Co/Mn/Mo掺杂加速NiSe2重构以提高其电催化尿素氧化性能

doi:10.1016/j.actphy.2025.100083

物理化学学报 >> 2025, Vol. 41 >> Issue (8): 100083.doi: 10.1016/j.actphy.2025.100083

Co/Mn/Mo掺杂加速NiSe₂重构以提高其电催化尿素氧化性能

雷明杰¹, 胡文婷², 林可心¹, 孙秀娟¹^,*(), 张澔珅¹, 钱烨¹, 康彤玥¹, 吴秀琳¹, 廖海龙¹, 潘园¹, 张玉微²^,*(), 魏笛野¹^,*(), 高平¹

¹ 湘潭大学化学学院, 环境友好与利用教育部重点实验室, 湖南湘潭 411105
² GDMPA手性药物过程控制和质量评价重点实验室, 华南师范大学化学学院, 广州生物医学分析化学重点实验室, 广东广州 510006

收稿日期:2025-01-21 修回日期:2025-03-08 录用日期:2025-03-23 发布日期:2025-06-07
通讯作者: Email: sunxj594@xtu.edu.cn (孙秀娟)ywzhang@scnu.edu.cn (张玉微)weidiye@163.com (魏笛野)
基金资助:
湖南省教育厅科研基金(23B0114); 湖南省自然科学基金(2024JJ5368); 国家自然科学基金(22122402); 广东省自然科学基金(2021B1515020048)

Accelerating the reconstruction of NiSe₂ by Co/Mn/Mo doping for enhanced urea electrolysis

Mingjie Lei¹, Wenting Hu², Kexin Lin¹, Xiujuan Sun¹^,*(), Haoshen Zhang¹, Ye Qian¹, Tongyue Kang¹, Xiulin Wu¹, Hailong Liao¹, Yuan Pan¹, Yuwei Zhang²^,*(), Diye Wei¹^,*(), Ping Gao¹

¹ Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education, College of Chemistry, Xiangtan University, Xiangtan 411105, Hunan Province, China
² GDMPA Key Laboratory for Process Control and Quality Evaluation of Chiral Pharmaceuticals, Guangzhou Key Laboratory of Analytical Chemistry for Biomedicine, School of Chemistry, South China Normal University, Guangzhou 510006, Guangdong Province, China

Received:2025-01-21 Revised:2025-03-08 Accepted:2025-03-23 Published:2025-06-07
Contact: Email: sunxj594@xtu.edu.cn (Xiujuan Sun)ywzhang@scnu.edu.cn (Yuwei Zhang)weidiye@163.com (Diye Wei)
Supported by:
the Scientific Research Fund of Hunan Provincial Education Department(23B0114); the Natural Science Foundation of Hunan Province(2024JJ5368); the National Natural Science Foundation of China(22122402); the Natural Science Foundation of Guangdong Province(2021B1515020048)

1. ACTPHY-2025.100083-SI-14p.pdf(10333KB)

摘要/Abstract

摘要：

尿素氧化反应(UOR)是一种很有前途的可再生能源生产技术，为电解水制氢提供了有效的替代方案，因此开发高效稳定的UOR催化剂至关重要。本文通过NaBH₄还原和硒化策略合成了富含Co、Mn和Mo的硒化镍催化剂(NiCoMnMo-Se)，该催化剂具有球形纳米颗粒与纳米片共存结构。X射线光电子能谱(XPS)、紫外-可见分光光度法(UV-vis)和原位bode相图表明，Mn和Mo的协同效应调节了Ni/Co的电子结构，提高了硒化物的电导率并加速加速电荷转移动力学，从而促进Ni²⁺/Co²⁺快速转变为活性Ni³⁺/Co³⁺，并显著降低了NiCoMnMo-Se的起始电位。在UOR过程中，大部分Mo和Se被氧化成钼酸盐和硒酸盐溶解在电解质中，暴露出更多的Ni(Co)OOH活性位点，从而加快UOR反应。另外，Mn的引入稳固了活性位点，极大地增强催化剂的整体稳定性。正如预期的那样，NiCoMnMo-Se催化剂在UOR过程中表现出优异的电催化和稳定性性能，在仅1.38 V vs. RHE (相对于可逆氢电极)的电位下实现了50 mA·cm⁻²的电流密度，并在50 mA·cm⁻²电流密度下运行50 h后电压仅上升3.0%。当NiCoMnMo-Se和商业Pt/C组装成用于碱性尿素电解的双电极体系时，它只需要1.59 V vs. RHE便达到50 mA·cm⁻²。

关键词: 尿素氧化反应, 制氢, NiCoMnMo-Se, 协同效应, 尿素电解, 镍基硒化物

Abstract:

As a highly promising renewable energy technology, the urea oxidation reaction (UOR) not only enables efficient utilization of urea wastewater but also provides an effective alternative for hydrogen production via water electrolysis, thereby reducing the energy consumption of conventional electrolysis. Therefore, the development of UOR catalysts with high catalytic activity and long-term stability is of great significance for advancing clean energy technologies. In this study, a nickel-based selenide catalyst (NiCoMnMo-Se) with coexisting nanoparticles and nanosheets was synthesized using a NaBH₄ reduction and selenization strategy. X-ray photoelectron spectroscopy (XPS), ultraviolet-visible (UV-vis) and in situ bode phase plots, revealed that the synergistic effect of Mn and Mo regulated the electronic structure of Ni/Co, enhancing the conductivity of selenide and accelerating charge transfer kinetics, which facilitates the rapid transformation of Ni²⁺/Co²⁺ into active Ni³⁺/Co³⁺ and significantly reduces the onset potential of NiCoMnMo-Se. During the UOR process, Mo and Se are oxidized to form molybdate and selenate, which subsequently dissolve into the electrolyte. This transformation results in the partial conversion of the original spherical nanoparticle surfaces into nanosheets, thereby exposing more Ni(Co)OOH active sites and significantly enhancing the UOR reaction. Additionally, the introduction of Mn stabilizes the active sites, thereby improving the overall stability of the catalyst. As anticipated, the synthesized NiCoMnMo-Se catalyst demonstrates outstanding electrocatalytic performance and stability in the UOR process, achieving a current density of 50 mA·cm⁻² at a potential of only 1.38 V vs. RHE (reversible hydrogen electrode), with a voltage increase of only 3.0% after 50 h of operation at a 50 mA·cm⁻². When NiCoMnMo-Se and commercial Pt/C were assembled into a dual-electrode system for alkaline urea electrolysis, it only requires 1.59 V vs. RHE to achieve a current density of 50 mA·cm⁻². This paper designs an efficient and stable Ni-based selenide catalyst, which is expected to promote the further development of selenides in relevant energy technologies.

Key words: Urea oxidation reaction, Hydrogen production, NiCoMnMo-Se, Synergetic effect, Urea electrolysis, Ni-based selenide

雷明杰, 胡文婷, 林可心, 孙秀娟, 张澔珅, 钱烨, 康彤玥, 吴秀琳, 廖海龙, 潘园, 张玉微, 魏笛野, 高平. Co/Mn/Mo掺杂加速NiSe₂重构以提高其电催化尿素氧化性能[J]. 物理化学学报, 2025, 41(8), 100083. doi: 10.1016/j.actphy.2025.100083

Mingjie Lei, Wenting Hu, Kexin Lin, Xiujuan Sun, Haoshen Zhang, Ye Qian, Tongyue Kang, Xiulin Wu, Hailong Liao, Yuan Pan, Yuwei Zhang, Diye Wei, Ping Gao. Accelerating the reconstruction of NiSe₂ by Co/Mn/Mo doping for enhanced urea electrolysis[J]. Acta Phys. -Chim. Sin. 2025, 41(8), 100083. doi: 10.1016/j.actphy.2025.100083

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100083

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I8/100083

图/表 6

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Co/Mn/Mo掺杂加速NiSe₂重构以提高其电催化尿素氧化性能

Accelerating the reconstruction of NiSe₂ by Co/Mn/Mo doping for enhanced urea electrolysis

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