Abstract
Activating ground-state molecular oxygen (O(2)) without added oxidants or external energy is a central challenge in aerobic catalysis because triplet O(2) imposes spin and electron-transfer constraints. Herein, we report a high-rate, energy-neutral O(2) activation platform that converts ambient air O(2) directly to singlet oxygen ((1)O(2)) under room-temperature, bias-free conditions. By engineering atomically adjacent Co-Mo dual sites, Co-Mo d-d coupling and electron delocalization create a short-range electron transfer pathway that strengthens O(2) adsorption, weaken the O-O bond via π* orbital population, and limit solvent-induced dissipation, thereby favoring selective (1)O(2) formation. These features enable the catalyst (1)O(2) productivity and pollutant degradation rates up to three orders of magnitude higher than previously reported air-fed O(2) heterogeneous catalysts and comparable to oxidant-driven processes, yet without chemical inputs or energy bias. The catalyst is robust and versatile across diverse applications, including the degradation of organic contaminants, transformation of inorganic ions and antibacterial applications. This work establishes a new approach for sustainable O(2) activation, pointing toward next-generation energy-neutral catalytic technologies.