空位工程构筑钌基碳纳米管用于安培级电解水

doi:10.1016/S1872-2067(26)65116-9

催化学报 ›› 2026, Vol. 88: 279-294.DOI: 10.1016/S1872-2067(26)65116-9

空位工程构筑钌基碳纳米管用于安培级电解水

Yusuf Bashir Adegbemiga^a^,¹, Jayawardana Hennayaka Mudiyanselage Charitha Madusanka^a^,¹, Yaseen Waleed^a, 谢吉民^a^,^b, 邓伊琳^a^,^*(), 孟素慈^a^,^b, 李永明^c, Mohammed Abdussamad Mukhtar^d, Magaji Aminu^e, 陈敏^a^,^*(), 谢萌^a, 徐远国^a^,^b^,^*()

^a 江苏大学化学化工学院, 材料科学与工程学院, 药学院, 能源研究院, 江苏镇江 212013, 中国
^b 江苏江科石墨烯研究院有限公司, 江苏江科复合材料有限公司, 江苏镇江 212009, 中国
^c 江苏金天辰新材料有限公司, 江苏镇江 212000, 中国
^d 约贝州立大学化学系, 约贝州达马图鲁市, 尼日利亚
^e 尼苏莱·拉米多大学化学系, 吉加瓦州卡芬豪萨市, 尼日利亚

收稿日期:2025-10-10 接受日期:2026-02-22 出版日期:2026-09-18 发布日期:2026-09-05
通讯作者: *电子信箱: yldeng@ujs.edu.cn (邓伊琳),
chenmin3226@sina.com (陈敏),
xuyg@ujs.edu.cn (徐远国).
基金资助:
国家自然科学基金(W2433031);国家自然科学基金(22350410392);江苏省自然科学基金(BK20221295);2024年镇江市基础研究与发展计划(产业前瞻与共性关键技术GY2024027);2024年镇江市基础研究与发展计划(GJ2024012)

Vacancy-engineered Ru-based CNT electrocatalysts for ampere-level water splitting in alkaline and anion-exchange membrane water electrolyzers

Bashir Adegbemiga Yusuf^a^,¹, Hennayaka Mudiyanselage Charitha Madusanka Jayawardana^a^,¹, Waleed Yaseen^a, Jimin Xie^a^,^b, Yilin Deng^a^,^*(), Suci Meng^a^,^b, Yongming Li^c, Abdussamad Mukhtar Mohammed^d, Aminu Magaji^e, Min Chen^a^,^*(), Meng Xie^a, Yuanguo Xu^a^,^b^,^*()

^a School of Chemistry and Chemical Engineering, School of Materials Science & Engineering, School of Pharmacy, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^b Jiangsu Jiangke Graphene Research Institute Co., LTD., Jiangsu Jiangke Composite Material Co., Ltd., Zhenjiang 212009, Jiangsu, China
^c Jiangsu Jin Tianchen New Material Co., Ltd., Zhenjiang, Zhenjiang 212000, Jiangsu, China
^d Department of Chemistry, Yobe State University, Damaturu-Yobe State, Nigeria
^e Department of Chemistry, Sule Lamido University Kafin Hausa, Jigawa State, Nigeria

Received:2025-10-10 Accepted:2026-02-22 Online:2026-09-18 Published:2026-09-05
About author:First author contact:1 共同第一作者.
1 Contributed equally to this work.
Supported by:
The National Natural Science Foundation of China(W2433031);The National Natural Science Foundation of China(22350410392);The Natural Science Foundation of Jiangsu Province of China(BK20221295);The Fundamental Research and Development Plan of Zhenjiang City in 2024(产业前瞻与共性关键技术GY2024027);The Fundamental Research and Development Plan of Zhenjiang City in 2024(GJ2024012)

摘要/Abstract

摘要：

水分解制氢因其绿色环保特性而备受关注. 在阴离子交换膜水电解槽中, 铂(Pt)、钌(Ru)基贵金属电催化剂应用广泛, 但成本高, 且Ru基催化剂存在反应动力学与稳定性问题, 亟需开发低成本、低/无贵金属的替代催化剂. 负载型电催化剂凭借原子利用率高以及金属-载体相互作用可调等优势成为研究重点. 氧化钼(MoO_x)基材料在碱性条件下对析氢反应(HER)和析氧反应(OER)表现出优异催化活性, 性能可媲美铂. 但其在高电流密度与强碱性环境下易氧化溶解, 耐久性难以满足工业需求, 抑制溶解是提升其稳定性的关键. 将二氧化钼(MoO₂)与过渡金属复合, 并引入硼(B)、氮(N)等杂原子掺杂, 可有效提升其催化活性与稳定性.
本文系统地探究了Ru纳米颗粒与嵌入镍-碳纳米管网络中的B、N共掺杂MoO₂纳米颗粒(Ru/B, N-MoO₂@Ni/CNTs, 简称RBNM/CNTs)之间的相互作用机制. 优化后的金属-载体相互作用在Ru位点诱导产生适度的电子富集, 从而抑制了OER反应过程中的晶格氧机制, 同时通过富氧空位的MoO₂单元促进去质子化, 从而在活性和稳定性之间实现了良好的平衡. X-射线衍射、高角环形暗场扫描透射电镜以及X-射线光电子能谱结果表明, RBNM/CNTs催化剂中各原子均匀分布. 对RBNM/CNTs₅₀₀ (500 °C煅烧)的电子顺磁共振测试在g = 2.003处观察到明显的共振信号, 证实了丰富的氧空位的存在, 这些氧空位优化了Ru的电子结构, 有助于增强电解水性能. 在碱性条件下, RBNM/CNTS₅₀₀表现出优异的双功能电催化性能, 在10 mA cm^‒2的电流密度下, HER过电位仅需9 mV, OER过电位仅需166 mV. 用于全水分解时, 其电解池电压仅需1.42 V, 并且该催化剂能在1000 mA cm^‒2的大电流密度下稳定运行120 h. 原位拉曼进一步深入研究RBNM/CNTS₅₀₀在OER反应过程中的结构演变, 在 OER过程中, Mo物种被氧化为高价态(如MoO_x_>2), 与动态形成的RuO_x物种共同作为活性中心增强催化活性. 理论计算结果进一步阐明, 氧空位和杂原子掺杂协同调节了Ru位点的电子环境, 优化了氢的吸附/解吸, 降低了水活化的能垒, 并在OER过程中稳定了含氧中间体. Ru-O-Mo键的强电子耦合以及导电的碳纳米管骨架进一步增强了电荷转移和结构稳定性, 确保了苛刻的条件下也能保持长期稳定性.
综上, 本工作通过构建RBNM/CNTs复合催化剂, 利用金属-载体相互作用在Ru位点诱导产生适度的电子富集, 通过吸附能调控和表面重构协同作用, 有效提升了催化活性与稳定性. 该研究为设计用于实际水分解的高效耐用电催化剂提供了新的思路与方向.

关键词: 空位工程, 钌基电催化剂, 安培级全水分解, 阴离子交换膜水电解槽

Abstract:

Robust metal-support interactions are crucial for designing efficient and corrosion-resistant electrocatalysts, as they significantly enhance charge separation and catalytic activity while also improving the stability and atomic utilization of metal catalysts. Here, we reported a temperature-regulated synthesis strategy to fabricate a self-supporting Ru/B,N co-doped MoO₂ electrocatalyst on a CNT framework (RBNM/CNTs₅₀₀), designed to simultaneously enhance catalytic activity and durability under practical electrolyzer conditions. The RBNM/CNTs₅₀₀ featured a unique nanostructure with excellent conductivity and strong chemical stability, while oxygen-vacancy-rich MoO₂ units at the interface reinforced metal-support interactions. This architecture stabilized Ru species during the OER and facilitated proton transfer, thus accelerating HER kinetics as confirmed by density functional theory calculations. As a result, RBNM/CNTs₅₀₀ exhibited outstanding bifunctional electrocatalytic performance, achieving exceptionally low overpotentials of 9 mV for the HER and 166 mV for the OER at 10 mA cm^‒2, along with superior overall water-splitting activity characterized by a low cell voltage of 1.42 V and stable ampere-level operation at 10, 1000, and 2000 mA cm^‒2 in alkaline media. When integrated into an anion-exchange membrane water electrolyzer, RBNM/CNTs₅₀₀ demonstrated exceptional durability and surpassed benchmark electrocatalysts in performance. This study offers mechanistic insights into defect engineering and underscores a rational design approach for next-generation energy conversion devices.

Key words: Vacancy engineering, Ruthenium-based electrocatalysts, Ampere level overall water splitting, Anion exchange membrane water electrolyzer

Yusuf Bashir Adegbemiga, Jayawardana Hennayaka Mudiyanselage Charitha Madusanka, Yaseen Waleed, 谢吉民, 邓伊琳, 孟素慈, 李永明, Mohammed Abdussamad Mukhtar, Magaji Aminu, 陈敏, 谢萌, 徐远国. 空位工程构筑钌基碳纳米管用于安培级电解水[J]. 催化学报, 2026, 88: 279-294.

Bashir Adegbemiga Yusuf, Hennayaka Mudiyanselage Charitha Madusanka Jayawardana, Waleed Yaseen, Jimin Xie, Yilin Deng, Suci Meng, Yongming Li, Abdussamad Mukhtar Mohammed, Aminu Magaji, Min Chen, Meng Xie, Yuanguo Xu. Vacancy-engineered Ru-based CNT electrocatalysts for ampere-level water splitting in alkaline and anion-exchange membrane water electrolyzers[J]. Chinese Journal of Catalysis, 2026, 88: 279-294.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65116-9

https://www.cjcatal.com/CN/Y2026/V88/I9/279

图/表 8

Scheme 1. A schematic illustration of the synthesis pathway of the standard RBNM/CNTsx.

Fig. 1. Morphology and structural characterization of the electrocatalysts. SEM images of RBNM/CNTs500 (a,b), RBNM/CNTs400 (c), RBNM/CNTs450 (d), RBNM/CNTs550 (e), and RBNM/CNTs600 (f). TEM image (g), HRTEM images (h,i), SAED pattern (j), HAADF line scan (k,l), and HAADF-STEM elemental mapping (m) of RBNM/CNTs500.

Fig. 2. Phase and surface chemical characterization of RBNM/CNTsx. PXRD patterns (a), Raman spectra (b), N2 adsorption-desorption isotherms (c), and high resolution XPS spectra of Ni 2p (d), Mo 3d (e), Ru 3p (f), N 1s (g), B 1s (h), O 1s (i), C 1s + Ru 3d (j), and water contact angle measurements (k) for RBNM/CNTs500.

Fig. 3. Evaluation of HER performance and durability in 1.0 mol L?1 KOH electrolyte. (a) LSV curves. (b) Corresponding overpotential values with error bars from multiple repeated experiments. (c) Comparison of η10 for RBNM/CNTs500 in HER with recently reported NF-based electrocatalysts (references in the Supporting Information). (d) Tafel plots. (e) CV curves. (f) Cdl values. (g) EIS data for synthesis catalyst. (h) Multistep CP test at current densities from 10 to 50 mA cm?2. (i) Long-term CA test of RBNM/CNTs500 at 100 mA cm?2 (inset: LSV curves before and after the 100-h stability test).

Fig. 4. Evaluation of OER performance and durability in 1.0 mol L?1 KOH electrolyte. (a) LSV curves. (b) Corresponding overpotential values with error bars from multiple repeated experiments. (c) Comparison of η10 for RBNM/CNTs500 in HER with recently reported NF-based electrocatalysts (references in the Supporting Information). (d) Tafel plots. (e) CV curves. (f) Cdl values. (g) EIS data for synthesis catalyst. (h) Multistep CP test at current densities from 10 to 50 mA cm?2. (i) Long-term CA test of RBNM/CNTs500 at 100 mA cm?2 (inset: LSV curves before and after the 100-h stability test).

Fig. 5. Overall water splitting results. (a) Schematic of the electrolytic water electrolyzer. (b) LSV curves of the two electrode electrolyzer. (c) Photograph of the RBNM/CNTs500‖RBNM/CNTs500 electrolyzer powered by a single commercial 1.5 V battery. (d) LSV curve under simulated industrial conditions. (e) Cell voltage comparison with recently reported noble-metal-based catalysts at 1 A cm?2. (f) Gas collection in an H-type cell: measured gas volumes and corresponding Faradaic efficiencies. (g) Long-term chronopotentiometry test at 1 A cm?2 for 120 h under simulated industrial conditions.

Fig. 6. DFT calculations. (a) Gibbs free energy diagram for the HER. (b) Gibbs free energy diagram for H2O dissociation. (c) Gibbs free energy diagram for the OER. (d) Top and side views of the optimized structures of Ru, Ru/B,N-MoO2@CNTs, and Ru/B,N-MoO2@CNTs-Ov. (e) Charge density difference plots (top and side views) of Ru/B,N-MoO2@CNTs and Ru/B,N-MoO2@CNTs-Ov, where yellow and blue regions denote electron accumulation and electron depletion, respectively. (f) Bader charge analysis of Ru, Mo, O, B, N, and neighboring C atoms in Ru/B,N-MoO2@CNTs and Ru/B,N-MoO2@CNTs-Ov.

Fig. 7. Electrochemical performance of the water-splitting cells. (a) Schematic illustration of the AEMWE setup. Polarization curves of RBNM/CNTs500 in 1.0 and 6.0 mol L?1 KOH at 25 and 60 °C (without iR correction). (b) LSV curves for HER. (c) Summary of HER overpotentials. (d) LSV curves for OER. (e) Summary of OER overpotentials. (f) OWS performance of the RBNM/CNTs500(+)‖RBNM/CNTs500(-) configuration. (g) Summary of cell voltages required for overall water splitting. (h) Durability measurements of the AEMWE cell in 6.0 mol L?1 KOH at 60 °C.

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空位工程构筑钌基碳纳米管用于安培级电解水

Vacancy-engineered Ru-based CNT electrocatalysts for ampere-level water splitting in alkaline and anion-exchange membrane water electrolyzers

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