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Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO2in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO2to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO2. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO2capture of ∼2.3 mmol g–1. This is on par with the best solution-phase amine chemical capture technologies available today.

The current study reports the application of chalcopyrite semiconductor CuInS2(CIS) nanofibers for the reduction of CO2to CO with a remarkable Faradaic efficiency of 77 ± 4%. Initially the synthesis of CuInS2nanofibers was carried out by adaptable electrospinning technique. To reduce the imperfection in the crystalline fiber, polyacrylonitrile (PAN) was selected as template polymer. Afterward, the desired chemical structure of nanofibers was achieved through sulfurization process. Making continuous CuInS2nanofibers on the cathode surface by the electrospinning method brings the advantages of being economical, environmentally safe, and versatile. The obtained nanofibers of well investigated size and diameter according to the SEM (scanning electron microscope) were used in electrochemical studies. An improvement of Faradaic efficiency was achieved with the catalytic active CuInS2in nanofibrous structure as compared to the solution processed CuInS2. This underlines the important effect of the electrode fabrication on the catalytic performance. Being less contaminated as compared to solution processing, and having a well-defined composition and increased catalytically active area, the CuInS2nanofiber electrodes prepared by the electrospinning technique show a 4 times higher Faradaic efficiency. Furthermore, in this study, attention was paid to the stability of the CuInS2nanofiber electrodes. The electrochemical reduction of CO2to CO by using CIS nanofibers coated onto FTO electrodes was carried out for 10 h in total. The observed current density of 0.22 mA cm–2and the stability of CIS nanofiber electrodes are found to be competitive with other heterogeneous electrocatalysts. Hence, we believe that the fabrication and application of nanofibrous materials through the electrospinning technique might be of interest for electrocatalytic studies in CO2reduction.