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ChemPhysMater 2024年第3期3卷 329-340页

作者： Patrick Ndouka Ndouka stephane kenmoe Jacques Richard Mache Elie Acayanka Dick Hartmann Douma Ralph Gebauer Patrick Mountapmbeme Kouotou Department of Chemistry Faculty of SciencesUniversity of MarouaP.O.Box 814 MarouaCameroon Department of Theoretical Chemistry University of Duisburg-EssenD-45141 EssenGermany Department of Mining Engineering School of Geology and Mining EngineeringUniversity of NgaoundéréP.O.Box 115 MeigangaCameroon Department of Inorganic Chemistry Faculty of ScienceUniversity of YaoundéIP.O.Box 812 YaoundéCameroon Groupe de Simulations Numériques en Magnétisme et Catalyse Facultédes Sciences et TechniquesUniversitéMarien NgouabiB.P.69 BrazzavilleCongo The Abdus Salam International Centre for Theoretical Physics(ICTP) 34151 TriesteItaly National Advanced School of Engineering of Maroua University of MarouaP.O.Box 46 MarouaCameroon Higher Institute of Agriculture WoodWater and EnvironmentUniversity of EbolowaP.O.Box 118 EbolowaCameroon

In this study,Mn_(3)O_(4) spherical particles(SPs)were synthesized by the sol-gel process,after which they were thermally annealed at 400℃,and comprehensively characterized.X-ray Diffraction(XRD)revealed that Mn_(3)O_(4) exhibited a tetragonal spinel structure,and Fourier transformed infrared(FTIR)spectroscopy identified surfaceadsorbed functional *** electron microscopy(SEM)and the specific surface area analyses by Brunauer−Emmett−Teller(BET)revealed a porous,homogeneous surface composed of strongly agglomerated spherical grains with an estimated average particle size of∼35 nm,which corresponded to a large specific surface area of∼81.5 m^(2)/g.X-ray photoelectron spectroscopy(XPS)analysis indicated that Mn_(3)O_(4) was composed of metallic cations(Mn^(4+),Mn_(3)+,and Mn^(2+))and oxygen species(O_(2)−,OH−and CO_(3)2−).The optical bandgap energy is∼2.55 *** of the catalytic performance of the Mn_(3)O_(4) SPs indicated T90 conversion of CH4 to CO_(2) and H2O at 398℃ for gas hourly space velocity(GHSV)of 72000 mL^(3) g^(−1) h^(−1).This observed performance can be attributed to the cooperative effects of the smallest spherical grain size with a mesoporous structure,which is responsible for the larger specific surface area and available surface-active oxygenated *** cooperative effect of the good reducibility,higher ratio of active species(OLat/OAds),and results of density functional theory(DFT)calculations suggested that the total oxidation of CH4 over the mesoporous Mn_(3)O_(4) SPs might take place via a two-term process in which both the Langmuir−Hinshelwood and Mars−van Krevelen mechanisms are cooperatively involved.

关键词： Sol-gel Manganese oxide Catalytic oxidation Methane Langmuir−Hinshelwood mechanism Mars−van Krevelen route Two−term process

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