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Flow electrode capacitive deionization (FCDI) has great advantages in high salinity wastewater desalination. However, due to the limited adsorption capacity of electrode material, membrane concentration polarization would form and increase energy consumption, and affect the continuity of desalination. In this work, milling technology was used to modify original activated carbon (AC), the obtained ball milled activated carbon (BAC) was used as FCDI electrode material. The milling process modified multiple physical and electrochemical characteristics of original AC. The highest average salt removal rate (ASRR) of BAC was 2.2 times of that of AC, which was attributed to the modified surface properties including more oxygenated functional group, larger electrostatic gravitation characteristics and better hydrophilicity. The reduced concentration polarization during the desalination was responsible for the increased adsorption capacity, which was due to larger electrolyte contact area, enhanced ions capacity by more suitable pore structures, and 5 times higher energy normalized removal salt (ENRS) of BAC flow electrode than that of AC. Because of its simple operation and remarkable modification effect, ball milling technology shows great potential in large scale modification of electrode materials. [ABSTRACT FROM AUTHOR]

• 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]