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[Display omitted] • The development history of capacitive deionization for defluorination is introduced. • Recent advances of electrode materials have been classified and reviewed. • Defluorination mechanisms have been summarized. • Challenges for engineering applications are presented. • Future perspectives on defluorination by capacitive deionization are provided. The combined need for advanced treatment of fluoridated water and low-energy technologies has inspired researchers to develop more efficient and green methods of fluoride removal. Capacitive deionization (CDI), a novel water treatment technology, has garnered significant attention in the defluorination field due to its exceptional ion selectivity. Recent decades, CDI has achieved remarkable advancements in electrode materials, F− storage mechanisms, and the potential for engineering applications in the realm of F− removal. However, there has been a lack of reviews that highlight design strategies for electrode materials in terms of fluoride ion properties in water and provide insights into key factors for designing CDI structures with excellent performance and promise for scale applications. Herein, starting from the background of fluorine pollution in surface water, and the selective removal of fluorine heavily relies on the crucial role played by electrode materials. Accordingly, all kinds of defluorinated electrode materials are reviewed. Secondly, the defluorination mechanism is summarized especially the distinctions among these processes. Additionally, the challenges existing in the promotion of CDI defluorination to large-scale applications are firstly analyzed in depth. Finally, future research opportunities and prospects by CDI for defluorination are proposed. In summary, CDI shows great potential for removing fluoride ions from water, offering a fresh approach to sustainable water resource management and environmental protection. [ABSTRACT FROM AUTHOR]

[Display omitted] • Scaling up preparation of modified catalysts by direct calcination in air. • Both defects and oxygen-containing groups contribute to performance enhancement. • Electro-Fenton for high pollutant removal kinetics in a wide pH range. • Industrializable case of 30 g catalyst synthesis theoretically for 5.4 m2 electrode. • Lab-scale demonstration for wastewater treatment with capacity of 7.2 L/h. Electro-Fenton (EF) regarded as a green substitution to traditional homogeneous Fenton, produces highly oxidizing OH through in-situ H 2 O 2 electrosynthesis and electrochemical Fe2+ regeneration. One of obstacles that hinders translation of bench-scale EF performance to water treatment practices is the difficulty of scaling up catalyst/electrode preparation in low cost while producing high performance. Here we report scalable preparation of modified carbon catalysts for high-efficiency EF by directly calcinating commercial carbonaceous materials in air. The EF with modified carbon cathode shows high kinetics of 0.296–0.569 min−1 for levofloxacin removal in much wider pH range of 3.0–6.6 using less Fe dosage compared with homogeneous Fenton. This EF system can reduce chemical oxygen demand (COD) of coking wastewater from 312.0 to 99.5 mg L−1 to satisfy wastewater discharge standard in China while consuming low electricity of 1.8–4.9 kWh kg−1 COD−1. We demonstrated the scalability of this EF process by scaling up preparative throughput of catalyst (30 g that can be processed into electrodes with total working areas of 54000 cm2), enlarging electrode size (230 cm−2) and reactor volume with wastewater treatment capacity of 7.2 L/h. This scalability demonstration of EF technology shows the promising potential of achieving low-cost advanced wastewater treatment. [ABSTRACT FROM AUTHOR]

[Display omitted] • The preparation process of the CDI electrode is simplified. • Laser-induced graphene (LIG) can be directly used as a CDI electrode. • LIG electrode is modified by one-step electrodeposition of Co 4 S 3. • The LIG6/Co 4 S 3 -15 presents a high adsorption capacity of 2702.79 mg g−1. • UO 2 2+ adsorption is attributed to the synergistic action of EDLs and pseudocapacitance. It has been proved that capacitive deionization (CDI) technology possesses a significant potential for uranium capture. However, the CDI performance has been limited by the complex preparation process of the electrodes and the poor adhesion between electrode materials and collectors. Here we combine the laser-induced graphene (LIG) and the electrodeposition to develop the LIG/cobalt sulfide (LIG/Co 4 S 3) electrodes with good adsorption performance. The obtained LIG6/Co 4 S 3 -15 electrode has both electrical double layers (EDLs) and pseudocapacitance properties, with a specific capacitance of 24.27 F g−1, which is 1.82 times higher than that of LIG6 (13.36 F g−1). The LIG6/Co 4 S 3 -15 electrode exhibited a high adsorption capacity of 2702.79 mg g−1. The advantages of this electrode preparation method are mainly attributed to the synergistic effect of the following aspects: (i) simplified graphene preparation by avoiding wet chemistry and post-treatment steps; (ii) simplified tedious electrode preparation such as electrode slurry distribution and sheet coating; (iii) the three-dimensional structure of LIG provides not only the conductive network but also the site for Co 4 S 3 nanosheet growth, thus avoiding nanosheet aggregation. The abundant pore structure of the conductive graphene substrate and the layered structure of the Co 4 S 3 nanosheets enable the LIG6/Co 4 S 3 -15 electrode with fast charge/ion transport, high hydrophilicity and superior pseudocapacitance, allowing uranyl (UO 2 2+) to be firstly electrosorbed, then physicochemically adsorbed, and finally electrocatalytically reduced/deposited onto the electrode. This study will offer a simple and environmentally friendly method for the synthesis of electrodes and provide a reference for the design of efficient electroadsorption materials. [ABSTRACT FROM AUTHOR]

A self-supported MoS 2 /CoS 2 @TiO 2 nanotube (TNT) hybrid electrode was fabricated by an in-situ hydrothermal process-assisted growth strategy, which achieved a significantly high gravimetric Na+ adsorption capacity and excellent regeneration performance. It also demonstrated amazing removal efficiencies close to 90% for various heavy metal ions (i.e., Fe3+, Cr3+, Cd2+, Pb2+, Cu2+ and Ni2+), revealing its great potential for wastewater purification. [Display omitted] • A self-supported MoS 2 /CoS 2 @TNT hybrid electrode was constructed. • The electrode achieved a gravimetric Na+ adsorption capacity of 44.22 mg g−1. • The electrode exhibited excellent regeneration performance and removal rates. • The electrode also realized removal efficiencies up to 90% for heavy metal ions. Recently, the rational design and construction of graphene-like layered transition-metal disulfides (TMDs) with chemical and physical superiorities to act as capacitive desalination (CDI) electrodes for water purification have attracted increasing interest worldwide. Herein, an advanced self-supported MoS 2 /CoS 2 @TiO 2 nanotube (TNT) hybrid electrode was grown on a TNT scaffold by a hydrothermal process-assisted in-situ growth strategy, and an asymmetric CDI cell was constructed with the as-fabricated MoS 2 /CoS 2 @TNT and commercial AC electrodes as cathode and anode, respectively. Benefiting from the effective structural feature (i.e., fully open nanosheet-assembled flowers and hierarchical pore alignment) and synergy effect of metal-like CoS 2 , state-of-the-art MoS 2 and TNTs with an efficient charge "superhighway", the MoS 2 /CoS 2 @TNT electrode achieved a significantly high gravimetric Na+ adsorption capacity of 44.22 mg g−1 in a 600 mg L−1 NaCl solution at 1.2 V. Moreover, the hybrid electrode possessed excellent regeneration performance with a capacity retention of nearly 100% even after 20 cycles. Most notably, such electrode also demonstrated amazing removal efficiencies close to 90% for various heavy metal ions (i.e., Fe3+, Cr3+, Cd2+, Pb2+, Cu2+ and Ni2+), revealing its great potential for wastewater purification. [ABSTRACT FROM AUTHOR]

• Floriform WO 3 /C electrode were developed for electrosorption of U(VI) from water. • The charge/discharge process of WO 3 /C primarily belongs to capacitive controlled behavior. • WO 3 /C electrodes achieve a maximum U(VI) electrosorption capacity of 449.9 mg g−1 at 1.2 V. • Electrosorption of U(VI) is credited to synergistic effect of EDLs and pseudocapacitance from WO 3 /C. Decontamination and recovery of uranium(VI) [U(VI)] from radioactive wastewater is vital to sustainable nuclear power production and reclamation of radioactive waste. As a promising technology of water treatment, capacitive deionization for adsorption of U(VI) started to attract attention. Herein, for the first time, a floriform WO 3 /C composite was developed as a pseudocapacitive electrode material for electrosorption of U(VI) from water. The as-prepared WO 3 /C composite was constructed from dozens of 2D nanosheets with a thin amorphous carbon layer, resulting in uniform flower-like particles with hierarchical nanostructure and superior open pore network. The charge/discharge process of WO 3 /C was demonstrated as prominent capacitive controlled behavior by quantization of capacitance contributions. As a result, the WO 3 /C electrodes achieved a maximum U(VI) electrosorption capacity of 449.9 mg g−1 at 1.2 V and good cycling stability after consecutive adsorption-desorption, which is superior to the conventional physical adsorption processes. The superior CDI performance of the WO 3 /C electrode is credited to the synergistic effect of EDLs and pseudocapacitance based on the combination of WO 3 and carbon layer with hierarchical nanostructure. Overall, the facile preparation strategy, the superior electrosorption performances, and the high cycling stability, endow the floriform WO 3 /C electrodes to be a promising electrode material for electrosorption of U(VI) from wastewater. [ABSTRACT FROM AUTHOR]