Pitch-based porous carbon via the solid–liquid synergistic oxidation of K₂FeO₄ for excellent electrocapacitive desalination

To address limited desalination capacity and insufficient charge efficiency for carbon materials in capacitive deionization (CDI), a solid–liquid synergistic oxidation strategy of potassium pertechnetate (VI) for pitch was proposed to construct porous carbon with a reasonable pore structure and high reactive surface. On the one hand, K₂FeO₄ is first utilized for the solid-phase oxidation (SPO) of pitch by a high-energy ball mill, introducing rich oxygen-containing groups such as ether bonds. Meanwhile, dehydro-condensation reactions occurred during SPO, resulting in the formation of the oxidized pitch with a high degree of condensation. Importantly, the pyrolysis yield of the oxidized pitch is as high as 46.9 % at 800 °C, almost twice that of the pristine pitch, meaning that the oxidized pitch with high polymer degree and rich C-O bridge bonds facilitates the carbon fixation and emission reduction during carbonization. On the other hand, the self-oxidation of K₂FeO₄ in aqueous solution forms bifunctional activators (KOH and Fe(OH)₃) for the preparation of pitch-based porous carbon. Benefiting from the crosslinking structure of oxidized pitch and the multi-effective activation, the prepared porous carbon (H-CBPF) exhibits a robust layered stacking topology with a high surface area and oxygen content. Thereby, it can deliver an excellent salt adsorption capacity (SAC) of 22.1 mg g⁻¹ with an average desalination rate of 1.89 mg g⁻¹ min⁻¹ and a high charge efficiency of 85 % at 1.2 V in 500 mg L^-1 NaCl solution. This work opens up a green and economical route for the preparation of pitch-derived porous carbon for high-performance CDI.