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The aldol condensation of acetone under supercritical conditions at 300–400°C and 11.0 MPa was carried out on BaSnO3-450 and BaSnO3-750 catalysts prepared by calcination of BaSn(OH)6 at 450 and 750°C, respectively. Conducting the reaction under these conditions makes it possible to overcome the problem of catalyst deactivation by coking and to obtain valuable chemicals with high selectivity. At 300°C, both catalysts provide selectivity of 85–87% to isomeric mesityl oxides (C6 products). At 400°C with the BaSnO3-450 catalyst, the selectivity significantly changes from C6 to C9 (phorones). Powder X-ray diffraction and TEM data attest to the multiphase nature of the samples, which contain barium stannates, barium carbonate, and tin oxide. It was found that the catalyst structure rearranges in situ, which greatly affects the catalytic properties and is most pronounced for BaSnO3-450. [ABSTRACT FROM AUTHOR]