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Photo-Excited High-Spin State Ni (III) Species in Mo-Doped Ni3S2 for Efficient Urea Oxidation Reaction.
Wang, Peichen; Zheng, Wei; Qu, Yafei; Duan, Naiyuan; Yang, Yang; Wang, Dongdong; Wang, Hui; Chen, Qianwang.
Afiliación
  • Wang P; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Zheng W; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Qu Y; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Duan N; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Yang Y; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Wang D; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
  • Wang H; The High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, 230031, China.
  • Chen Q; Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
Small ; : e2403107, 2024 Jul 19.
Article en En | MEDLINE | ID: mdl-39030942
ABSTRACT
Designing robust catalysts for increasing the sluggish kinetics of the urea oxidation reaction (UOR) is challenging. Herein, the regulation of spin states for metal active sites by photoexcitation to facilitate the adsorption of urea and intermediates is demonstrated. Mo-doped nickel sulfide nanoribbon arrays (Mo-Ni3S2@NMF) with excellent light-trapping capacity are successfully prepared. Under AM 1.5G illumination, the activity of the Mo-Ni3S2@NMF exhibits a 50% improvement in the UOR current. Compared with those under dark conditions, Mo-Ni3S2@NMF achieve 10 mA cm-2 at 1.315 VRHE for UOR and 1.32 Vcell for urea electrolysis, which are decreases of 15 and 80 mV, respectively. The electron spin resonance, in situ Fourier transform infrared spectroscopy analysis and density functional theory calculations reveal that illumination led to the formation of Ni3+ active sites in a high-spin state, which strengthens the d-p orbital hybridization of Ni-N, hence facilitating the adsorption of urea. C─N cleavage of the *CONN intermediate is further inhibited, which promotes the oxidation of urea molecules via the active N2 pathway, thereby accelerating the UOR rate.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Small Asunto de la revista: ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Small Asunto de la revista: ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania