镍位点局域原子环境调控用于工业级海水制氢

doi:10.1016/S1872-2067(26)65051-6

催化学报 ›› 2026, Vol. 87: 254-268.DOI: 10.1016/S1872-2067(26)65051-6

镍位点局域原子环境调控用于工业级海水制氢

武鹏飞^a, 娄志昊^a, 马元硕^a, 王鹏飞^a, 薛达^a, 马方怡^a, 崔学晶^a, 刘光波^a^,^*(), 周新^b^,^c^,^*(), 王二东^d, 姜鲁华^a^,^*()

^a 青岛科技大学材料科学与工程学院, 山东青岛 266042
^b 辽宁师范大学化学与生物学交叉研究中心, 辽宁大连 116029
^c 大连大学环境与化学工程学院, 辽宁大连 116622
^d 中国科学院大连化学物理研究所, 大连清洁能源国家实验室, 辽宁大连 116023

收稿日期:2025-12-02 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: liugb@qust.edu.cn (刘光波),
xzhou@lnnu.edu.cn (周新),
luhuajiang@qust.edu.cn (姜鲁华).
基金资助:
国家自然科学基金(22279069);国家自然科学基金(22478211);国家自然科学基金(22372017)

Local-atomic environment engineering of Ni-sites for industrial hydrogen production from seawater

Pengfei Wu^a, Zhihao Lou^a, Yuanshuo Ma^a, Pengfei Wang^a, Da Xue^a, Fangyi Ma^a, Xuejing Cui^a, Guangbo Liu^a^,^*(), Xin Zhou^b^,^c^,^*(), Erdong Wang^d, Luhua Jiang^a^,^*()

^a College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^b Interdisciplinary Research Center for Biology and Chemistry, Liaoning Normal University, Dalian 116029, Liaoning, China
^c College of Environment and Chemical Engineering, Dalian University, Dalian 116622, Liaoning, China
^d Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2025-12-02 Accepted:2026-01-12 Online:2026-08-18 Published:2026-06-24
Supported by:
National Natural Science Foundation of China(22279069);National Natural Science Foundation of China(22478211);National Natural Science Foundation of China(22372017)

摘要/Abstract

摘要：

氢能是未来清洁能源体系中的关键载体, 对实现碳中和目标具有重要意义. 海水电解与可再生能源相结合, 是绿色可持续的制氢途径, 但其实际应用严重受限于低成本、高活性和可扩展电极的缺乏. 镍基催化剂是碱性/中性析氢反应(HER)的潜力材料, 但其活性受到强氢吸附与缓慢水解离动力学的限制. 研究表明, 构建异质结构界面可通过调控Ni的原子与电子结构来提升其HER活性. 然而, Ni位点的局部原子环境与其催化性能之间的构效关系尚不明确. 因此, 有必要通过精确设计具有不同Ni位点微环境的催化剂, 从原子层面阐明其内在的结构-活性关联, 以推动实际应用.

本文设计合成了多种Ni/VO_x催化剂, 利用不同价态的V实现了对Ni局部环境的调控, 从而有助于阐明Ni位点局域环境与HER活性之间的相关性. 结果表明, Ni价态与氢吸附自由能(∆G_H*)和零电荷电势(PZC)之间存在火山型关系, 其中∆G_H*和PZC均与HER活性呈线性相关. 原位傅里变换红外光谱(FTIR)证实, 较低的PZC有利于电极表面附近更多自由水分子的形成, 从而促进了HER过程. 理论研究结果表明, V₂O₃修饰可弱化过强的H*吸能, 同时增强中间体OH*的稳定性, 从而加速水解离, 提高Ni的HER活性. 此外, V₂O₃的引入在Ni位点附件形成高OH^‒覆盖度, 进而有效抑制Cl^‒腐蚀, 增强长期耐久性. 实验结果显示, Ni/V₂O₃电极具有最优的Ni位点局部原子环境(Ni-O配位数0.6, Ni价态+0.21)使其在碱性海水中表现出优异的HER活性, 在283/361 mV的过电位下, 达到500/1000 mAcm^‒2的电流密度. 同时, 该Ni/V₂O₃电极面积可扩大至50 cm², 以此组装的千瓦级碱性海水电解槽能够在25 A的超高电流下连续运行长达880 h, 衰减率低至34.1 μV h^-1, 展现出极佳的工业应用潜力. 此外, 经济性分析表明, 该电解槽的能耗仅有48.67 kWh kg^-1 H₂, 对应每公斤氢气的生产成本仅为2.48美元, 低于欧盟委员会制定的2030年产氢成本目标(2.50美元).

综上, 本文提出了一种合理设计非贵金属Ni基催化剂的方法, 明确了其HER反应机理, 并开展了面向工业制氢的探索性实验. 结果表明, 该方法具备良好的工业应用潜力, 实现了从基础研究向实际应用的有效推进. 这不仅为满足日益增长的氢气需求提供了新的可能, 也为后续高效催化剂的设计与应用提供了有益借鉴.

关键词: 局部原子环境, 镍位点, 析氢反应, 界面水, 零电荷电位

Abstract:

Seawater electrolysis integrated with renewable energy sources represents a green and sustainable pathway for hydrogen production, yet its practical application is severely constrained by the lack of cost-effective, highly active, and scalable electrodes. Herein, we report the construction of a high-performance hydrogen evolution reaction (HER) electrode by engineering the local-atomic environment of Ni sites through vanadium oxide modification. This optimized electrode delivers current densities of 500/1000 mA cm^-2 at only 283/361 mV in alkaline seawater. Impressively, a kW-scale alkaline seawater electrolyzer achieves continuous operation at an industrial-level current up to 25 A for over 880 h with an ultra-low degradation rate of 34.1 μV h^-1. Combined experimental and theoretical investigations reveal a volcano-type relationship between the chemical state of Ni and the adsorption energy of the key intermediate H* (∆G_H_*), as well as the potential of zero charge (PZC) of the electrode. Furthermore, in-situ Fourier-transform infrared spectroscopy confirms that a lower PZC promotes the formation of more free water molecules near the electrode surface, thereby facilitating the HER process. This work uncovers atomic environment-governed HER mechanisms and develops a scalable, industrially stable seawater electrolysis electrode, bridging lab-innovation to practical hydrogen production.

Key words: Local-atomic environment, Ni-sites, Hydrogen evolution, Interfacial water, Potential of zero charge

武鹏飞, 娄志昊, 马元硕, 王鹏飞, 薛达, 马方怡, 崔学晶, 刘光波, 周新, 王二东, 姜鲁华. 镍位点局域原子环境调控用于工业级海水制氢[J]. 催化学报, 2026, 87: 254-268.

Pengfei Wu, Zhihao Lou, Yuanshuo Ma, Pengfei Wang, Da Xue, Fangyi Ma, Xuejing Cui, Guangbo Liu, Xin Zhou, Erdong Wang, Luhua Jiang. Local-atomic environment engineering of Ni-sites for industrial hydrogen production from seawater[J]. Chinese Journal of Catalysis, 2026, 87: 254-268.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65051-6

https://www.cjcatal.com/CN/Y2026/V87/I8/254

图/表 7

Fig. 1. Synthesis and structure characterizations. (a) Schematic process for synthesizing Ni/VOx. SEM (b), TEM (c) and HRTEM (d) images of Ni/V2O3 catalyst. (e) HAADF image and EDS elemental mappings of Ni/V2O3 catalyst.

Fig. 2. Chemical state and electronic structure characterizations. High resolution XPS spectra of Ni 2p (a), V 2p (b), and O 1s (c) for NF@Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5. XANES spectra of the Ni K-edge (d) and average valence state (e) of Ni in Ni/V2O3, Ni/VO2 and Ni/V2O5. EXAFS spectra of the Ni K-edge (f) and wavelet-transform plots (g) for the Ni, NiO, Ni/V2O3, Ni/VO2 and Ni/V2O5.

Fig. 3. Electrocatalytic HER performances. Polarization curves (a), overpotentials at 500 and 1000 mA cm-2 (b), and Tafel curves (c) of NF@Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5 in 1 mol L?1 KOH. Polarization curves (d), overpotentials at 500 and 1000 mA cm-2 (e), and Tafel curves (f) of NF@Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5 in 1 mol L?1 KOH + seawater. Comparison of overpotentials at 100 mA cm-2 (η100) and Tafel slopes between Ni/V2O3 and reported catalysts in 1 mol L?1 KOH (g) and 1 mol L?1 KOH + seawater (h). (i) Chronopotentiometry curves of NF@Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5 electrodes in 1 mol L?1 KOH and 1 mol L?1 KOH + seawater.

Fig. 4. In-situ impedance and interfacial water behavior. Bode plots of the in-situ electrochemical impedance spectra of NF@Ni (a), Ni/V2O3 (b), Ni/VO2 (c), and Ni/V2O5 (d) in 1 mol L-1 KOH. In-situ FTIR contour plots and spectra of interfacial water at surface of NF@Ni (e,i), Ni/V2O3 (f,j), Ni/VO2 (g,k), and Ni/V2O5 (h,l) under different potentials in 0.1 mol L-1 KOH. The proportion of 2-HB·H2O (m), 4-HB·H2O (n) and free-H2O (o) on surface of NF@Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5. (p) PZC values of NF@Ni, Ni/V2O3, Ni/VO2, and Ni/V2O5.

Fig. 5. DFT calculations. (a) The structure and differential charge density of Ni/V2O3, Ni/VO2 and Ni/V2O5. (b) Partial density of state analysis and d-band centers for Ni, Ni/V2O3, Ni/VO2, and Ni/V2O5. (c) Calculated adsorption energy of H2O* (EH2O*) and OH* (EOH*) on Ni, Ni/V2O3, Ni/VO2 and Ni/V2O5. (d) Calculated hydrogen adsorption free energy on the Ni, Ni/V2O3, Ni/VO2, and Ni/V2O5. (e) Alkaline HER process on Ni/V2O3. (f) Schematic illustration of the interfacial water structure and HER process on Ni/V2O3 in seawater. (g) Relationships among calculated ΔGH*, PZC values, Ni valence, conversion rate of free-H2O, and overpotentials at 500 mA cm?2 for Ni, Ni/V2O3, Ni/VO2, and Ni/V2O5.

Fig. 6. Large-area Ni/V2O3 electrode production and uniformity characterizations. (a) Optical image of the Ni/V2O3 electrode with a geometric area of approximately 50 cm2. (b?h) SEM images of Ni/V2O3 in the selected regions in (a). LSV curves and corresponding overpotentials for the HER of the selected region of Ni/V2O3 in alkaline freshwater (i,l), alkaline seawater (j,m), and natural seawater (k,n).

Fig. 7. Performances of the kW-scale three-cell ASWE stack with Ni/V2O3 || NiFe-LDH electrodes. (a) Component and structure of one ASWE cell. (b, c) Digital images of the three-cell ASWE stack. Polarization curve (d) and Nyquist plot (e) of the three-cell ASWE stack in 6 mol L-1 KOH + seawater at 60 °C. (f) Durability and energy consumption of the three-cell ASWE stack at 25 A (0.5 A cm-2) in 6 mol L-1 KOH + seawater at 60 °C.

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镍位点局域原子环境调控用于工业级海水制氢

Local-atomic environment engineering of Ni-sites for industrial hydrogen production from seawater

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[1]	任宇曦, 许堡荣, 靳瑜, 肖航, 牛冉冉, 刘威, 欧鸿辉, 杨贵东. NiMoO₄同质结d带工程促进选择性电化学氮还原制氨[J]. 催化学报, 2026, 85(6): 216-225.
[2]	吴立清, 黄文霞, 赵冰冰, 蔡苹, 罗威. 钌氧化物表面阴离子介导的动态界面自由水富集微环境助力高效酸性氧析出反应[J]. 催化学报, 2026, 85(6): 237-246.
[3]	万自杰, 杨矞琦, 王振权, 武林睿, 张海鹏, 时晴芳, 刘翔, 杨翰林, 康博晗, 徐泉, 罗佳庆, 刘坚. 空间限制与含氮缺陷锚定协同增强钌纳米颗粒催化剂在工业电流密度下的析氢性能[J]. 催化学报, 2026, 84(5): 130-143.
[4]	初铭涛, 张慧敏, 任变清, 曹景, 章腾, 宋平, 王子准, 韩策, 徐维林. 非晶-晶体异质结构Ru_MoNiN/Ni-MoO₂用于高效稳定的碱性析氢反应[J]. 催化学报, 2026, 84(5): 96-105.
[5]	刘沛林, 庄夏青, 崔天泽, 魏子森, 徐华, 张若霖, 杨矞琦, 罗佳庆, 宋卫余, 刘云鹏, 孔裕, 李振兴, 赵震, 刘坚, 孙源卿. 钌单原子/纳米簇双引擎活性中心协同提升析氢反应性能[J]. 催化学报, 2026, 84(5): 80-95.
[6]	张洪文, 蔡颖慧, 李秉岳, 山巍, 唐华. Cu单原子与CuO纳米团簇协同增强TiO₂光催化析氢性能[J]. 催化学报, 2026, 83(4): 162-171.
[7]	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.
[8]	岳健超, 张昱, 熊茜茜, 罗威. 桥接氧诱导氢键网络重构提升磷掺杂碳包覆镍催化剂的碱性氢氧化电催化活性[J]. 催化学报, 2026, 82(3): 144-152.
[9]	石苗苗, 何月轩, 张宁, 鲍迪, 赵大明, 钟海霞, 鄢俊敏, 蒋青. 室温下直接电化学液氨分解实现现场产氢[J]. 催化学报, 2026, 81(2): 310-318.
[10]	宋鑫, 李中华, 盛利, 刘扬. 单原子催化剂中自旋密度对称性破缺介导的析氢反应[J]. 催化学报, 2026, 80(1): 213-226.
[11]	靳一鸣, 成文静, 罗威. 单原子钌诱导界面水结构调控实现高效的碱性氢氧化反应[J]. 催化学报, 2025, 74(7): 240-249.
[12]	姚瑶, 徐菊萍, 邵敏华. 多晶金表面上析氢反应与氧还原反应的竞争[J]. 催化学报, 2025, 73(6): 271-278.
[13]	纳国豪, 郑红顺, 陈明鹏, 孙华传, 吴阅文, 李德全, 陈赟, 赵勃然, 赵博, 周桐, 何天威, 张雨潇, 赵建红, 张裕敏, 张瑾, 刘锋, 崔浩, 柳清菊. Pt原位还原诱导NiFe-MOF拓扑转变用于工业级电解海水制氢[J]. 催化学报, 2025, 72(5): 211-221.
[14]	贾萁森, 王雅楠, 赵艳, 田圳铭, 任璐瑶, 崔学晶, 刘光波, 陈鑫, 李文震, 姜鲁华. 通过调节钛氧化物界面水结构驱动光电催化海水选择性氧化产氧[J]. 催化学报, 2025, 72(5): 154-163.
[15]	冯超, 邵佳新, 吴汉洋, 杨恒攀, 蔚佳莹, 胡琪, 何传新. 超高过电位诱导NiS₂深度重构显著提高HER性能[J]. 催化学报, 2025, 72(5): 230-242.