Electrosorption, Desorption, and Oxidation of Perfluoroalkyl Carboxylic Acids (PFCAs) via MXene-Based Electrocatalytic Membranes.

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MXenes exhibit excellent conductivity, tunable surface chemistry, and high surface area. Particularly, the surface reactivity of MXenes strongly depends on surface exposed atoms or terminated groups. This study examines three types of MXenes with oxygen, fluorine, and chlorine as respective terminal atoms and evaluates their electrosorption, desorption, and oxidative properties. Two perfluorocarboxylic acids (PFCAs), perfluorobutanoic acid (PFBA) and perfluorooctanoic acid (PFOA) are used as model persistent micropollutants for the tests. The experimental results reveal that O-terminated MXene achieves a significantly higher adsorption capacity of 215.9 mg·g-1 and an oxidation rate constant of 3.9 × 10-2 min-1 for PFOA compared to those with F and Cl terminations. Electrochemical oxidation of the two PFCAs (1 ppm) with an applied potential of +6 V in a 0.1 M Na2SO4 solution yields >99% removal in 3 h. Moreover, PFOA degrades about 20% faster than PFBA on O-terminated MXene. The density functional theory (DFT) calculations reveal that the O-terminated MXene surface yielded the highest PFOA and PFBA adsorption energy and the most favorable degradation pathway, suggesting the high potential of MXenes as highly reactive and adsorptive electrocatalysts for environmental remediation.