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• The first high entropy oxides based multifunctional electrode material is synthesized by simple grinding technique. • Nano-sized (< 10 nm) high entropy oxides are incorporated in surface functionalized biowaste derived activated carbon. • High salt adsorption capacity of 241 mg g−1 and cycle repeatability upto 20 cycles is demonstrated. • The excellent desalination capacity is attributed to the combined electric-double layer and pseudocapacitive mechanism. Nano-sized high entropy oxides (particle size < 10 nm) are expected to possess enhanced stability, electrochemical properties and increased potential in versatile applications than bulk metal oxides. In this study, nano-sized high entropy oxides incorporated surface functionalized coconut shell derived activated carbon (HEO/f-CSAC) is synthesized, characterised and used as an advanced multifunctional material for electrochemical energy storage and desalination. Attributed to its unique microstructure and extraordinary properties, HEO/f-CSAC shows an excellent salt adsorption capacity of 241 mg g−1 at 1.2 V in 500 mg L−1 concentration of NaCl solution, which is very high as compared to previous reports. The reason behind high salt adsorption capacity is its outstanding specific capacitance of 147.5 F g−1 at current density 1 A g−1. Moreover, the assembled lab-scale CDI unit demonstrates extremely good performance upto 20 adsorption-desorption cycles due to the long cycle life with good capacitance retention of fabricated HEO/f-CSAC based two-electrode supercapacitor. Additionally, a red light-emitting diode illumination by connecting three supercapacitors in series, indicates the high efficiency and potential of HEO/f-CSAC for real life energy-related application. These results prove that HEO/f-CSAC can be implemented for water desalination with enhanced supercapacitive performance manifesting its multifunctionality for energy and environmental applications. [Display omitted] [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) is an emerging technology as a sustainable low energy process for desalination of brackish water. Activated carbon electrodes are often used in the CDI devices. Electrosorption capacity was found to be improved on asymmetric electrode configuration using activated carbon cloth doped with fluorine due to redistribution of electric potential. This led to improvement in desalination performance up to 12.4 mg/g for a desalination cycle of 6 min employing an asymmetric fluorinated electrode as cathode (ACC//F-ACC). A relatively high charge efficiency of 77 % was obtained representing 92 % charge efficiency neglecting the leakage currents. Furthermore, the ion adsorption rate was found to improve substantially due to an increased surface conductivity of the fluorinated electrode confirmed by Mott-Schottky analysis. Energy consumption during desalination of 1000 ppm sodium chloride solution of 0.71kWh/m3 for symmetric electrode configuration was found to reduce by 36 % upon employing asymmetric configuration. This study shows some of the benefits of asymmetric configuration to achieve an optimal operation of CDI device, as well as improvements related to energy consumption. Image, graphical abstract [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]