Catechol-Isolated Atomically Dispersed Nanocatalysts for Self-Motivated Cocatalytic Tumor Therapy

Nanocatalytic tumor therapy based on Fenton nanocatalysts has attracted considerable attention because of its therapeutic specificity, enhanced outcomes, and high biocompatibility. Nevertheless, the rate-determining step in Fenton chemistry, which involves the transition of a high-valence metallic center (FeIII) to a Fenton-active low-valence metallic center (FeII), has hindered advances in nanocatalyst-based therapeutics. In this study, we constructed mesoporous single iron atomic nanocatalysts (mSAFe NCs) by employing catechols from dopamine to coordinate and isolate single iron atoms. The catechols also serve as reductive ligands, generating a field-effect-based cocatalytic system that instantly reduces FeIII species to FeII species within the mSAFe NCs. This self-motivated cocatalytic strategy enabled by mSAFe NCs accelerates the kinetics of the Fenton catalytic reaction, resulting in remarkable performance for nanocatalytic tumor therapy both in vitro and in vivo. Catechol-isolated mesoporous single iron atomic nanocatalysts (mSAFe NCs) with ligand-field-effect-promoted cocatalytic Fenton catalysis have been constructed. The catechols from dopamine serve as both an iron coordination site for atomic isolation and a reductive ligand to generate a field-effect-based cocatalytic system that instantly reduces FeIII species to FeII species within the mSAFe NCs, thereby promoting in vivo Fenton catalytic effects against tumors.+image