非晶-晶体异质结构RuMoNiN/Ni-MoO2用于高效稳定的碱性析氢反应

doi:10.1016/S1872-2067(26)65011-5

催化学报 ›› 2026, Vol. 84: 96-105.DOI: 10.1016/S1872-2067(26)65011-5

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

初铭涛^a^,^b, 张慧敏^a^,^b, 任变清^a^,^b, 曹景^a^,^b, 章腾^a^,^b, 宋平^a, 王子准^c, 韩策^a(), 徐维林^a^,^b()

^a 中国科学院长春应用化学研究所, 电分析化学重点实验室, 吉林长春 130022
^b 中国科学技术大学应用化学与工程学院, 安徽合肥 230026
^c 吉林大学电子显微镜中心, 吉林长春 130012

收稿日期:2025-11-12 接受日期:2026-01-06 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: hance@ciac.ac.cn (韩策);
weilinxu@ciac.ac.cn (徐维林).
基金资助:
科技部重点研发计划(2022YFB4002000);科技部重点研发计划(2022YFA1203400);国家自然科学基金(22372155);国家自然科学基金(22102172);国家自然科学基金(22005294);吉林省氢能产业综合研究院科技专项(20240302002ZD)

Amorphous-crystalline heterostructured Ru_MoNiN/Ni-MoO₂ for highly efficient and stable alkaline hydrogen evolution reaction

Mingtao Chu^a^,^b, Huimin Zhang^a^,^b, Bianqing Ren^a^,^b, Jing Cao^a^,^b, Teng Zhang^a^,^b, Ping Song^a, Zizhun Wang^c, Ce Han^a(), Weilin Xu^a^,^b()

^a State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^b School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, Anhui, China
^c Electron Microscopy Center, Jilin University, Changchun 130012, Jilin, China

Received:2025-11-12 Accepted:2026-01-06 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: hance@ciac.ac.cn (C. Han),
weilinxu@ciac.ac.cn (W. Xu).
Supported by:
Key Research and Development Program sponsored by the Ministry of Science and Technology (MOST)(2022YFB4002000);Key Research and Development Program sponsored by the Ministry of Science and Technology (MOST)(2022YFA1203400);National Natural Science Foundation of China(22372155);National Natural Science Foundation of China(22102172);National Natural Science Foundation of China(22005294);Jilin Provincial Hydrogen Industrial Comprehensive Research Institute Science and Technology Special Project of China(20240302002ZD)

摘要/Abstract

摘要：

电解水析氢反应(HER)是实现清洁能源转化与储存的核心途径之一, 贵金属基材料因具备优异的电催化性能, 成为HER电催化剂的研究热点. 非晶化与异质结构是提升贵金属基材料HER催化性能的两大有效策略, 其中非晶化策略可赋予材料丰富的不饱和活性位点与灵活的原子排列方式, 构筑异质结构则能实现多晶相的精准耦合, 并通过界面电子结构调控, 促进电荷转移效率优化与反应能垒降低, 进而达成催化性能的协同增强. 然而, 开发简易、可控的方法构建兼具高活性与长稳定性的贵金属基非晶-晶体异质结构催化剂,仍是该领域亟待解决的关键问题, 对推动电解水技术的实际应用具有重要意义.

为解决碱性条件下HER催化剂活性不足、稳定性欠佳的关键技术难题, 本文选取(NH₄)₄[NiH₆Mo₆O₂₄]·5H₂O(NiMo₆)多酸作为钼-镍双金属前驱体, 利用多酸分子结构规整、元素组成可控及配位位点丰富的独特优势, 与三氯化钌水合物进行均匀复合, 在Ar/NH₃混合气氛下热解, 成功制备出由非晶Ru_MoNiN相和晶态Ni掺杂MoO₂相结合的异质结构电催化剂(Ru_MoNiN/Ni-MoO₂). 为系统探究催化剂的微观结构、电子态特征及催化反应机理, 本文采用X射线衍射、透射电镜(TEM)、X射线光电子能谱(XPS)等多种结构表征手段, 结合密度泛函理论计算开展深入研究. 研究结果表明, NiMo₆多酸前驱体的结构导向作用与NH₃气氛的修饰效应, 是形成独特非晶-晶体异质结构的核心因素; 该结构可通过‒NH₂基团的配位作用与异质界面的电子相互作用, 对Ru活性位点的电子结构实现协同调控, 从而有效降低碱性HER过程中水分解步骤的能垒, 并优化H中间体的吸附-脱附行为. 催化性能测试结果表明, 所制备的Ru_MoNiN/Ni-MoO₂异质结构催化剂展现出优异的HER电催化性能与工业应用潜力: 在10 mA cm^‒2的常规测试电流密度下, 过电位仅为18.3 mV, 优于商业Pt/C催化剂及多数已报道的贵金属基催化剂; 在1 A cm^‒2的工业级高电流密度下连续运行100 h后, 其过电位仅衰减62 mV, 未出现明显的微观结构坍塌, 表现出良好的催化稳定性与抗衰减能力. 稳定性测试后样品的XPS和TEM表征结果显示, 材料表面键合的‒NH₂基团出现了一定程度的流失, 从而导致了Ru位点电子结构的变化以及晶态Ru颗粒的出现. 这一现象再次印证了‒NH₂基团对于非晶Ru的形成以及电子结构调控意义重大.

综上, 本研究为贵金属基非晶-晶体异质结构电催化剂的简易构建与精准结构调控提供了建设性思路, 所揭示的配位作用与界面相互作用协同调控活性位点电子结构的机理, 也为设计高性能能源转化电催化剂提供了理论参考, 有望推动该类材料在电解水等领域的进一步发展.

关键词: 贵金属, 非晶态, 异质结构, 析氢反应, 电催化

Abstract:

The amorphization and heterostructuralization of noble metal-based materials are effective approaches to enhance the electrocatalytic performance towards the hydrogen evolution reaction (HER) in water splitting. Herein, (NH₄)₄[NiH₆Mo₆O₂₄]·5H₂O (NiMo₆) polyoxometalate was employed for the Ru combination to fabricate a heterostructured catalyst consisting of amorphous Ru_MoNiN and crystalline Ni-MoO₂ (Ru_MoNiN/Ni-MoO₂) via a simple annealing process under Ar/NH₃ atmosphere. Comprehensive structural characterizations and theoretical investigations suggest that the formation of such unique amorphous-crystalline heterostructures is governed by the application of NiMo₆ precursor and Ar/NH₃ atmosphere, which leads to the joint regulation on the electronic structure of Ru sites through -NH₂ coordination and heterostructured interaction, and thus facilitating the water dissociation and H intermediates sorption steps in the alkaline HER process. Accordingly, the as-fabricated Ru_MoNiN/Ni-MoO₂ manifests excellent HER performance demanding an overpotential of only 18.3 mV at the current density of 10 mA cm^‒2 with a minimal overpotential decay rate of 0.62 mV h^‒1 during continuous operation at 1 A cm^‒2. This work offers constructive suggestions for the facile construction and structural regulation of amorphous-crystalline heterostructured noble metal-based electrocatalysts for various promising energy applications.

Key words: Noble metal, Amorphous, Heterostructured, Hydrogen evolution reaction, Electrocatalysis

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: 96-105.

Mingtao Chu, Huimin Zhang, Bianqing Ren, Jing Cao, Teng Zhang, Ping Song, Zizhun Wang, Ce Han, Weilin Xu. Amorphous-crystalline heterostructured Ru_MoNiN/Ni-MoO₂ for highly efficient and stable alkaline hydrogen evolution reaction[J]. Chinese Journal of Catalysis, 2026, 84: 96-105.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65011-5

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Fig. 1. (a) Schematic illustration for the fabrication process of RuMoNiN/Ni-MoO2. (b) XRD patterns of RuMoNiN/Ni-MoO2, POM-pre-sample and Salt-pre-sample. TEM image (c), HRTEM image (d) and corresponding magnified lattice fringes (e) of RuMoNiN/Ni-MoO2. (f) HAADF-STEM image of the amorphous phase in RuMoNiN/Ni-MoO2. Inset: corresponding Fourier transform pattern. Elemental mappings (g) and line scanning analysis (h) of O, Mo, Ni, Ru, and N for RuMoNiN/Ni-MoO2. TEM (i), HRTEM (j) images and elemental mappings (k) of Ar-sample. (l) TEM images of POM-pre-sample.

Fig. 2. (a) XPS survey spectrum of RuMoNiN/Ni-MoO2. XPS spectra of Mo 3d (b), Ni 2p (c), and N 1s (d) for RuMoNiN/Ni-MoO2 and the POM-pre-sample. (e) XPS spectrum of Ru 3d for RuMoNiN/Ni-MoO2. (f) EPR spectra of RuMoNiN/Ni-MoO2 and POM-pre-sample.

Fig. 3. (a) LSV curves with 85% iR compensation for RuMoNiN/Ni-MoO2, POM-pre-sample, Salt-pre-sample, Ru-pre-sample, and Pt/C. Corresponding Tafel plots (b) and EIS spectra (c). (d) Electrochemical double-layer capacitances of RuMoNiN/Ni-MoO2, POM-pre-sample, Salt-pre-sample, and Ru-pre-sample. (e) Chronopotentiometry measurements of RuMoNiN/Ni-MoO2 at the current densities of 10 and 1000 mA cm?2.

Fig. 4. (a) Theoretical model of the amorphous-crystalline heterostructured RuMoNiN/Ni-MoO2 with diverse Ru sites from the top view. Bader charge analysis (b), and calculated free-energy profiles for water dissociation (c) and hydrogen sorption (d) at diverse Ru sites within RuMoNiN/Ni-MoO2.

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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

Amorphous-crystalline heterostructured Ru_MoNiN/Ni-MoO₂ for highly efficient and stable alkaline hydrogen evolution reaction

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