Preparation of two-dimensional (2D) ferromagnetic nanomaterials and the study of their magnetic sources are crucial for the exploration of new materials with multiple applications. Herein, two-dimensional room-temperature ferromagnetic (FM) CaTiO3 nanosheets are successfully constructed with the assistance of supercritical carbon dioxide (SC CO2). In this process, the SC CO2-induced strain effect can lead to lattice expansion and introduction of O vacancies. More importantly, experimentally it can be found out that the breakage of the Ti-O2 bond by CO2 directly results in the equatorial plane of the TiO6 octahedron being exposed. This leads to more opportunities for oxygen vacancies and low-valent titanium to appear, where Ti3+ can optimize the spin structure, releasing the macroscopic magnetization. Greatly improved room-temperature ferromagnetic behavior, with an optimal magnetization of 0.1661 emu g-1 and a high Curie temperature (Tc) of 300 K can be achieved.
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