Vibrational Spectral Analysis of Natisite (Na(2)TiSiO(5)) and its Structure Evolution in Water and Sulfuric Acid Solutions

Natisite (Na(2)TiSiO(5)) is a layered sodium titanosilicate containing TiO(5) square pyramids. The structure evolution of natisite in water and acid solutions is the basis for its potential applications. With Na(2)SiO(3) as the silicon source, natisite with the shape of the square sheet was selectively prepared from the hydrothermal method with 14.3 mol/L NaOH solution at 240 °C. Natisite has 20 Raman active modes and 22 infrared active modes from the first-principles calculations within density functional theory, and the calculated Raman and infrared spectra agree well with the experimental ones. The characteristic Raman peak at 844 cm(−1) is caused by the symmetric stretching of the apical Ti–O bond in the TiO(5) unit, assigning to A(1g) and B(2g) modes. Natisite remains relatively stable in water with a sodium leaching percentage of lower than 6%. When washing with sulfuric acid solutions, the interlayer spacing of natisite is reduced due to the extensive removal of sodium ions, and an intermediate composed of SiO(4) and newly formed TiO(6) units may be formed. Moreover, after washing with water and acid solutions, 95.5%, 63.4%, and 35.2% of Na, Si, and Ti in natisite can be leached in total, respectively, resulting in the structural disintegration of natisite.