This study aimed to explore the effects of the full-scale replacement (up to 100%) of Ca2+ ions with Ag1+ ions in the structure of brushite (CaHPO4·2H2O). This substitution has potential benefits for producing monophasic and biphasic Ca1−xAgxHPO4·nH2O compounds. To prepare the starting solutions, (NH4)2HPO4, Ca(NO3)2·4H2O, and AgNO3 at different concentrations were used. The results showed that when the Ag/Ca molar ratio was below 0.25, partial substitution of Ca with Ag reduced the size of the unit cell of brushite. As the Ag/Ca molar ratio increased to 4, a compound with both monoclinic CaHPO4·2H2O and cubic nanostructured Ag3PO4 phases formed. There was a nearly linear relationship between the Ag ion ratio in the starting solutions and the wt% precipitation of the Ag3PO4 phase in the resulting compound. Moreover, when the Ag/Ca molar ratio exceeded 4, a single-phase Ag3PO4 compound formed. Hence, adjusting the Ag/Ca ratio in the starting solution allows the production of biomaterials with customized properties. In summary, this study introduces a novel synthesis method for the mono- and biphasic Ca1−xAgxHPO4·nH2O compounds brushite and silver phosphate. The preparation of these phases in a one-pot synthesis with controlled phase composition resulted in the enhancement of existing bone cement formulations by allowing better mixing of the starting ingredients.
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