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Triggering the interaction of nanomaterials with molecules by means of electrical potentials in aqueous media remains challenging, especially if 3D through-flow systems are used as electrodes, as in potential-controlled liquid chromatography (PCC). In this paper, multi-walled carbon nanotubes (MWCNTs) function as a particulate packed bed electrode in order to study the system’s response to various applied potentials and electrolyte compositions. The process principle was analyzed using chronoamperometry and cyclic voltammetry. Applying an electrical potential to the hydrophilic MWCNTs induces the presence of both capacitive and faradaic currents. This leads, over time, to a degradation of the electrode due to structural changes of the MWCNT matrix and an increase in redox reactions on the surface. The role of the electrochemical double layer (EDL) is highlighted as a main player in the process, directly influencing the adsorption capability of the electrode. The EDL rearrangement time and coverage radius depend on the composition of the mobile phase and on the potential applied. The capacity of the electrode for the target (maleic acid) increases at high positive potentials (+800 mV vs. Ag/AgCl), while the presence of electrolytes leads to a capacity decrease. Our research enhances the understanding of capacitive through-flow cells.

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The design of 3D monoliths provides a promising opportunity to scale the unique properties of singular carbon nanotubes to a macroscopic level. However, the synthesis of carbon nanotube monoliths is often characterized by complex procedures and additives impairing the later macroscopic properties. Here, we present a simple and efficient synthesis protocol leading to the formation of free-standing, stable, and highly conductive 3D carbon nanotube monoliths for later application in potential-controlled adsorption in aqueous systems. We synthesized monoliths displaying high tensile strength, excellent conductivity (up to 140 S m−1), and a large specific surface area (up to 177 m2 g−1). The resulting monoliths were studied as novel electrode materials for the reversible electrosorption of maleic acid. The process principle was investigated using chronoamperometry and cyclic voltammetry in a two-electrode setup. A stable electrochemical behavior was observed, and the synthesized monoliths displayed capacitive and faradaic current responses. At moderate applied overpotentials (± 500 mV vs. open circuit potential), the monolithic electrodes showed a high loading capacity (~20 µmol g−1) and reversible potential-triggered release of the analyte. Our results demonstrate that carbon nanotube monoliths can be used as novel electrode material to control the adsorption of small organic molecules onto charged surfaces.

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