The article presents an analysis of the synergy of structural transformations of phyllosilicates subjected to high temperatures and microwave radiation in terms of the destruction and formation of crystal structures. Studying the synergy of transformations of crystal structures is essential for the development of new materials and technologies, because it helps to create materials with unique properties, which cannot be obtained when using the same factors separately. The material used in the study was a polymineral complex, which contained quartz, montmorillonite, kaolinite, chlorite, paragonite, and iron oxides (listed from the largest to the smallest mass fraction). The methods used in the study allowed us to assess the structural transformations. Averaged structural formulas of the studied phyllosilicates were calculated using the oxygen method combined with a recalculation method based on the results of a microprobe analysis. Differential thermal analysis demonstrated a synergistic effect of high temperature and microwave fields registered as a decrease inthe temperature gradient of the ceramics and initiation of the sintering process at lower temperatures and with greater intensity. All the treated samples contained the amorphous phase in significant concentrations: from 15 to 25 vol. %. Half of the three-layer phyllosilicates (chlorite and montmorillonite) were destroyed by the microwave field. Kaolinite and paragonite practically did not react to external factors. The synergistic effect was the most obvious in the structural transformations of silicon and iron oxides. Our experiments demonstrated for the first time the mechanism of formation of magnetite and hematite crystals from X-ray amorphous iron-containing films covering the particles of clay minerals. The use of the MW field and the resulting dehydration led to the formation of crystals of nuclei of iron oxides. The following high-temperature processes activated an increase in aggregated iron (magnetite and hematite). The X-ray diffraction analysis determined the presence of a synergistic effect in the evolution of structures, which could not be identified by means of IR-spectroscopy. The EPR spectroscopy allowed us to register the states of rare irregular cells with foreign paramagnetic atoms. The shift of the foreign Fe3+ from the geometric centers of octahedral crystal cells towards the minima of potential energy caused by the Jahn-Teller effect decreased the potential energy of the crystal lattice. At the same time, some chemical bonds forming the crystal cellbecame stronger, while others weakened
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