Double-Layered Silica-Engineered Fluorescent Nanodiamonds for Catalytic Generation and Quantum Sensing of Active Radicals

Abstract: Fluorescent nanodiamonds (FNDs) hosting nitrogen-vacancy (NV) centers have attracted considerable attention for quantum sensing applications, particularly owing to notable advancements achieved in the field of weak magnetic signal detection in recent years. Here, we report a practical quantum-sensing platform for the controlled production and real-time monitoring of ultra-short-lived reactive free radicals using a double-layered silica modification strategy. An inner dense silica layer preserves the intrinsic properties of NV centers, while an outer porous silica layer facilitates efficient adsorption and stabilization of hydroxyl radicals and their precursor reactants. By doping this mesoporous shell with gadolinium (III) catalysts, we achieve sustained, light-free generation of hydroxyl radicals via catalytic water splitting, eliminating reliance on external precursors. The mechanism underlying this efficient radical generation is discussed in detail. The radical production is monitored in real time and in situ through spin-dependent T1 relaxometry of the NV centers, demonstrating stable and tunable radical fluxes, with concentration tunable across a continuous range from approximately 100 mM to molar levels by adjusting the catalyst condition. This study extends the technical application of nanodiamonds from relaxation sensing to the controlled synthesis of reactive free radicals, thereby providing robust experimental evidence to support the advancement of quantum sensing systems in intelligent manufacturing.