Hollow Conductive Polymer Nanospheres with Metal–Polyphenol Interfaces for Tunable Hydrogen Peroxide Activation and Energy Conversion

Hydrogen peroxide (H2O2) is a key oxidant for green chemical processes, yet its catalytic utilization and activation efficiency remain limited by material instability and uncontrolled radical release. Here, we report a dual-functional, hollow conductive polymer nanostructure that enables selective modulation of H2O2reactivity through interfacial physicochemical design. Hollow polypyrrole nanospheres functionalized with carboxyl groups (PPy@PyCOOH) were synthesized via a one-step Fe2+/H2O2oxidative copolymerization route, in which H2O2simultaneously served as oxidant, template, and reactant. The resulting structure exhibits enhanced hydrophilicity, rapid redox degradability (>80% optical loss in 60 min (82.5 ± 4.1%, 95% CI: 82.5 ± 10.2%), 10 mM H2O2, pH 6.5), and strong electronic coupling to reactive oxygen intermediates. Subsequent tannic acid–copper (TA–Cu) coordination produced a conformal metal–polyphenol network that introduces a controllable Fenton-like catalytic interface, achieving a 50% increase in ROS yield (1.52 ± 0.08-fold vs. control, 95% CI: 1.52 ± 0.20-fold) while maintaining stable photothermal conversion under repeated NIR cycles. Mechanistic analysis reveals that interfacial TA–Cu complexes regulate charge delocalization and proton–electron transfer at the polymer–solution boundary, balancing redox catalysis with energy dissipation. This work establishes a sustainable platform for H2O2-driven redox and photo-thermal coupling, integrating conductive polymer chemistry with eco-friendly catalytic pathways.