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Abstract In capacitive deionization (CDI) systems, more Faradaic reactions generally occur at a higher cell voltage, resulting in the poor ion-removal efficiency and high energy consumption, but a low cell voltage may lead to a low deionization capacity. In this study, an integrated strategy, consisting of (1) selecting the acceptable charge/discharge time ratio, (2) finding the potential windows of both positive and negative electrodes, and (3) using the charge-balanced method for determining the optimal mass ratio between the positive and negative electrodes (denoted as (m+)/(m−)), is proposed to find the optimal cell voltage of a CDI system with a high desalination efficiency and low energy consumption. According to this strategy, two newly designed cells using two types of activated carbon (AC) show excellent CDI performances; cell 1 with AC = ACS679, (m+)/(m−) = 1:1.4, and cell voltage = 1.4 V: salt adsorption capacity of 12 mg g−1, charge efficiency of 62%, and energy consumption of 109 kJ mol−1 and cell 2 with AC = ACS25, (m+)/(m−) = 1:1, and cell voltage = 1.2 V: salt adsorption capacity of 13 mg g−1, charge efficiency of 81%, and energy consumption of 72 kJ mol−1 although the potential window of water decomposition for such AC-coated electrodes in 8 mM NaCl is about 2 V. This universal strategy is applicable to all CDI systems utilizing various electrode materials. Graphical abstract Image 1 Highlights • We demonstrate a universal strategy for constructing the AC//AC cell with high CDI performances. • The same charge/discharge time ratio with high reversibility on both electrodes is the key. • Influences of two-electrode mass ratio on the desalination performances are studied. • The pH change is affected by the Faradaic reactions from the potential windows of electrodes. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) is a promising technology for the desalination of brackish water due to its potentially high energy efficiency and its relatively low costs. One of the most challenging issues limiting current CDI cell performance is poor cycling stability. CDI can show highly reproducible salt adsorption capacities (SACs) for hundreds of cycles in oxygen-free electrolyte, but by contrast poor stability when oxygen is present due to a gradual oxidation of the carbon anode. This oxidation leads to increased concentration of oxygen-containing surface functional groups within the micropores of the carbon anode, increasing parasitic co-ion current and decreasing SAC. In this work, activated carbon (AC) was chemically modified with titania to achieve additional catalytic activity for oxygen-reduction reactions on the electrodes, preventing oxygen from participating in carbon oxidation. Using this approach, we show that the SAC can be increased and the cycling stability prolonged in electrochemically highly demanding oxygen-saturated saline media (5 mM NaCl). The electrochemical oxygen reduction reaction (ORR) occurring in our CDI cell was evaluated by the number of electron transfers during charging and discharging. It was found that, depending on the amount of titania, different ORR pathways take place. A loading of 15 mass% titania presents the best CDI performance and also demonstrates a favorable three-electron transfer ORR. [ABSTRACT FROM AUTHOR]

While Electrical Double-Layer Capacitors (EDLC's) have been proven to achieve round-trip efficiencies of over 95%, electrical efficiencies of Capacitive Deionization (CDI) systems are still far from those values. Since this issue seems to be crucial for CDI to commercially compete with other water treatment processes including Reverse Osmosis (RO) it is essential that these efficiencies be improved. In this work, the electrical response of a commercial EDLC's and a CDI system are compared. Results of asymmetric constant current experiments reveal that the main electrical inefficiency occurs during the discharge stage (i.e. in CDI this refers as salt desorption or electrode's regeneration). Here, we propose an operational mode of CDI focused on improving performance of regeneration by simply conducting this stage in a more concentrated solution (3.5M NaC) brine water. The experimental findings suggest that this operational strategy led to 1) an increase from ≈40% to 75% in the round-trip efficiency of CDI, approaching (although admittedly not reaching) those of EDLC's; 2) a drop in ohmic resistance in the discharge cycle of 92% (from 19.77 Ω to 1.45 Ω) consequently increasing the amount of energy that could be potentially recovered from 0.24 J to 0.50 J, and thus, reducing significantly the energy consumption of the process; 3) a wider range of deionization/regeneration current density ratios (0.1–1.25) in which high efficiency values (65–75%) are still maintained. In general, we find that this operational mode might have practical relevance as it implies that CDI systems may be operated with a higher degree of flexibility allowing them to be coupled more readily with renewable energy technologies. Furthermore, the use of a highly concentrated electrolyte (i.e. not deionized water) during regeneration offers an innovative solution for brine concentration. Image 1 • The electrical performance of a CDI flow-cell and an EDLC were compared. • Low round-trip efficiency of CDI cell was mainly associated to discharge step. • New operational mode based on electrolyte replacement was successfully tested. • Round-trip efficiency of CDI can be boosted up to 75%. • Wider range of charge/discharge current density ratios can be used. [ABSTRACT FROM AUTHOR]