO42--LDH. LSV curves (b) and Tafel plots (c) of Ac--LDH, SO42--LDH, and RuO2. Cdl plots (d) and Nyquist plots (e) of Ac--LDH and SO42--LDH. (f) Comparison of comprehensive electrochemical properties. (g) Durability test curves (insets: SEM images of Ac--LDH and SO42--LDH after stability testing). (h) Comparison of OER performance between Ac--LDH and reported catalysts.

Fig. 5. Enhancement mechanism of OER activity. In-situ Bode plots of Ac--LDH (a) and SO42--LDH (b). (c) Histogram of phase-angle changes with applied potential. (d) Schematic of equivalent circuit and correlations of equivalent resistances. (e) Charge-transfer resistance at different potentials. (f) Open-circuit potential measured in 1.0 mol L-1 KOH before and after injection of 6.0 mol L-1 KOH. (g) Zeta potential in 1.0 mol L-1 KOH. (h) Schematic of GCS model and OH- enrichment at electrode-electrolyte interface for Ac--LDH.

Fig. 6. Reaction mechanism investigation of Ac--LDH catalyst. In-situ Raman spectra of Ac--LDH (a) and SO42--LDH (b). Potential-dependent (c) and time-dependent (d) Raman intensity ratio for Ac--LDH and SO42--LDH. (e) In-situ infrared spectra of Ac--LDH. (f) DEMS signals for 32O2 and 61CH3COOD of Ac--LDH. (g) Proposed OER pathways for Ac--LDH and SO42--LDH.

Fig. 7. Theoretical calculations of the OER activity of Ac--LDH electrocatalyst. (a) Electrostatic potential maps of HAc, H2SO4, Ac-, and SO42-. 2D differential electron density maps of Ac--LDH (front (b), top (d), and side (f) views) and SO42--LDH (front(c), top (e), and side (g) views). 3D differential electron density maps of Ac--LDH (h) and SO42--LDH (i). DOS (j) and PDOS (k) curves of Ac--LDH and SO42--LDH. (l) Schematic of p- and d-band center alignment for Ac--LDH and SO42--LDH. (m) Gibbs free energy profiles of Ac--LDH and SO42--LDH.

Fig. 8. Performance tests of Ac--LDH catalyst in AEMWE. (a) LSV curves for overall water electrolysis. (b) Comparison of voltage at 10 and 50 mA cm-2. (c) The measured O2 amount of of Ac--LDH. (d) Durability test curves. (e) Schematic of AEMWE device. (f) Polarization curves of Ac--LDH in AEMWE. (g) Durability test curves in AEMWE.

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乙酸根介导的仿生质子穿梭机制构筑高效析氧催化剂

Bioinspired acetate-mediated proton shuttling toward robust oxygen evolution

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