Selective and autonomous generation of singlet oxygen for synergistic heavy metal-organic removal without energy input

A fundamental challenge across environmental catalysis is the reliance on external energy or chemical inputs to drive detoxification reactions. Here, we transcend this limitation with a pollutant-driven framework, demonstrated by a variable-valent molybdenum oxide (MoOx). A vacancy-anchored dual-site polarization mechanism enables the selective conversion of adsorbed oxygen into singlet oxygen (1O2), bypassing radical intermediates, driven by the synergistic interaction between low-valent Mo and high-valent metal ions. This process achieves simultaneous heavy-metal reduction and organic degradation without the addition of molecular oxygen (O2) gas, external energy (e.g., light, electricity, or heat), or chemical oxidants (e.g., persulfate or peroxide). The MoOx material maintains robust performance in complex water and retains over 99% removal efficiency after closed-loop regeneration. This work establishes a general design principle for energy-autonomous catalysis, bridging environmental remediation with sustainable chemistry and suggesting a potential pathway for self-sustaining processes in wastewater and beyond. A variable-valent molybdenum oxide generates singlet oxygen from ambient oxygen without energy, oxidants, or added O2, enabling synergistic removal of heavy metal ions and organics, bypassing radicals and offering a facile remediation route.