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[Display omitted] • A parametric investigation of the electrochemical desalination cell was carried out. • The longer residence time of the flow electrode and the feed water augmented the desalination. • Surface area of carbon and redox couple play a crucial role in desalination. • A reduction of 235 mg/L of total dissolved solids in tap water was observed. Flow Electrode Capacitive Deionization (FCDI) is a promising technology that uses carbon materials as flow electrodes in aqueous conditions to enable continuous desalination. In this work, the parametric investigation of the FCDI cell was carried out for low and high surface area activated carbon. When 1 mM/1 mM ferri-/ferrocyanide redox couple in the 1 M NaCl supporting electrolyte containing the 5 wt% high surface area activated carbon and 0.5 wt% MWCNT is circulated as flow electrode at the flow rate of 8 mL/min in the electrode chamber and 0.1 mM NaCl feed water is circulated in single-pass mode at 8 mL/min, the FCDI system achieved a significant improvement in desalination performance up to 76.38 % of SRE, with a high average salt removal rate of 43.925 µg/cm2s @ 2 V, charge efficiency of 20.11 % and average energy consumption of 0.27 kWh/mol, through a thorough parametric investigation. When the FCDI cell was tested with tap water, the average salt removal rate, average energy consumption, and salt removal efficiency were calculated at 6.11 μg/cm2s, 2.46 kWh/mol, and 46.61 % respectively, resulting in the reduction of total dissolved solids of 600 mg/L at the inlet to 365 mg/L at the outlet. The combination of microporous high surface area carbon and ferro-ferri redox couple propelled the desalination performance in comparison with the macroporous low surface area carbon, maximizing the ion removal rate, which further reduced the energy consumption and operating voltage for the process. [ABSTRACT FROM AUTHOR]

[Display omitted] • State of the art in electrosorption of organic compounds (EOC) critically reviewed. • EOC shows promise against poorly adsorbable, highly polar, and ionized pollutants. • Enhanced adsorption and active control of ad-/desorption by electric potential. • Insightful performance parameters proposed to unify rapidly growing EOC research. • EOC application for on-site regenerable adsorbers and in treatment trains discussed. The widespread contamination of water resources with emerging organic contaminants necessitates the development of sustainable and cost-effective water treatment technologies. Adsorption, as a widely used water remediation process, is hampered by severe performance limitations against ionic and hydrophilic organic contaminants. In addition, no facile on-site regeneration techniques are available. Electrosorption of organic compounds (EOC) is a promising alternative to not only improve adsorption performance, but also to facilitate adsorbent regeneration by green electricity. The number of studies on EOC has grown exponentially over the past decades. There are numerous examples showing that applied electric potentials can significantly enhance the adsorption affinity, capacity, and kinetics of conductive carbon adsorbents. However, whether these effects are specific to certain compound classes or more generally applicable remains unclear as well as the optimal criteria for designing EOC processes. Therefore, we critically evaluated the current state of the art of EOC in terms of active control of adsorption and desorption processes and the achievable effects for ionic and neutral organic compounds. Through a detailed consideration of compound speciation and surface chemistry of electrode materials, we derive mechanistic insights into the EOC process and discuss differences between electrosorption of inorganic and organic compounds. We provide definitions and propose insightful performance parameters to unify the rapidly growing EOC research. Potential application scenarios and future research directions are discussed. Overall, EOC is less likely to be a one-fits-all solution for removing contaminants, but adds a valuable tool especially for the hydrophilic and ionic organic contaminants that challenge conventional adsorption processes. [ABSTRACT FROM AUTHOR]

Asymmetrical capacitive deionization (A-CDI) is expected to be a promising desalination technique with high salt removal capacity. In this work, the novel A-CDI are proposed where the negative and positive electrode are Na 4 Ti 9 O 20 (NTO) and activated carbon (AC), respectively. Basically, the NTO nanotubes with the specific surface area of 142.43 m 2 /g have been prepared by hydrothermal reaction. The electrochemical test shows that the specific capacitance of optimum NTO electrode can reach 120.45 F/g in 1 M Na 2 SO 4 solution with the scan rate of 1 mV/s by employing three-electrodes method. Moreover, the electrosorption capacity of AC/NTO asymmetrical electrodes is approach to 23.35 mg/g in NaCl solution with an initial concentration of 250 ppm. To improve the conductivity of NTO, reduced graphene oxide (rGO) is proposed to couple with NTO, named as rGO@NTO, to constitute the AC/rGO@NTO A-CDI. As a result, the AC/rGO@NTO A-CDI exhibited an ultrahigh desalination capacity of 41.8 mg/g in NaCl solution with an initial concentration of 250 ppm under 1.4 V, which is almost twice higher than that of AC/NTO electrodes and the highest value among all reported data anywhere. Besides, the charge efficiency of AC/rGO@NTO approaches to 1, implying the co-ions impaction has been successfully restricted. [ABSTRACT FROM AUTHOR]

• Strong coupling was established between NiCo-DH and OAC by oxidation modification. • NiCo-DH@OAC exhibited excellent electrochemical performance for synergistic effects. • ASCs were demonstrated effective in solar panel integrated supercapacitors. NiCo double hydroxide (NiCo-DH) and oxidized activated carbon (OAC) were used to synthesize a three-dimensional (3D) NiCo-DH@OAC via hydrothermal method. OAC acts as the support for in-situ growth of NiCo-DH nanowires, and oxygen-containing groups on the surface of OAC are crucial for the uniform loading of NiCo-DH and keeping structural stability of the composites. Due to the synergistic effect between NiCo-DH and OAC, NiCo-DH@OAC presents an excellent specific capacitance (1990 F g−1 at 1 A g−1). The asymmetric supercapacitor (ASC) is assembled with NiCo-DH@OAC as the positive electrode and OAC as the negative electrode, and exhibits a superior energy density (46.5 Wh kg−1 at 800 W kg−1) and a cycling stability (90.7% after 10,000 cycles). Furthermore, ASC has been demonstrated effective in solar panel integrated supercapacitors. [ABSTRACT FROM AUTHOR]

[Display omitted] • Modified carbon black (CB) by O 2 plasma technology for improving CDI capacity. • The effect and mechanism of plasma modified CB (PCB) to improve CDI were explored. • PCB improved the salt removal performance 6.9 times that of the original CB (OCB) • PCB can be applied to improve CDI of various active materials. • PCB has universal applicability in purifying brine, heavy metals and radionuclides. Previous research on capacitive deionization (CDI) mainly focuses on electrode active materials, while the research on conductive additive and their modification for improving CDI performance are rarely reported. In this work, we mainly investigate the effect and mechanism of oxygen (O 2) plasma-modified carbon black (PCB) to enhance CDI performance. The CB treated with O 2 plasma at 100 W for 10 min (CB-100 W-10 min) was assembled with activated carbon (AC) to form a CB-100 W-10 min/AC electrode with excellent desalination performance (32.54 mg g−1), 6.9 times that of the original CB/AC electrode (OCB/AC, 4.91 mg g−1). The roles of the specific surface area, hydrophilicity, electrical conductivity, and specific capacitance of CB in enhancing the performance of CDI were explored, and the interaction mechanism between H 2 O molecules and CB was investigated using molecular dynamics (MD) simulations. The advantages of PCB are mainly attributed to the synergy of the following aspects: (i) The excellent three-dimensional network structure acts as a "bridge" between activated carbon and increases the contact sites for allowing more PCB and AC to participate in the electrosorption process; (ii) Shorter electron transmission paths and more electron transmission channels between PCB and AC promote the electrosorption rate; (iii) High surface roughness and oxygen-containing functional groups of PCB boost hydrophilicity and dispersibility. Interestingly, we found that PCB possesses universal applicability in the enhancement of deionization performance of various active materials for purification of brine, heavy metals and radionuclides. This work unprecedentedly applies plasma technology to the modification of conductive additive, providing new ideas for material modification and improvement of CDI technology. [ABSTRACT FROM AUTHOR]

The functional combination of methylene blue and activated carbon successfully introduced a significant redox reaction in the activated carbon, increasing the specific capacitance of the material and significantly improving the rate performance. The methylene blue adsorbed on the surface of activated carbon enables fast proton-coupled electron transfer. [Display omitted] • Anthracite can be activated at low temperature and show large specific surface area. • Oxygen groups could effectively contribute the pseudo-capacitance to AC. • The π-π binding endows AC/MB excellent electrochemical properties. • The optimized AC/MB as positive can deliver ultrahigh energy and power density. • Mathematical simulation can optimize the ratio of positive to negative electrodes. Supercapacitors are desired to deliver high power and energy density concurrently, and the introduction of a redox reaction is an effective strategy to improve their capacitive performance. Herein, methylene blue (MB) with redox was employed to functionalize coal-based activated carbons (ACs) as electrode materials for energy storage. The optimized AC shows a high specific capacitance of 408.1 F g−1 in 6 M KOH, deriving from the contribution of the electrical double-layer capacitance of pores and pseudocapacitance of oxygen groups. Interestingly, pure MB shows no capacitive performance mainly due to its low conductivity, while the optimized composite of AC adsorbed MB (AC/MB) surpasses the pure MB and optimized AC in any capacitive performance, displaying a relationship of mutual promotion based on functional combination. The best AC/MB sample exhibits a high specific capacitance of 431.8 F g−1 at 1 A g−1, and 356.1 F g−1 (82.5%) at an ultrahigh current density of 180 A g−1, implying an excellent rate performance. Aiming to deliver maximum energy density, an accurate universal method is proposed to match the mass ratio of negative to positive. The optimized asymmetric supercapacitor AC/MB(+) || AC(-) delivers an energy density of 11.0 Wh kg−1, a power density up to 15.3 kW kg−1 and a high capacity retention rate of 96.3% after 10,000 cycles, displaying good chemical stability. This work proposes a promising strategy for ultrafast store/release energy at high energy density, and also provides an application direction for AC and MB. [ABSTRACT FROM AUTHOR]

[Display omitted] • First attempt to remove salt from the anaerobic OMBR sludge by FCDI. • The hybrid FCDI-OMBR obtained a higher net energy gain. • Desalination performance of AC, CB, CNT as FCDI electrode material were compared. • Synergistic desalination between different electrode materials was found. Osmotic membrane bioreactors (OMBRs) for anaerobic digestion of waste sludge have many advantages, but salt accumulation in the feed solution is a major problem. In this study, the feasibility of using flow-electrode capacitive deionization (FCDI) to mitigate salinity buildup was investigated. Three types of carbon materials, i.e., activated carbon (AC), carbon black (CB), and carbon nanotubes (CNTs), were tested as flow-electrode materials in desalination via FCDI. The results showed that, the salt removal efficiency (SRE) of CNTs was 110% higher than that of AC. Addition of CB and CNTs to 5.0 wt% AC as conductive additives at concentrations of 0.5 or 1.0 wt% synergistically enhanced the FCDI desalination performance. Cyclic voltammetry, galvanostatic charge–discharge, and electrical impendence spectroscopy showed that use of a combination of 5.0 wt% AC and 1.0 wt% CNTs gave an excellent capacitive performance, and the highest SRE, fastest average salt adsorption rate (0.84 μg cm−2 s−1), and the highest charge efficiency (85.0%) were achieved. The optimal voltage and sludge flow rate for FCDI of real OMBR sludge were 1.5 V and 80 mL min−1, respectively. In comparison with a control OMBR, a hybrid FCDI-OMBR system showed many advantages such as slower salinity buildup, alleviation of inhibition by ammonia, lower production of soluble microbial products, greater volumetric methane production, and higher net energy gains. The proposed hybrid FCDI-OMBR system provides a novel and cost-effective approach to recovering resources and energy from waste sludge or other types of biomass. [ABSTRACT FROM AUTHOR]

[Display omitted] • Charging activated carbon (AC) tunes adsorption of ionic but not nonionic compounds. • Defunctionalized AC allows better electro-assisted trap&release performance. • Combine surface modification and electric polarization for promoted removal. • Long-term (20 d) stable electro-assisted trap&release with high enrichment effects. • Electro-assisted trap&release promising for on-site AC regeneration. Highly water-soluble, persistent, and mobile organic compounds (PMOCs) are more and more often detected in surface and groundwater, evoking potential threats to the environment and human health. Traditional water treatment strategies, including adsorption by activated carbon materials, fail to efficiently remove PMOCs due to their hydrophilic nature. Electro-assisted sorption processes offer a clean, facile, and promising solution to remove PMOCs on activated carbon-based electrodes and potentially allow an easy on-site sorbent regeneration (trap&release). In this work, the electrosorption of five selected PMOCs, that is, tetrapropylammonium (TPA+), benzyltrimethylammonium (BTMA+), p -tosylate (p -TsO-), p -toluenesulfonamide (p -TSA), and methyl- tert -butyl ether (MTBE), were investigated on two comprehensively characterized activated carbon felt (ACF) types carrying different surface functionalities. Significant enrichment factors in ranges of 102 to 103 for charged PMOCs were expected by our first estimation for electro-assisted trap&release on ACFs in flow systems applying potentials in the range of −0.1 V/+0.6 V vs. SHE for ad-/desorption, respectively. Defunctionalized ACF carrying larger density in surface π-systems and lower O-content promises a higher capability in electrosorption processes than the pristine material in terms of better material stability (tested for 5 cycles over 500 h) and better removal efficiency of ionic PMOCs. To improve ACFs adsorption performance for cationic and anionic PMOCs, permanent chemical surface modification and reversible electric polarization as alternative strategies are compared. Our findings explore future electrode and process design of electrosorption for applications to treat water contaminated by emerging PMOCs. [ABSTRACT FROM AUTHOR]

[Display omitted] • Fungal hypha activated carbon pad (FhACPad) is a promising electrode for desalination. • FhACPad is a freestanding electrode readily prepared from the fungus suspension for CDI. • The continuous and porous structure of FhACPad facilitates both electron and ion transfer. • FhACPad with hierarchical pores exhibits a high desalination capacity of 35.6 mg NaCl /g. Capacitive deionization (CDI) is an emerging technology for water desalination, especially low-salinity water. Freestanding porous carbon-based electrodes with rapid electron transfer rate and effective ion diffusion features are desired to achieve high desalination performance. Here, a porous carbon pad derived from the fungal hyphae of Aspergillus niger was prepared as a precursor of the electrode. After carbonization and activation, the intertwined and hierarchical porous structure of the fungal hypha pad was well-preserved, producing a freestanding fungal hypha activated carbon pad (FhACPad) electrode for MCDI. The interconnected carbon fibers and open pore structure of the FhACPad yielded an electrode with high electrical conductivity and rapid ion transport properties. The novel FhACPad exhibited a gravimetric salt adsorption capacity of 35.6 ± 2.3 mg NaCl /g with an average desalination rate of 1.2 mg NaCl /g electrode /min from a 585 mg/L NaCl aqueous solution at a cell voltage of 1.2 V and a flow rate of 1 mL/min. As a result, the FhACPad outperformed conventional powdered activated carbon (PAC) electrodes and the most recently reported porous carbon electrodes under similar desalination conditions. This work also provides insights into the structure-performance relationships of CDI electrodes and shows a great potential of fungal biomass-derived porous carbon electrodes for high-performance MCDI applications. [ABSTRACT FROM AUTHOR]

[Display omitted] • Crude glycerol from biodiesel was used to obtain a new sustainable activated carbon. • The polyglycerol activated carbon electrodes successfully desalinate brackish water. • Operation within the potential stability window ensured the long-term stability. • Asymmetric configurations (CDI) and MCDI improved the charging efficiency. • The best stable desalination performance was achieved using the membrane CDI at 1.6 V. Capacitive deionization (CDI) is a promising electrochemical technology for water desalination that can contribute to reducing water scarcity. At the same time, appropriate routes for the disposal or reuse of liquid wastes are also a major current concern. Based on the water-waste nexus concept, this work demonstrates that crude glycerol from biodiesel plants can be successfully used to obtain a new sustainable activated carbon. After polymerization, the crude glycerol was carbonized and activated to obtain polyglycerol activated carbon (PGAC), which was employed as an electrode for CDI desalination of brackish water. Evaluation was made of the electrode performance and stability over cycles of electrosorption/desorption, using different cell configurations (symmetric, asymmetric, and membrane CDI) and cell voltages (E cell). It was observed that maintaining the potential of zero charge of the negative and positive electrodes outside their working domains during the cycles enabled minimization of that part of the applied potential deviated to co-ion repulsion, consequently improving the salt adsorption capacity (SAC) and charge efficiency (Q E). Furthermore, maintaining the potential of the positive electrode below the oxidation potential by controlling the applied E cell could ensure electrode stability. The best desalination performance using the PGAC electrode was achieved using the membrane CDI configuration (at 1.6 V), resulting in stable SAC (∼ 27.1 mg g−1) and Q E (∼100%) over 50 cycles. The low cost and high SAC and Q E values suggested that the PGAC electrode could be considered a potential candidate for use in CDI desalination. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ion sorption on EDL and pseudocapacitor was studied at constant potential. • α-MnO 2 was the best in diffusive capacitance among polymorphs. • Effects of ion solvation and valence on sorption of inert ions were studied. • Monolayer capacity as affected by electrode polarity was estimated via Langmuir model. • Isoelectric point of the reversible MnO 2 /AC composite was modified. The capability of manganese dioxide (MnO 2) supported on loofah-derived activated carbon (AC) in the electrosorptive removal of common inert ions was studied in constant potential mode. Four MnO 2 polymorphs were prepared by redox chemical precipitation and characterized by XRD, SEM, BET and XPS. The pseudocapacitance property of the MnO 2 /AC electrode, significantly affected by the surface- and diffusion-controlled charge storage mechanism, was assessed via voltammetry and modified Langmuir adsorption isotherm. Batch electrosorption experiments were then performed at constant potential in the range of −1.5 V to + 1.5 V (vs. Ag/AgCl) using AC and α-MnO 2 /AC electrodes in the presence of common simple electrolytes, including NaNO 3 , Li 2 SO 4 , and Ca(ClO 4) 2. Consequently, the applied working potential (E app) positively affected the ion electrosorption rate and capacity. Faradaic processes occurred on MnO 2 , i.e., Mn(III)/Mn(IV) transition, increased the diffusion capacitance of AC, thus enhancing the first-order rate and monolayer capacity, mainly for the electrosorption of cations. Results showed that ion solvation, controlled by the ionic radius and valence of an ion, which impacted ion intercalation in MnO 2 and affected ion adsorption characteristics. The cation sorption capacity of α-MnO 2 /AC followed the order of Na+ (2.8 × 10-4 mol g−1) > Ca2+ (2.1 × 10-4 mol g−1) > Li+ (0.76 × 10-4 mol g−1) at E app = -1.5 V. The differential capacitance as affected by polarized potential and the shift of zero net charge or IEP toward more positively charging potential further highlighted the contribution of pseudocapacitance to ion adsorption on α-MnO 2 /AC electrode. [ABSTRACT FROM AUTHOR]

[Display omitted] • QRAC electrodes selectively adsorb NO 3 – due to the difference in binding energy. • The selectivity coefficient of QRAC-5 to NO 3 – reaches 2.7 at 0.4 V. • The electrosorption behavior of QRAC depends on physical adsorption and ion exchange adsorption. Nitrate pollution has become an increasingly serious water pollution problem worldwide. Capacitive deionization (CDI) technology is an emerging water treatment technology that can efficiently remove nitrate in water with advantages of simple process, high water recovery rate, low cost and energy consumption. In this work, we engineer a covalently bonded quaternized activated carbon (QRAC) material by silanization and investigate its selective adsorption of nitrate in mixed solution with extended voltage capacitive deionization (eV-CDI) mode. The results show that (1) the QRAC electrodes achieve selective adsorption due to the different adsorption binding energies of the quaternary ammonium group with Cl- and NO 3 –. The selectivity coefficient of QRAC-5 to NO 3 – reaches 2.7 at 0.4 V and the electrosorption capacity is 140% higher than that of AC in 5/5 mM KCl/KNO 3 solution. (2) The electrosorption of QRAC electrodes are dominated by two aspects: physical adsorption by external electric field which occurs in the incipient stage and ion exchange adsorption by quaternary ammonium groups occurring in the following stage. (3) CDI experiments in simulated municipal wastewater show that SO 4 2- had a negative effect on the adsorption capacity of NO 3 –, but QRAC electrode can still achieve separation effect in Cl-/NO 3 – solution system. These results show that covalently bonded quaternized activated carbon can achieve the effective separation and removal of NO 3 – in polluted water, and our work provides new insights into the selective electrosorption of CDI technology. [ABSTRACT FROM AUTHOR]

• Adding low dose carbon materials can inhibit bromate formation in O 3 /PMS process. • The inhibition of bromate formation by three carbon materials is: GO > CNT > PAC. • Carbon materials can reduce HOBr/OBr− to form Br− and block bromate formation. • Formation of bromate in O 3 /PMS/carbon material was further reduced in actual water. Ozone/peroxymonosulfate (O 3 /PMS), firstly proposed by our group, is an efficient advanced oxidation process for the degradation of organic pollutants. However, the elevation of bromate formation was the main problem in the treatment of bromide-containing water. In this work, adding low dosage of powdered activated carbon (PAC), carbon nanotube (CNT) and graphene oxide (GO) in the inhibition of bromate formation and the enhanced degradation of organic pollutants during the O 3 /PMS process were firstly investigated. As 10 mg/L of PAC, CNT and GO were added, the bromate conversion efficiency (25.1%) was decreased to 15.9%, 14.1%, and 8.8% at pH = 7.0, 50 μM PMS addition and 1.135 mg min−1 ozone injection after 25 min reaction. It is shown that the carbon materials played a crucial role in reducing intermediate products (HOBr/OBr−) in the reaction, thereby blocked the bromate formation. This may be due to the defects such as vacancies and zigzag/armchair-like edges on the graphene boundary, which were reported as active sites for oxygen reduction reaction. Meanwhile, the addition of three carbon materials would also promote the degradation of oxalic acid and para -chlorobenzoic acid, and the effect of GO was better than the other two. According to the release of TOC in the reaction, the stability of GO was obviously stronger than that of PAC and CNT, which was attributed to that GO had a relatively stable lamellar structure. Finally, compared with the deionized water, the water matrices that would trap free radicals in actual water samples can significantly inhibit the bromate formation. Therefore, adding low dosage of carbon materials is an effective way to control the bromate formation and promote the degradation of organic pollutants in the O 3 /PMS process. [ABSTRACT FROM AUTHOR]

• CDI was applied for nitrate removal from synthetic domestic wastewater. • Concentrated nitrate stream was obtained during CDI regeneration. • CDI operational parameters were investigated. • Effect of PVDF on AC electrode was estimated. Capacitive deionization (CDI), an emerging technology, has attracted attention recently and has been applied for various purposes. Herein, we investigated the application of a CDI system using activated carbon (AC) electrodes for nitrate removal and recovery in the scope of domestic wastewater treatment. The electrochemical behavior and structural parameters of AC electrodes were investigated as a part of this work. CDI electrodes were fabricated from microporous activated carbon, and the specific surface area of the electrode material was 210 m2/g. The negative effect of polymeric binder on the AC electrodes performance was observed as well. The specific capacitance of the fabricated AC electrodes at 40 mV/s scan rate was 0.5 F/g and 19 F/g for 1 and 1000 mM electrolyte (NH 4 NO 3), respectively. The CDI performance was examined as a function of flow rate (2, 4, 9, 14 mL/min), applied voltage (0.6, 0.8, 1.0, 1.2 V), and initial nitrate concentration (10, 25, 50, 70 mg/L) in single-pass (SP) mode. Regeneration performance and recovery efficiency of the CDI cell were observed during 5 subsequent operational cycles. The recovery efficiency of nitrate ions from low salinity water was 21%, while the electrosorption capacity of 5.5 mg/g and removal efficiency of 48% was achieved. Presence of the competitive ions in the tested solution resulted in a slight decrease (~10%) of nitrate removal efficiency. [ABSTRACT FROM AUTHOR]