Manganese oxides were synthesized systematically via the solution combustion procedure using two kinds of fuels, namely glycine and urea. The influences of the type of fuel and the fuel ratio were deeply investigated to explain the phase evolution and morphology of the product. The synthesized nanostructured powder was characterized by X-ray diffraction, particle size analysis, and FESEM. Furthermore, the thermodynamic aspects of all the synthesis reactions were studied by the calculation of the adiabatic temperature. Various manganese oxides, such as MnO, Mn3O4, Mn2O3, and MnO2, were obtained by varying the fuel ratio from 0.15 to 2. It was found that decreasing the fuel ratio promoted the formation of MnO2 by declining the combustion temperature and reductive conditions of the system. However, α-MnO2 could be simply achieved by adding KNO3 in a modified solution combustion process under fuel-lean conditions. Further heat treatment of the product was found to increase the crystallinity of the α-MnO2 nanoparticles.

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