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The apatite phase already appears after milling for 5 min. Phase, structural and microstructural studies on the nanocrystalline lanthanum silicates were carried out by using XRD, TEM, and IR, <jats:sup>27<\/jats:sup>Al and <jats:sup>29<\/jats:sup>Si MAS NMR spectroscopy to clarify the mechanism of ATLS formation. The cluster\u2010topotactic mechanism of the formation of apatite by mechanochemical treatment involving hydration of the starting compounds and acid\u2013base reactions is suggested. Al\u2010doping results in promoting the formation of apatite. However, a secondary LaAlO<jats:sub>3<\/jats:sub> phase may be present in the sample depending on its stoichiometry. This suggests the existence of a biphase domain in the La<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub>\u2013SiO<jats:sub>2<\/jats:sub>\u2013Al<jats:sub>2<\/jats:sub>O<jats:sub>3<\/jats:sub> phase diagram at room temperature, in which Al\u2010doped apatite and LaAlO<jats:sub>3<\/jats:sub> phases coexist. 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