Electron‐Donating Aminosilane Bridging Enables General Access to Full‐Color Aqueous Phosphorescent Nanospheres

ABSTRACT The pursuit of a universal and efficient strategy for converting organic molecules into aqueous‐phase phosphorescent nanoparticles (PNPs) exhibiting prolonged afterglow and uniform morphology represents a persistent challenge in materials chemistry. In this study, we report a general in situ silanization platform that enables the integration of organic precursors into silica‐based matrices via an aminosilane‐mediated “bridge”, yielding monodisperse, size‐tunable (10∼320 nm) full‐color PNPs with emission spanning blue‐purple to red. Aminosilanes with electron‐donating characteristics not only promote an intramolecular charge transfer (ICT) state to enhance intersystem crossing (ISC) efficiency but also facilitate the encapsulation of silanized anhydride within silica frameworks (ASLs@SiO 2 ), effectively shielding the emitters from aqueous and oxygen quenching. Orthogonal screening across 14 anhydrides and 12 aminosilanes validated the strategy's universality, achieving full‐color afterglow with a maximum lifetime of 1128.07 ms and a quantum yield of 24.04%. Furthermore, to precisely control dispersion and size, two distinct ASLs@SiO 2 architectures were engineered: one embedding silanized anhydride within a concentric silica interlayer, and another infusing it into dendritic porous silica spheres. This scalable, low‐cost synthesis (∼$1 per 150 g) underscores the commercial viability of the approach and establishes a new approach for designing high‐performance aqueous‐phase PNPs.