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2025 (English) In: Carbon Energy, E-ISSN 2637-9368, article id e672Article in journal (Refereed) Epub ahead of print
Abstract [en] Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds, but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis. Herein, we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides (Ni1−xFexPS3) during the oxidation of benzylamine (BA). In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1−x)FexPS3 undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide (NiFeOOH/Ni1−xFexPS3) heterostructure. Interestingly, the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53% for benzonitrile (BN) synthesis. Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1−xFexPS3 heterostructure could offer optimum free energy for BA adsorption and BN desorption, resulting in promising BN synthesis.
Place, publisher, year, edition, pages
John Wiley & Sons, 2025
Keywords 2D layered materials, benzylamine oxidation, metal phosphorus trichalcogenides, surface‐reconstructed heterostructure
National Category
Materials Chemistry
Research subject
Experimental Physics
Identifiers urn:nbn:se:ltu:diva-111800 (URN) 10.1002/cey2.672 (DOI) 001390533300001 () 2-s2.0-85214479017 (Scopus ID)
Funder The Kempe Foundations
Note Funder: National Natural Science Foundation of China (22179029); Fundamental Research Funds for the Central Universities (buctrc202324); BAST (BYESS202309); Ministero dell'Istruzione, dell'Università e della Ricerca (2022FNL89Y);
Full text license: CC BY
2025-03-032025-03-032025-03-03