Porous 3D-graphene functionalized with MnO2 nanospheres and NiO nanoparticles as highly efficient electrodes for asymmetric capacitive deionization: Evaluation by impedance-derived capacitance spectroscopy

Abstract

Capacitive deionization (CDI) is a novel desalination technology for brackish water purification. Here, we report the rational design of an efficient asymmetric CDI system considering several steps. First, three-dimensional graphene nanostructures (3DG) were synthesized using the hydrothermal method, followed by the freeze-drying process, and then drop casting onto the carbon fiber paper (CFP) substrate. Second, a facile and controllable electrodeposition technique was used for the in-situ synthesis of MnO2 nanospheres and NiO nanoparticles onto the CFP/3DG surface to prepare CFP/3DG/MnO2 cathode and CFP/3DG/NiO anode. Third, the prepared nanocomposite electrodes were used to fabricate an asymmetric CDI cell. Here, MnO2 (pI = 4.5) and NiO (pI = 10) nanostructures provide opposite surface charges due to their dissimilar isoelectric points, enhancing cations and anions electrosorption. The surface morphology, chemical and electrochemical characteristics, as well as the capacitive performance of the fabricated CFP/3DG/MnO2 and CFP/3DG/NiO electrodes, were investigated using SEM, EDX, XRD, FTIR, TGA, BET/BJH, and electrochemical techniques. Besides, impedance-derived capacitive analysis was used to evaluate the ions retention time on the fabricated electrodes. Finally, the fabricated CFP/3DG/NiO||CFP/3DG/MnO2 asymmetric CDI cell was used in water desalination with high reversibility, good regeneration rate, and high electrosorption capacity (21.01 mg g−1) for the initial salt concentration of 1000 mg L−1 in 1.2 V. These results suggest that the proposed asymmetric CDI system is a promising candidate for the efficient capacitive desalination process.