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

作     者：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 

作者机构：State Key Laboratory of Chemical Resource EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijingChina CAS Key Laboratory of Nanosystem and Hierarchical FabricationNational Center for Nanoscience and Technology(NCNST)BeijingChina Shaanxi Provincial Key Laboratory of Electroanalytical ChemistryKey Laboratory of Synthetic and Natural Functional Molecule of the Ministry of EducationCollege of Chemistry&Materials ScienceNorthwest UniversityXi'anChina State Key Laboratory of Multiphase Flow in Power EngineeringInternational Research Center for Renewable EnergyXi'an Jiaotong UniversityShaanxiChina Fundamental Science Center of Rare EarthsGanjiang Innovation AcademyChinese Academy of ScienceGanzhouChina Ocean Hydrogen Energy R&D CenterResearch Institute of Tsinghua University in ShenzhenShenzhenChina Department of Molecular Sciences and NanosystemsCa'Foscari University of VeniceVenezia MestreItaly Testing and Analysis CenterInstitute of Chemistry Chinese Academy of SciencesBeijingChina Department of Engineering Sciences and MathematicsDivision of Materials ScienceLuleåUniversity of TechnologyLuleåSweden 

出 版 物：《Carbon Energy》 (碳能源(英文))

年 卷 期：2025年第7卷第3期

页      面：133-147页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：National Natural Science Foundation of China,Grant/Award Number:22179029 Fundamental Research Funds for the Central Universities,Grant/Award Number:buctrc202324 Young Elite Scientists Sponsorship Program by BAST,Grant/Award Number:BYESS2023093 Ministero dell'Istruzione,dell'Universitàe della Ricerca,Grant/Award Number:2022FNL89Y Kempestiftelserna 

主　　题：2D layered materials benzylamine oxidation metal phosphorus trichalcogenides surfacereconstructed heterostructure 

摘      要：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 ***,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(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)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))***,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)*** calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.