Nonporous Metal–Organic Framework Enables Record‑High Uranium Extraction and Complete Diglyme Degradation

ABSTRACT Nuclear energy accommodates rising energy demand of artificial intelligence yet poses environmental risks, making uranium extraction from wastewater important. We herein report a nonporous metal–organic framework CuTTB‐3 as cathode in an H‐type electrolytic cell (two compartments separated by an anion‐exchange membrane) for uranium extraction. Unlike single‐chamber cell limited by diglyme‐induced redissolution of uranium deposits, CuTTB‐3‐based H‐type configuration facilitates 99.8% uranium extraction within 1 h and complete diglyme degradation. This system overcomes concentration limits of 100 g L −1 diglyme and 100 mg L −1 uranyl in conventional setups. It retains >96.4% extraction efficiency over 15 cycles, achieving a cumulative U(VI) extraction amount of 28855 mg g −1 within 10 h and an extraction rate of 2886 mg g −1 h −1 , both record‐high values among reported materials. A flow‐cell setup treated 1 L simulated wastewater, delivering 96.8% extraction efficiency and cumulative capacity of 19360 mg g −1 . Comparisons with porous analogue CuTTB‐4 confirm structural robustness and interfacial charge transfer kinetics dominate electrochemical uranium extraction. Different from traditional adsorption‐based uranium extraction materials that rely heavily on porostiy, this work realizes efficient uranium extraction via an electrochemical deposition route based on a nonporous MOF, which expands the application scenario of nonporous materials in radioactive wastewater treatment.