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Novel silver compounds in higher oxidation states, Ag (II) and Ag (III), have emerged as desirable alternatives to existing forms of antimicrobial silver compounds. Offering enhanced efficacy without sacrificing biocompatibility. Unique physiochemical characteristics associated with higher oxidation state silver confer desirable therapeutic traits. However, these same characteristics create challenges in terms of long-term stability and chemical compatibility with conventional biomedical materials. Core-shell methodologies, utilizing silica as a mesoporous or amorphous shell, have been adopted to enhance the stability of reactive active ingredients or cores. These methodologies commonly utilize controlled condensation of silicic acids in non-aqueous media by way of hydrolyzing alkyl silicates: the Stöber process or modified processes thereof. However, these strategies are not conducive to cores of higher oxidation state silver wherein hydroxyl organic precursors and by-products are incompatible with strong oxidizing agents. Addressing these challenges, we present a strategy herein for the preparation of a self-directed silver oxynitrate-silica, Ag₇NO₁₁:SiO₂, framework. The method described utilizes pH gradients generated from the oxidation reaction of soluble silver, Ag (I), with a strong oxidizing agent/alkaline silicate media to facilitate spatial control over the protonation and subsequent condensation of silicic acid from aqueous solution. The resulting Ag₇NO₁₁:SiO₂ framework confers enhanced long term and thermal stability to silver oxynitrate without impairing aqueous degradation profiles or subsequent antimicrobial and antibiofilm activities. Full article