Bridging Uranium Uptake and PET Plastics Degradation Within an All‐Inorganic Polyoxoniobate Framework

Abstract The escalating crisis of polyethylene terephthalate (PET) plastic waste is constrained by the high energy consumption and high cost of recycling methods. Here, we propose a “one stone, two birds” strategy based on an all‐inorganic polyoxoniobate (PONb) framework, which not only serves as an adsorbent for selectively capturing trace uranyl ions from uranium‐containing wastewater with high removal rate of ∼98.5%, but also, when uranyl ions are anchored within the framework, acts as a photocatalyst capable of efficiently oxidizing and degrading PET plastic waste with 92.3% isolated yield of value‐added terephthalic acid (TPA). Notably, trace uranium uptake achieves extremely high catalytic activity, with a maximum turnover frequency (TOF) value exceeding that of homogeneous uranyl nitrate by 160 times, while maintaining yield over multiple cycles. The efficient catalytic activity stems from the coupling of hydrogen atom transfer (HAT) and single electron transfer (SET) processes involving highly oxidizing excited‐state uranyl. This work provides a low‐energy and low‐cost method that simultaneously addresses the dual pollution challenges of uranium‐containing wastewater and PET plastic waste, recovers uranium resources, and obtains value‐added chemicals, demonstrating potential to play a key role in advancing circular economy and sustainable development.