The synergistic effect between polyaniline (PANI) and graphene nanosheets significantly enhances the monolithic capacitance and cycling stability, making it an attractive choice for use as an anode material in capacitive deionization (CDI). However, traditional preparation processes are usually complex and time-consuming. Herein, we proposed a simplified solid-phase strategy by using air-plasma technique to fabricate 3D puffy graphene aerogel supported PANI (PANI@PG) nanocomposites within 1 s. In this material, elongated dumbbell-shaped PANI particles with diameters of 30–60 nm were firmly anchored and highly dispersed on graphene sheets, meanwhile, the exfoliated graphene sheets with a large interlayer distance of 0.4 nm were well interconnected. It was demonstrated that as prepared PANI@PG is characteristic of 2–50 nm mesopores, which both ensures a sufficient exposure of PANI active sites to electrolyte and favors the Cl− diffusion-intercalation process. The freestanding PANI@PG electrode exhibited excellent figure-of-merits of the salt adsorption capacity (43.5 mg g−1), charge efficiency (88.6 %), and cycling stability (retention of 77.1 % after 40 cycles). This work paves a new way for constructing 3D conducting polymer/graphene nanocomposites with promising applications in CDI and beyond.
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