original data

Exploring highly active and cost-efficient electrocatalysts with in-situ regeneration of coordination sites is crucial for the large-scale application of electro-assisted uranium extraction technology, which can effectively solve the problem of limited coordination sites for traditional catalysts. Herein, we tailor the charge distribution of La(CrFeCoNiCu)O3 via high-entropy effect to induce in-situ surface hydroxylation, thereby enabling robust uranium recovery from fluoride-containing uranium wastewater. The as-prepared La(CrFeCoNiCu)O3 exhibits exceptional uranium removal performance, achieving a 97.8% removal rate in fluoride-containing uranium wastewater and still maintaining over 91.3% efficiency with real uranium wastewater. Relying on in-situ ATR-SEIRAS and quasi-in-situ XPS, we confirm that Cu sites serve as hydroxylation active sites, enabling precise capture of fluoro-uranium complexes, followed by uranium mineralization via electron reduction-free radical reoxidation pathway. In addition, large-scale application verification of real nuclear wastewater is conducted on the self-designed flow electrolysis device, confirming its cost advantage.