journal article·2025-03Open access

Electrochemical evolution of a metal oxyhydroxide surface on two‐dimensional layered metal phosphorus trisulfides enables the oxidation of amine to nitrile

Binglan Wu, Karim Harrath, Marshet Getaye Sendeku, Tofik Ahmed Shifa, Yuxin Huang, Jing Tai, Fekadu Tsegaye Dajan, Kassa Belay Ibrahim, Xueying Zhan, Zhenxing Wang, Elisa Moretti, Ying Yang, Fengmei Wang, Alberto Vomiero

Carbon Energy· Volume 7· Issue 3

Abstract

Abstract 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 (Ni 1− x Fe x PS 3 ) 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 ) Fe x PS 3 undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide (NiFeOOH/Ni 1− x Fe x PS 3 ) 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/Ni 1− x Fe x PS 3 heterostructure could offer optimum free energy for BA adsorption and BN desorption, resulting in promising BN synthesis.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Catalysis and Hydrodesulfurization Studies · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Chemical Resource Engineering, College of Chemistry Beijing University of Chemical Technology Beijing China

CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology (NCNST) Beijing China

Shaanxi Provincial Key Laboratory of Electroanalytical Chemistry, Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry & Materials Science Northwest University Xi'an China

State Key Laboratory of Multiphase Flow in Power Engineering, International Research Center for Renewable Energy Xi'an Jiaotong University Shaanxi China

Fundamental Science Center of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Science Ganzhou China

Ocean Hydrogen Energy R&D Center Research Institute of Tsinghua University in Shenzhen Shenzhen China

Department of Molecular Sciences and Nanosystems Ca' Foscari University of Venice Venezia Mestre Italy

Testing and Analysis Center, Institute of Chemistry Chinese Academy of Sciences Beijing China

Department of Engineering Sciences and Mathematics Division of Materials Science, Luleå University of Technology Luleå Sweden

Funding

National Natural Science Foundation of China · Fundamental Research Funds for the Central Universities · Kempestiftelserna

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