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

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 (MoO_x). 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 MoO_x 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.