第41卷第3期2024年6月J.At.Mol.Phys.,2024,41:032004(6pp)Fe/Co/Ni－N共掺杂石墨烯氧还原反应活性的DFT研究马俊杰，宁错，王婷"，刘建峰"，袁斌霞"，潘卫国"，施正荣12（1.上海电力大学能源与机械工程学院，上海200090；2.上海非碳基能源转换与利用研究院，上海200240）摘要：为了研究Fe/Co/Ni-N掺杂石墨烯的氧还原反应（ORR）活性，比较单金属原子和氮不同的掺杂方式对石墨烯ORR活性的影响。利用MaterialsStudio软件建立了Fe/Co/Ni-N掺杂石墨烯模型,然后将氧气分子分别吸附在Fe/Co/Ni-N掺杂石墨烯模型表面上，采用CASTEP模块对构建的模型进行结构优化并模拟计算，分析了Fe/Co/Ni-N掺杂石墨烯的吸附能、脱附能和导电性变化规律：基于模拟计算，发现单金属原子掺杂石墨烯时,Fe掺杂石墨烯的ORR活性优于Co和Ni；单金属原子和氮共掺杂石墨烯时，Fe-N掺杂石墨烯的ORR活性高于Co-N和Ni-N掺杂石墨烯，且M-N4-G形态的ORR活性优于M-N,-G、M-N2-G和M-N,-G.关键词：单金属原子；氮掺杂；石墨烯；氧还原反应；DFT模拟中图分类号：0646.51DFTstudyonoxygenreductionreactionactivityofFe/Co/Ni-Ndopedgraphene原子与分子物理学报JOURNALOFATOMICANDMOLECULARPHYSICS文献标识码：AVol.41No.3Jun.2024D0I:10.19855/j.1000-0364.2024.032004MAJun-Jie',NINGKai',WANGTing,LIUJian-Feng',YUANBin-Xia',PANWei-Guo',SHIZheng-Rong"1,2(1.CollegeofEnergyandMechanicalEngineering,ShanghaiUniversityofElectricPower,Shanghai200090,China;2.ShanghaiNon-carbonEnergyConversionandUtilizationInstitute,Shanghai200240,China)Abstract:Inordertostudytheoxygenreductionactivity(ORR)ofFe/Co/Ni-Ndopedgraphenes,theinflu-encesofsinglemetalatomandnitrogenco-dopingonORRactivityofgraphenewerecompared.TheFe/Co/Ni-NdopedgraphenemodelswereestablishedusingMaterialsStudio,andthenoxygenmoleculeswereadsorbedrespectivelyonthesurfacesofFe/Co/Ni-Ndopedgraphenemodels.CASTEPmodulewasusedtooptimizethestructureofthemodelandsimulationcalculation.Theadsorptionenergies,desorptionenergiesandconductivitiesofFe/Co/Ni-Ndopedgrapheneswereanalyzed.Basedonthesimulationresults,itisfoundthattheORRac-tivityofFedopedgrapheneisbetterthanthatofCoorNidopedgraphenewhengrapheneisdopedwithsinglemetalatom.AsgrapheneisCo-dopedwithsinglemetalatoman...
