Acta Phys. -Chim. Sin. ›› 2025, Vol. 41 ›› Issue (8): 100083.doi: 10.1016/j.actphy.2025.100083

• ARTICLE • Previous Articles     Next Articles

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. 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)

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