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The ubiquitous presence of perfluoroalkyl acids (PFAAs) in the environment remains a serious environmental concern. In this study, the electrochemical oxidation (EO) of PFAAs from the waste of ion exchange (IX) still bottoms was assessed at the laboratory and semi-pilot scales, using full boron-doped diamond (BDD) electrochemical cells. Multiple current densities were evaluated at the laboratory scale and the optimum current density was used at the semi-pilot scale. The results at the laboratory scale showed >99% removal of total PFAAs with 50 mA/cm² after 8 h of treatment. PFAAs treatment at the semi-pilot scale showed 0.8-fold slower pseudo-first-order degradation kinetics for total PFAAs removal compared to at the laboratory scale, and allowed for >94% PFAAs removal. Defluorination values, perchlorate (ClO₄⁻) generation, coulombic efficiency (CE), and energy consumption were also assessed for both scales. Overall, the results of this study highlight the benefits of a tandem concentration/destruction (IX/EO) treatment approach and implications for the scalability of EO to treat high concentrations of PFAAs.