Engineering dynamic heterogeneous–homogeneous hybrid interfaces for solar-driven in situ water remediation

For in situ remediation of surface waters, where contaminant sources and distributions are highly heterogeneous, developing an approach that combines broad-spectrum oxidative capacity with selective removal of trace yet high-risk pollutants remains a central challenge. Here we report a light-responsive Cu-anchoring strategy on a UiO-66-NH₂ metal–organic framework that establishes a dynamic heterogeneous–homogeneous photocatalytic platform. Upon illumination, photolabile Cu sites release mobile Cu⁺ species that function as long-lived reductive mediators, dramatically promoting multi-electron O₂ activation and boosting •OH generation by nearly two orders of magnitude. The regenerated Cu²⁺ concurrently imparts molecular selectivity, enabling efficient antibiotic degradation and robust disinfection even in organic-rich natural waters. Embedding this catalyst into a buoyant membrane further enhances deployment flexibility and environmental adaptability. In an amplified 28-day outdoor evaluation treating real lake water, the membrane achieved high contaminant degradation efficiency while sustainably suppressing microbial and pollutant rebound, underscoring its long-term operational robustness in natural aquatic systems.