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Anatase (TiO2) nanoparticles co-doped with Ni/Al ions were synthesized by a thermo-precipitation method. The samples were characterized by using X‐Ray diffraction and optical absorption spectroscopy. The structural/optical investigations established the development of substitutional solid solutions: TiO2:Ni:Al. The magnetization investigations were performed to study the generated stable ferromagnetic properties of the samples due to the Ni2+ doping. To boost the created ferromagnetic properties, Al ions co-dopings were employed to supply/densify the itinerant electrons. It was planned to decide the suitable hydrogenation conditions and temperature (TH), which are necessary to create appreciable strength of ferromagnetic properties in the host co-doped samples based on TiO2 for practical uses. The results established that the ferromagnetic energy (Umag) was increased by ~240% and the saturation magnetization by ~140% with increasing of TH from 400 oC to 500oC. The obtained Msat was higher by ~50 times than that previously attained for Ni-doped TiO2. Such novel results were discussed and explained through the spin-spin Heisenberg interactions.
