Search

Two sodium alginate-based Pb2+-imprinted thermosensitive hydrogels (SPIT (without ɛ-PL) and SPPIT (with ɛ-PL)) were synthesized, with sodium alginate and ɛ-polylysine (ɛ-PL) as the matrix, N-isopropylacrylamide as the monomer. Characterization with differential scanning calorimeter, Fourier transform infrared spectroscopy, thermogravimetric analyzer, scanning electron microscopy, X-ray photoelectron spectroscopy, and Raman spectroscopy confirmed the aimed structure of the hydrogels. The adsorption capacity of SPIT and SPPIT for Pb2+ was 98.64 mg/g and 153.49 mg/g, respectively. Washing the Pb2+-loaded adsorbent with 10 °C deionized water, SPIT and SPPIT achieved a desorption efficiency of 94.59 % and 97.51 %, respectively. After 10 cycles of adsorption-desorption process, the adsorption capacity and desorption efficiency remained at about 80–88 % of the original ones, expressing excellent reusability. In a mixture containing eight metal ions (Pb2+, Cu2+, Mg2+, Ca2+, Cd2+, Na+, K+, Fe3+), the adsorption capacity of SPIT to Pb2+ was 92.49 mg/g, and that of SPPIT was 102.49 mg/g, much higher than that to the other ions (1.50–11.38 mg/g on SPIT, 9.48–27.45 mg/g on SPPIT), showing excellent adsorption selectivity. The introduction of ɛ-PL enhanced the adsorption capacity, antibacterial ability and stability of the hydrogel, ensuring better application potential in real wastewater. • Two Pb2+-imprinted adsorbents were prepared with sodium alginate as the matrix. • The differential scanning calorimeter test confirmed the reversible thermosensitivity of the adsorbents. • Washing with cold water (5-10 °C) could regenerate the Pb2+-loaded adsorbents. • After 10 cycles of reuse, 80–88 % of the adsorption capacity was remained. • The adsorptive selectivity coefficient of adsorbent was up to 33.99. [ABSTRACT FROM AUTHOR]

The low capacity, poor rate capability and sluggish kinetics limit the practical application of carbonaceous materials. Heteroatom doping is an effective method to regulate the intrinsic property and improve electrochemical reactivity of carbon-based materials. Herein, we prepare N/O co-doped porous carbon nanofibers (N/O–PCNF) with large surface area and high heteroatom doping for sodium ion batteries. The excellent electrochemical performance of optimized N/O–PCNF sample is due to high diffusion coefficient and low charge transfer resistance during the sodiation/desodiation process. Kinetic analysis reveals that the capacitive behaviors play an important role in sodium storage performance of N/O–PCNF sample. Moreover, density functional theory calculations further demonstrate that N/O co-doping can promote the adsorption capacity of sodium ions, and provide theoretical guidance for the excellent sodium storage performance of the electrode. [ABSTRACT FROM AUTHOR]

• Structure evolution features of LDHs precursors with pH was investigated. • Role of pH on activating the performance of LDHs type adsorbents was concluded. • Precipitative formation mechanism of LDHs adsorbents was firstly proposed. Aluminum-based adsorbents, simply prepared by eluting the lithium-aluminum layered double hydroxide precursors with deionized water, is the only industrialized adsorbents for selectively separating Li+ from saline brines. Taking the roles of lattice and surface Li+ active sites on its performances into consideration, influence of ending pH modulating on prominently improving the adsorbing capacity and stability of aluminum-based adsorbents prepared by precipitation method is initially investigated. As experimentally evidenced that, the maximum desorption amount of Li+ at the eluting stage should be controlled to around 20 mg/g Li+ rather than thoroughly removed to effectively avoid the topotactic solid-phase transformation from adsorbent to α-Al(OH) 3. As-prepared adsorbents not only has high adsorption capacity up to 8.4 mg/g in 400 ppm LiCl solution, but also owns unique self-healing ability, thus promising the excellent cycling stability. It is firstly proposed that the formation of the layer-structured precursor by precipitation method is well in accordance with the three-step formation mechanism and pH modulating mainly contributes to the anions exchange between solution Cl- and interlayer OH–. This study experimentally proves the importance of pH adjusting for preparing high performance lithium adsorbents by precipitation method, which is very significant and important for effectively extracting lithium resources from the complicated multi-component liquid minerals. [ABSTRACT FROM AUTHOR]

• K 2 FeO 4 is first utilized for the solid-phase oxidation of pitch by a high-energy ball mill. • The solid-phase reaction mechanism involving in oxidation and condensation was revealed. • Advanced pitch-based porous carbon (H-CBPF) was prepared by a solid–liquid synergistic strategy. • The synergistic effect improves both the porous geometric configuration and O content of H-CBPF. • H-CBPF delivers an excellent salt adsorption capacity and a superior charge efficiency. To address limited desalination capacity and insufficient charge efficiency for carbon materials in capacitive deionization (CDI), a solid–liquid synergistic oxidation strategy of potassium pertechnetate (VI) for pitch was proposed to construct porous carbon with a reasonable pore structure and high reactive surface. On the one hand, K 2 FeO 4 is first utilized for the solid-phase oxidation (SPO) of pitch by a high-energy ball mill, introducing rich oxygen-containing groups such as ether bonds. Meanwhile, dehydro-condensation reactions occurred during SPO, resulting in the formation of the oxidized pitch with a high degree of condensation. Importantly, the pyrolysis yield of the oxidized pitch is as high as 46.9 % at 800 °C, almost twice that of the pristine pitch, meaning that the oxidized pitch with high polymer degree and rich C-O bridge bonds facilitates the carbon fixation and emission reduction during carbonization. On the other hand, the self-oxidation of K 2 FeO 4 in aqueous solution forms bifunctional activators (KOH and Fe(OH) 3) for the preparation of pitch-based porous carbon. Benefiting from the crosslinking structure of oxidized pitch and the multi-effective activation, the prepared porous carbon (H-CBPF) exhibits a robust layered stacking topology with a high surface area and oxygen content. Thereby, it can deliver an excellent salt adsorption capacity (SAC) of 22.1 mg g−1 with an average desalination rate of 1.89 mg g−1 min−1 and a high charge efficiency of 85 % at 1.2 V in 500 mg L-1 NaCl solution. This work opens up a green and economical route for the preparation of pitch-derived porous carbon for high-performance CDI. [ABSTRACT FROM AUTHOR]

[Display omitted] • A comprehensive review to highlight the application of 3D faradic materials in CDI field is presented. • The desalination performances of non-3D faradic electrodes and 3D faradic electrodes are systematically compared. • The perspective of 3D faradic materials is discussed to provide guidelines for future CDI development. To address the water scarcity issue, capacitive deionization (CDI) as a burgeoning desalination technology for removing different ions from sea and wastewater have been intensively explored. However, the low salt adsorption capacity and poor cycling stability of widely used carbon materials are difficult to fulfill the demand of practical CDI application, while the non-three-dimensional (non-3D) faradic electrode materials manifest the drawbacks of low specific capacitance and dissolution loss of metal ions, which severely limit their CDI application. Notably, three-dimensional (3D) faradic materials usually possess higher desalination capacity and better cycling stability than carbon materials and non-3D faradic materials, due to their wide ion diffusion channels and versatile structure, which are highly promising for achieving practical CDI application. However, few review papers have specifically focused on the limitations and advantages of 3D faradic materials in CDI field. In this review, a comprehensive insight into 3D faradic materials in terms of the solutions of limitations and corresponding desalination performance (via comparing with the desalination performance of non-3D faradic materials) is provided and the development prospect of 3D faradic materials is also expounded. [ABSTRACT FROM AUTHOR]

Energy shortage severely impedes the advancement of human society and economy. The vigorous development of nuclear energy is a viable solution to address this issue. The escalating depletion of uranium resources necessitates prioritizing the selective extraction of uranyl from seawater and wastewater to ensure the prosperity of nuclear power. A bismuth-based MOF, CAU-17, was synthesized by the one-step solvothermal method for targeted selection of uranyl in the first time. The uranium adsorption tests demonstrated that CAU-17 exhibited a high adsorption capacity of 421.9 mg g−1 (T = 25 °C, pH = 7), exceptional selectivity, outstanding salt tolerance, and favorable stability with 83.6 % of the initial capacity retained after 5 cycles. Through the utilization of XPS and theoretical calculations, it was elucidated that the carboxyl oxygen that connects the Bi played a pivotal role in the binding process between CAU-17 and uranium ions, with bismuth acting as an electron regulator through its bridging effect with carboxyl oxygen. This work not only presents an exceptional uranium adsorption material but also elucidates the role of core metal atoms in MOFs during the binding to uranium process, thereby offering a novel perspective for future advancements in MOFs-based adsorbents. [Display omitted] • A bismuth-based MOF, CAU-17, was synthesized by the one-step solvothermal method for targeted selection of uranyl. • CAU-17 exhibited a high adsorption capacity (421.9 mg g-1), outstanding salt tolerance, and favorable stability with 83.6% of the initial capacity retained after 5 cycles • CAU-17 formed a complex coordination with uranium through carboxyl oxygen atoms while bismuth played a role in charge regulation. [ABSTRACT FROM AUTHOR]

The efficiency of saturated Activated Carbon (AC) electrochemical regeneration was evaluated. Reactor configurations in cathodic/anodic process, applied current effect on the properties of AC and Methylene Blue MB-AC interactions and adsorption/desorption mechanisms were studied. The efficiency was measured by adsorption capacity adsorption/regeneration cycles and changes in the adsorbent characteristic were analyzed through FTIR, BET, Optical Microscopy (OM) and SEM before and after the regeneration. The energy consumption was analyzed to assess the economic feasibility. It was found that the electrochemical treatment was efficient in returning the AC adsorption capacity, maximum efficiencies of approximately 79% and 84% were reached when the Carbon Fiber Cloth-AC electrode was subjected to anodic and cathodic currents, respectively, at a current of 0.1 A. In addition, the material demonstrated good stability through adsorption-regeneration cycles by cathodic process, with the material's adsorption capacity being almost totally recovered for 8 consecutive cycles. The removal percentage around 80% was kept after the cycles, with optimal conditions when the electrode was subjected to cathodic currents, NaCI as electrolyte at a current of 0.1 A for 2 h. The characterization techniques provided results that allow to explain the higher and prolonged efficiency of the cathodic current. Furthermore, these reactor configurations achieved an electrical energy consumption of 2.3 and 2.1 kWh kg-1 of material for cathodic and anodic, respectively. These results indicate that the electrochemical is an economical and environmental suitable technique capable of restore carbon adsorbents to be reusable for several water treatment cycles. [ABSTRACT FROM AUTHOR]

[Display omitted] • Electrode material with efficient and selective phosphate adsorption was developed. • ZnFe-PANI/CNT electrode exhibited remarkable capacitive behavior and charge storage capacity. • ZnFe-PANI/CNT had excellent phosphate adsorption capacity over a wide parameters range. • The high phosphate removal rate was maintained after 10th regeneration processes. Capacitive deionization technology possesses puissant competitiveness in the field of water treatment due to its low cost and high efficiency. In this study, polyaniline (PANI) doped and carboxyl intercalated metal hydroxide composite (ZnFe-PANI/CNT) was developed by a simple co-precipitation method, and used as anode electrode for phosphate removal in sewage. The results show that ZnFe-PANI/CNT electrode can efficiently remove phosphate at concentration of 2–10 mg/L at a wide range of pH (3–10) by electric double layer capacitive adsorption and pseudocapacitive adsorption. The concentration of phosphate in the effluent was as low as 0.095 mg/L, and the coexisting anions (Cl−, NO 3 −, SO 4 2− and HCO 3 −) hardly inhibited the phosphate adsorption by ZnFe-PANI/CNT composite electrode. In addition, under the optimal phosphate adsorption conditions (pH = 7 and applied voltage of 1.2 V), the energy consumption of CDI system was calculated as low as 0.00274 kWh/g P and 0.017 kWh/m3 water, realizing the expectation of low cost and high efficiency operation. [ABSTRACT FROM AUTHOR]

It is widely recognized that greenhouse gas emissions (e.g., CO 2 , SF 6 , and CH 4) play a significant role in global warming. Adsorption at point sources, using a suitable adsorbent, is an important method to reduce their release. Zn(mIm) 2 , where mIm = 2-methylimidazolate (referred to as SOD-ZIF-8), is a typical Zeolitic Imidazolate Framework (ZIF) that has shown outstanding performance in the adsorption of greenhouse gases. However, its conventional synthesis is time-consuming and requires the addition of large amounts of organic solvents. Herein, we report a solid-state synthesis of ultramicroporous n-ZIF-8 nanocrystals at room temperature within 5 min. The comprehensive characterization of n-ZIF-8 involved FTIR, XRD, SEM, TGA analyses, and N 2 adsorption. The obtained results indicate that n-ZIF-8 has potential as an adsorbent for greenhouse gas adsorption. The physisorption process of CO 2 , SF 6 , and CH 4 is corroborated by the isosteric heat of adsorption (Q ads) data. To further support the experimental data, quantum computational DFT-GD3 calculations were performed. Validation by the quantum theory of molecules (QTAIM) confirms that the selected gases are well adsorbed through major electrostatic interactions. Additional support from the 3D-ELF/2D-LOL analyses, agreeing with QTAIM claims, highlights that ZIF-8 highly adsorbs CO 2 and CH 4 through van der Waals interactions. In conclusion, ZIF-8 exhibits remarkable adsorption capabilities, efficiently adsorbing CO 2 in the cavity and N 2 on the surface, making it a potential candidate for greenhouse gas removal. [Display omitted] • A new n-ZIF-8 was synthesized and characterized. • The n-ZIF-8 has shown a high CO 2 adsorption capacity vs SF 6 , CH 4 , and N 2. • The CO 2 and SF 6 adsorption capacities were constant in multiple adsorption cycles. • CO 2 gas is adsorbed in the center of the cavity through electrostatic interactions. • The n-ZIF-8 nanoparticle is powerful for new generations of adsorbent systems. [ABSTRACT FROM AUTHOR]

[Display omitted] • The roles of specific N-containing groups on HCHO removal were comprehensively studied. • The ACN-600 exhibited the superior HCHO adsorption capacity (16.37 mg/g). • DFT calculation results indicated that pyrrolic-N exhibited the highest HCHO adsorption energy (−32.83 kJ/mol). • Pyridinic-N could trigger the Cannizzaro-type disproportionation reaction. Inserting nitrogen (N) heteroatoms into the carbonaceous adsorbents has been confirmed to be one of efficient strategies for enhancing HCHO removal. However, the essential promotion mechanisms of specific N-containing groups (such as pyridinic-N, pyrrolic-N, and quaternary-N) remain blurred. Herein, a series of N-doped activated carbons were prepared by annealing the melamine impregnated activated carbons at 600–900 °C and used for HCHO elimination. It manifested that the HCHO elimination performance of samples was remarkably improved after N-doping and their HCHO adsorption capacities were in the order of ACN-600 (16.37 mg/g) > ACN-750 (9.87 mg/g) > ACN-900 (7.28 mg/g) > AC (5.09 mg/g). DFT calculation results revealed that there existed stronger attractive noncovalent interactions between pyrrolic-N doped carbon and HCHO due to the formation of stronger H-bonds. Therefore, the HCHO physisorption energy on pyrrolic-N doped carbon was the highest (−32.83 kJ/mol). Compared with the single physisorption mechanism of previous studies, the in-situ DRIFTS results manifested that the pyridinic-N atom (as a typical strong Lewis base) could trigger the Cannizzaro-type disproportionation reaction, which would transform toxic HCHO into relatively less toxic methanol and formic acid. Benefiting from the dual enhanced mechanisms of attractive noncovalent interactions and Cannizzaro-type disproportionation reaction, the ACN-600 manifested excellent HCHO removal performance. This study not only intrinsically discloses the promotion mechanism of specific N-containing groups on HCHO removal at molecular level but also provides guidelines for rational design and development of carbonaceous materials for effective HCHO elimination. [ABSTRACT FROM AUTHOR]

• A novel capacitive deionization with a three-phase architecture (T-CDI) was proposed. • Cathodic oxygen reduction was enhanced in T-CDI without affecting desalination. • SAC value and H 2 O 2 generation were 14.91 mg/g and 25.55 mg/L, respectively. • Simultaneous desalination and organics control was achieved by T-CDI/UV. • Applicability of T-CDI in long-term operation was investigated. Cathodic oxygen reduction, as a Faradaic side reaction, has been proven to be thermodynamically favorable for H 2 O 2 generation in capacitive deionization (CDI), which may provide a greener manner for organics control alongside desalination. However, the low levels of dissolved oxygen (DO) in saline water and its potential Faradaic degradation of carbon-based electrodes limit the H 2 O 2 generation in the conventional CDI (C-CDI). Herein, a novel three-phase CDI architecture (T-CDI) was proposed to simultaneously achieve stable desalination and supplementary H 2 O 2 generation. Unlike C-CDI architecture, T-CDI was open-ended at the cathode side, where porous nickel foam was used as current collector and air diffusion layer. Accordingly, a stable gas–liquid-solid three-phase interface was created inside the cathode, thus enhancing the diffusion and utilization of atmospheric air and preventing the damaging effects of excessive DO on the electrode. A stable electrosorption and electrocatalysis performance for T-CDI was obtained by regulating electrode hydrophilic-hydrophobic properties, comparing with other CDI configurations, and altering operating conditions. The salt adsorption capacity and H 2 O 2 accumulative concentration were 14.91 mg/g and 25.55 mg/L, respectively. Furthermore, the simultaneous desalination and organics control in T-CDI were investigated with the assistance of UV irradiation (T-CDI/UV). When treating NaCl and sulfamethazine (SMR) mixture solution, T-CDI/UV significantly reduced the irreversible electrode organic fouling and improved the desalination stability. Additionally, the potentially hazardous SMR was effectively removed alongside desalination. Finally, the long-term operation of T-CDI demonstrated that the generated H 2 O 2 cannot induce an additional substantial deterioration in desalination stability. The techno-economic assessment showed T-CDI was economically competitive compared with C-CDI. This study provides insights into the synergy of non-Faradaic and Faradaic processes and further diversifies the application of CDI in water treatment. [ABSTRACT FROM AUTHOR]

[Display omitted] • Dual cation titanosilicate(DTS) was utilized in CDI to capture Cs+ and Sr2+. • By applying −1.2 V, the DTS electrode exhibits a high adsorption capacity. • DTS electrode showed rapid kinetics over 95 % of adsorption capacity within 30 min. • It provides a high selectivity of 5x103 mL/g in 10000-fold Na concentrated solution. • It was regenerated by applying + 2.0 V and its structural integrity remains intact. The utilization of ion intercalate capacitive deionization technology is garnering attention as an electrified water treatment method. This study proposes a capacitive deionization technology incorporating Dual-cation TitanoSilicate (DTS) to enable efficient electro-sorption/desorption of radioactive ions Cs and Sr. The synthesized DTS possesses a robust structure, high selectivity for Cs and Sr, and substantial adsorption capacity, incorporating redox-active titanium. Employing DTS as an active material in the electrode demonstrated a high adsorption capacity (186 mg Cs/g, 177 mg Sr/g) and rapid adsorption kinetics, reaching maximum capacity within 30 min, even in environments with a tenfold excess of competing ions. Furthermore, our system exhibited stable performance over 5 cycles of adsorption/desorption, and post-desorption analyses confirmed the durable structure stability without significant alterations. This study highlights the feasibility of CDI technology utilizing DTS for cesium and strontium removal. [ABSTRACT FROM AUTHOR]

The open-cell bio-based biodegradable polymer foams show good application prospect in dealing with the serious environmental issue caused by oil spill and organic solvents spills, while the cell structures and hydrophobic properties of the foams limit their performance. In this work, the poly(3-hydroxybutyrate- co -3-hydroxyvalerate) (PHBV) was selected to help prepare bio-based biodegradable poly(lactic acid) (PLA) foams. Based on a two-step foaming method, the crystallization ability of different samples was regulated by the "original crystals" together with PHBV in the foaming process, where skeleton structures were provided to facilitate the open-cell structures and promote their mechanical property. As illustrated, PHBV facilitated the formation of open-cell PLA foams, where the foams displayed superior oil-water separation capacity. The maximum volume expansion ratio of the foams was 80.08, the contact angle of deionized water reached to 134.5°, the adsorption capacity for oil or organic solvents was 10.8 g/g-51.8 g/g, and the adsorption capacity for CCl 4 can still maintained 83.5 % of the initial value after 10 adsorption-desorption cycles. This work not only clarified the foaming mechanism of open-cell foams, but also provided a green and simple method for preparing bio-based biodegradable foams possessing excellent oil-water separation performance. [ABSTRACT FROM AUTHOR]

Efficient recovery of rare scattered metal Re(VII) from various resources is a prerequisite due to its important application. Herein, a type of novel nanofibrous membrane, 0.4P(Ph-3MVIm-Br)-3PVP/2TPU, is successfully prepared by electrospinning, where poly(ionic liquid) P(Ph-3MVIm-Br) is incorporated and could supply more adsorption sites. Meanwhile, PVP (polyvinyl pyrrolidone) and TPU (thermoplastic polyurethane) ensured the water flux and the structural stability of the membrane. The nanofibrous membrane exhibited a high adsorption capacity for ReO 4 −, which can reach 128 mg g−1 at pH 5. Its water flux is as high as 433 L m−2 h−1 at 0.4 g of poly(ionic liquid) addition, membrane thickness of 20 μm, and pressure of 1 bar. Furthermore, 0.4P(Ph-3MVIm-Br)-3PVP/2TPU nanofibrous membrane can remove 91.7% of ReO 4 − within 30 min. After 9 times recycling, the adsorption efficiency of the membrane can still maintain more than 90%. Dynamic ReO 4 − removal with 0.4P(Ph-3MVIm-Br)-3PVP/2TPU after one cycle was accomplished with a breakthrough volume of 24 mL ReO 4 − solution (feed 10 mg L−1, 100 mg membrane). The exchange of ReO 4 − and Br− of poly(ionic liquid) mostly promote the adsorption of ReO 4 −. Moreover, the structure of the membrane has excellent selectivity, mechanical performance, strong acid and alkali resistance stability, which endow the membrane easy to operate in practical applications. [Display omitted] • Nanofibrous membrane can remove 91.7 % of ReO 4 − within 30 min. • It has a great adsorption capacity of 128 mg g−1 for ReO 4 − at pH 5. • It has a good selectivity for ReO 4 − in the presence of SO 4 2− or NO 3 −. • It unfolds prominent regeneration ability after nine consecutive cycles. • It can achieve a water flux of 433 L m−2 h−1. [ABSTRACT FROM AUTHOR]

[Display omitted] • Amidoxime-modified g-C 3 N 4 electrode was hydrothermally synthesized. • Th(IV) electrosorption was studied by varying voltage, time, and concentration. • Maximum adsorption capacity was 275.74 mg.g−1 at – 1.0 V within 30 min. • Chemisorption and double-layer charging occurred with AX/g-C 3 N 4 in electrosorption. • The electrosorption occurs via the abundant of N and O redox sites of AX/g-C 3 N 4. Electrosorption is a technique that combines electrical and adsorption processes and has been established to displace Th(IV) from aqueous solutions. The present study successfully synthesised a novel electrode, where graphitic carbon nitride was modified with amidoxime amidoxime groups (g-C 3 N 4 /AX) via the hydrothermal method. The batch experiments conducted in this study revealed that the g-C 3 N 4 /AX electrode possessed a favourable thorium adsorption capacity of 275.74 mg.g−1 and a swift elimination equilibrium of within 30 min. Furthermore, the removal efficiency at − 1.0 V (84.46 %) of the electrode was almost threefold greater than the removal efficiency at open circuit potential (24.09 %). The results were due to the free electrical charges on the g-C 3 N 4 /AX electrode, which induced the electrical driving force and facilitated the adsorption of Th(IV) ions onto the g-C 3 N 4 /AX surface. The shifted bands from the Fourier transform-infrared (FT-IR) spectrum post-electrosorption demonstrated a substantial complexation of Th(IV) with the amine groups of amidoxime and g-C 3 N 4. A significant transference in energy band peaks was also observed during the XPS assessment, indicating that the electrosorption process included oxygen (O), carbon (C), and nitrogen (N) species. In the practical real wastewater involving rare earth residue, which contains Ce, La, Nd and Pr ions, g-C 3 N 4 /AX exhibited good capabilities in selectively adsorbing Th(IV). The electrode synthesised in this study also exhibited the ability to regenerate with a reasonable ∼ 80 % removal ratio after five runs. The results indicated that the amidoxime-modified graphitic carbon nitride electrode demonstrated a good potential in removing thorium from aqueous solutions via electrosorption applications. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) holds great promise for phosphorus adsorption and recovery from wastewater, while current electrodes exhibit poor salt adsorption capacity (SAC) and selectivity due to co-ion effect and interference of co-existed ions with high concentration. Herein, to overcome these issues, a facile route was proposed to prepare a covalent organic framework-membrane coating electrode (COF-MCE) by depositing polyvinyl alcohol/polyethyleneimine membrane onto activated carbon fiber (ACF) followed by the in-situ growth of COF-LZU1. Compared to ACF and MCE, COF-MCE, with abundant functional groups and specific sites, facilitated electrical double layer (EDL)-based adsorption and induced hydrogen-bond interaction with phosphorus, contributing to a higher SAC of phosphorus (10.5 mg/g) in treating 1 mM NaH 2 PO 4. When treating different mixtures of NaH 2 PO 4 /NaCl, NaH 2 PO 4 /NaNO 3 , and NaH 2 PO 4 /Na 2 SO 4 with molar ratio of 1:5, COF-MCE exhibited the high phosphorus selectivity of 3.62, 5.98 and 7.01, respectively, which was attributed to the synergistic effects of EDL-based adsorption, hydrogen-bond and pseudocapacitance. Desorption experiments revealed that high reversal voltage and alkaline condition can weaken the hydrogen-bond interaction and strengthen the electrostatic repulsion between COF-MCE and phosphorus, thus improving the desorption and recovery of phosphorus. These findings confirmed the high potential of COF-MCE in the effective electrosorption and recovery of phosphorus from wastewater. • COF-MCE was prepared by casting followed by in-situ growth of COF powders. • Inhibited co-ion effect and enhanced EDL formation led to superb P adsorption. • Hydrogen-bond and redox-reaction interaction contributed to high selectivity for P. • A reversal voltage and high pH weakened the interaction and favored P recovery. [ABSTRACT FROM AUTHOR]

[Display omitted] • Defective MoS 2 electrode exhibited highly efficient and selective lead(II) adsorption. • Removal efficiency at initial concentration from 1 to 100 mg/L can reach ∼ 100 % • Adsorption capacity and removal efficiency were enhanced almost 8 folds after applying voltage. • Introduction of defects strengthened chemicalsorption and electrosorption. • A complete lead(II) desorption and reusability of electrodes can be achieved. Developing method for efficient lead(II) removal from aqueous solutions over a wide concentration range is urgent but challenging. In this work, defective molybdenum disulfide (MoS 2) was served as electrode coating to capture lead(II) over a wide range from aqueous solution via chemisorption and electrosorption coupling (CEC) process. The distinct adsorption behaviors of lead(II) on defective MoS 2 electrode were theoretically and experimentally investigated. In a wide concentration range (1 ∼ 100 mg/L), the removal efficiency of lead(II) from aqueous solutions can be close to ∼ 100 %. Adsorption capacities for lead(II) removal at initial concentration of 8.37 and 18.71 mg/L were 64.99 and 159.98 mg/g, respectively. After applying voltage, adsorption capacity and removal efficiency were enhanced almost 8 folds due to strengthened migration of ions, electrostatic interaction and electric double layer. Besides, lead(II) was completely desorbed from defective MoS 2 electrode within 60 min, and defective MoS 2 electrode by CEC process maintained excellent regeneration ability even after 10 cycles. Defective MoS 2 electrode has shown superior properties for lead(II) removal, such as (i) great specific capacitance and (ii) low charge transfer resistance toward the enhanced adsorption capacity and diffusion for lead(II) in the electrical double layer, compared with MoS 2. Extensive computations and characterizations of defective MoS 2 -lead(II) interaction demonstrated that the active unsaturated S sites were indispensable for lead(II) adsorption, which was beneficial for chemisorption. Based on the strong interaction with lead(II), defective MoS 2 electrode showed high-selectivity lead(II) adsorption with co-existence metal ions. Overall, defective MoS 2 as electrode coating by CEC has a great potential for the practical application in removing heavy metal ions from aquatic environment. [ABSTRACT FROM AUTHOR]

Based on the electro-negativity and structural characteristics of CR, a novel copper-organic framework (Cu-MOF) was synthesized with unique cage topology and cation network. The Cu-MOF exhibited efficient and targeted adsorption, separation and recovery characteristics for CR. The DFT calculation and two-dimensional correlation spectroscopy analysis further revealed that the energy distribution in CR adsorption was dominated by electrostatic interactions, followed by π-π stacking and van der Waals interactions. [Display omitted] • A novel Cu-MOF with caged topology and cation framework was synthesized for Congo Red (CR) specific-adsorption. • The Cu-MOF exhibited the efficient performance with the maximal adsorption capacity of 119.76 mg/g. • The Cu-MOF realized the separation, purification and recovery of the CR from mixed dyes. • Mechanism revealed the adsorption was spontaneous and exothermic with monolayer diffusion. • DFT and 2D-COS analysis clarified the adsorption was generated through electronic interaction and π-π stacking. Metal-organic frameworks (MOFs) with a three-dimensional (3D) caged structure and charged networks are promising adsorbents for separation and purification applications. However, it is a challenge to synthesize the MOFs in crystalline structures with a targeted ability of efficiently removing and reutilizing the individual diazo dye from sewage. Here, we report the synthesis of a novel copper-organic framework (Cu-MOF) with a 3D caged stucture and cationic networks using CuCl 2 and a triazole ligand (methyl-1H-1,2,4-triazole-3-carboxylate MTC). The novel Cu-MOF exhibited highly efficient and targeted adsorption, separation and recovery characteristics for Congo Red (CR). Specifically, the maximal adsorption capacity was 119.76 mg·g−1, and the adsorbed CR can be efficiently released in NaCl-DMF solution with a recovery rate of almost 100%. After suffered from three adsorption–desorption cycles, the Cu-MOF could still reach a adsorption rate of >85% and maintain an intact skeleton structure. The batch-equilibrium experiment combined with density functional theory calculation further revealed that the adsorption process was spontaneous and exothermic, following the pseudo-second-order kinetic equation with monolayer diffusion. The specific adsorption of Cu-MOF for CR was precisely generated through electronic interaction with the –NH 2 and -SO 3 groups, exhibiting the adsorption energies of −2.16 eV and −2.04 eV, respectively. The two-dimensional correlation spectroscopy analysis comfirmed that the energy distribution in CR adsorption was dominated by electrostatic interactions, followed by π-π stacking and van der Waals interactions. In summary, our work not only presents a promising strategy for the targeted separation and purification of CR from wastewater, but also contributes to the design of highly efficient MOF-adsorbents for other organic pollutants. [ABSTRACT FROM AUTHOR]

As an eco-friendly technique with the superior adsorption performance, electroadsorption has shown great potential for application in uranium (U(VI)) recovery in recent years. However, the electrodes used in the electrosorption generally suffer the adsorbent to be loaded on the conductors, which greatly limited the adsorption performance of the electrodes for uranyl ions. In present study, a flexible self-supporting Na 3 MnTi(PO 4) 3 @C fibers (NMTP@C fibers) electrode material was rationally designed and prepared by electrostatic spinning method and annealing technique, and its ability to capture U(VI) efficiently was preliminarily demonstrated by batch adsorption and electro sorption. The plentiful phosphate groups provide sufficient active sites for adsorption, while the axially continuous electron conduction and radially short-range ion transport give NMTP@C fibers fast charge/ion transport capability. The NMTP@C fiber can remove 99% of 5 ppm U(VI) in seawater by electro absorption within 1 h. After several cycles of adsorption under seawater conditions, the adsorbent can still maintain a stable adsorption capacity. The adsorption mechanism of NMTP@C nanofibers for U(VI) was investigated by XPS, FT-IR, Raman, SEM-EDS, and XRD, which was electrostatic interactions and surface complexation. These results suggest that NMTP@C fibers are promising high-capacity adsorbents for efficient and selective capture of U(VI) from seawater. [Display omitted] • Na 3 MnTi(PO 4) 3 @C was rationally designed as flexible self-supporting electrode. • Na 3 MnTi(PO 4) 3 @C is ecofriendly, low cost and low energy consumption. • Na 3 MnTi(PO 4) 3 @C exhibit high selectivity and uptake capacity for U(VI) with remarkable reusability. • U(VI) adsorption mechanism involves electrostatic interactions and surface complexation. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) technology represents a potent approach towards energy-efficient and sustainable access to potable water, with minimal environmental impact. However, the ion removal capacity of CDI systems remains inadequate for desalination of saline water. Herein, mesopore-enhanced graphene foam with modified hydrophilicity via O 2 -plasma treatment (MGFP) is proposed for ultrahigh CDI. This developed MGFP encompasses abundant mesopores, outstanding electrical conductivity and good hydrophilicity, enabling fast ions migration, efficient solution/pores contact and high adsorption capacity. As such, MGEP delivers a high specific capacitance of 156.64 F g−1 at 1 mV s−1, and a maximum salt adsorption capacity (SAC) up to 40.76 mg g−1 (1000 mg L−1, 1.2 V), much higher than most of the CDI systems leveraging the carbon-based materials. What's more, MGFP can be employed in the treatment of wastewaters containing various heavy metals, with the SAC of 89.96, 83.38, and 91.80 mg g−1, as for CuCl 2 , CoCl 2 , and NiCl 2 (1000 mg L−1, 1.6 V), respectively. This well-developed MGFP undoubtedly presents a promising material platform within the CDI system, effectively tackling the pressing concern of water scarcity. Mesopore-enhanced MGFPs electrodes with modified hydrophilicity have been successfully proposed for ultrahigh CDI performance. MGFP exhibits abundant mesopores, outstanding electrical conductivity and good hydrophilicity, enabling fast ions migration, efficient solution/pores contact and high adsorption capacity. As a result, MGEP delivers a maximum salt adsorption capacity (SAC) up to 40.76 mg g−1 (1000 mg L−1, 1.2 V), and demonstrate the SACs of 96.69, 83.38 and 91.80 mg g−1 when treating heavy metal salt wastewater containing CuCl 2 , CoCl 2 and NiCl 2 , respectively. [Display omitted] • High performance capacitive deionization with Mesopore-enhanced graphene electrodes with modified hydrophilicity. • The interaction mechanism of the modified material in solution for Na+ was investigated. • The highest salt adsorption capacity of NaCl during CDI was 40.76 mg g–1. • MGFP3 showed great potential in treating wastewater containing CuCl 2 , CoCl 2 and NiCl 2 with high SACs. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) technology has shown practicality and cost-effectiveness for water desalination. However, electrode development remains a major challenge. Carbon electrodes, commonly used in CDI, have limited adsorption capacity, necessitating the improvement of their physicochemical and electrochemical properties. To address these limitations, Faradaic electrodes based on the redox process have emerged as an alternative. Faradaic reactions in CDI systems offer benefits such as pseudocapacitive/intercalation effects and the development of charged species. Different types of Faradaic reactions include anodic oxidation reactions (to be avoided in CDI), cathodic oxygen reduction reactions, and Faradaic ion storage processes involving intercalation effects. Faradaic electrodes exhibit higher ion storage capacity due to their redox reactions and have been produced in various forms, expanding the range of available CDI electrodes. This indicates a promising future for Faradaic materials in CDI technology. The review highlights recent strategies in the development of capacitive and Faradaic electrode materials for CDI, along with progress in material synthesis and its impact on desalination. The review also introduces approaches to address complexities in defining optimal electrode parameters and achieve material optimization in electrochemical desalination. Overall, advancements in material development for electrochemical desalination processes are overviewed. [Display omitted] • Electrochemical desalination of seawater/brine was reviewed. • A wide range of electrode material design has been analyzed. • Faradaic redox reactions in CDI were represented. • The performances of various electrode materials have been summarized and compared. • Future challenges in the field of CDI have been discussed. [ABSTRACT FROM AUTHOR]

Cathode materials with high capacity and cyclic durability are urgently needed for capacitive deionization. Na 3 V 2 (PO 4) 3 is an emerging pseudocapacitive candidate for this process on account of its high capacity and Na+ reversible insertion, while it suffers from the intrinsic low electrical conductivity and small electrolyte-accessible surface area. Herein, a sea urchin-like Na 3 V 2 (PO 4) 3 @carbon (NVP@C) compound material was synthesized from MXene-V 2 C via hydrothermal method followed by annealing treatment, and then assembled as capacitive deionization (CDI) electrode material. Benefiting from three-dimensional sea urchin-like structure, where the nanoneedles of NVP@C serve as fast transport channel for Na+, NVP@C performed high specific capacity (437 F g−1 at 5 mV s−1) and fast ionic diffusion kinetics. Moreover, the NVP@C showed attractive desalination performance as cathode material for CDI, achieving a remarkable adsorption capacity of 74.0 mg g−1 in a NaCl salt solution (1000 mg L−1) and long life cycle stability. The present work provides a novel perspective to construct practical redox-active and stable CDI electrode with 3D structure from MXene for highly capacitive and durable desalination application. [Display omitted] • An urchin-like NVP@C derived from V 2 C MXene was used for capacitive deionization. • The NVP@C showed superior electrochemical performance with high capacity of 437 F g−1. • The NVP@C exhibited an outstanding salt (Na+) adsorption capacity of 74.0 mg g−1. • The unique structure provides fast ion transfer channels and ensures the stability. [ABSTRACT FROM AUTHOR]

Heteroatom doping, involving the introduction of atoms with distinct electronegativity into carbon materials, has emerged as an effective approach to optimize their charge distribution. In this study, we designed a strategy to synthesize in-situ Mn, N co-doped carbon nanospheres (Mn-NC) through the polycondensation of 2,6-diaminopyridine and formaldehyde in synchronization with Mn2+ chelation to form Mn-polytriazine precursor, followed by calcination to form carbonaceous solid. Then Mn-NC was fabricated into a capacitive deionization (CDI) electrode for the selective removal of uranium ions (U (VI)), which is commonly found in radioactive water. Interestingly, Mn-NC exhibited good selectivity for UO 2 2+ capture with a demonstrated adsorption capacity of approximately 194 mg/g @1.8 V. The systematic analysis of the adsorption mechanism of UO 2 2+ revealed that N dopants within Mn-NC can coordinate with the U (VI) ions, thereby facilitating the removal process. Our study presents a straightforward and convenient strategy for removing UO 2 2+ ions by harnessing the coordination effect, eliminating the requirement for pore size control. [Display omitted] • Trace Mn in N doped carbon can boost charge density and adsorption energy. • Mn–N–C adsorbs UO 2 2+ ions by coordination interaction with high selectivity. • This material has a good adsorption capacity of 194 mg/g @1.8 V. [ABSTRACT FROM AUTHOR]

[Display omitted] • Dopamine-functionalized carbon interface enhances interfacial activity. • Boron and oxygen are codoped to optimize the capacitive behavior of carbon materials. • The inside-out pore creating method of body phase improves the activation efficiency. As a typical double-layer capacitive electrode material, carbon nanomaterials show desirable application potential in the field of capacitive deionization (CDI) and supercapacitors (SCs). In this work, interfacial functional groups and B\O co-doping defects are simultaneously introduced into multi-chamber carbon with confinement effect, and their practical applications in CDI and flexible capacitors are also studied. Specifically, the oxygen-rich carbon source and boron source, dissolved and mixed completely via co-crystallization method, released amount of gas during the pyrolysis process to produce multi-chamber honeycomb-like carbon with ultrathin walls, which were further introduced into abundant interfacial functional groups by dopamine to optimize the carbon surface. At the same time, part of boron atoms entered the carbon lattice to form boron doping at high temperature, followed by the integration with the oxygen heteroatoms in carbon source to generate abundant boron and oxygen codoping defects. The as-prepared diatomic defects by the synergistic effect promote the wettability and pseudocapacitance of the material. In addition, the derived carbon materials are endowed with good hydrophilic ability and surface activity under the modification of dopamine functional groups. The ideal hydrophilic ability ensures that the porous structure of material can be infiltrated by electrolyte to provide large effective specific surface area, which enhances the electrical double-layered capacity. The interfacial functional groups also offer additional pseudocapacitance, so as to improve the ion adsorption capacity of PDA-BOC. [ABSTRACT FROM AUTHOR]

• The effect of operating conditions on the desalination rate was studied. • Under various conditions, ion adsorption follows a quasi-first order kinetic model effectively. • MCDI outperforms other CDI methods in desalination rate and ion adsorption. • Optimal conditions: 1.6 V voltage, 30 mL/min flow rate, 1000 mg/L initial concentration. Membrane Capacitive Deionization (MCDI) is an efficient desalination technology using ion-selective membranes and capacitive principles to remove ions. Highly mineralized water flows through parallel electrode plates separated by ion-selective membranes. An applied electric field adsorbs ions onto electrodes, creating an electric double layer, and periodic field reversals release enriched ions back into the water while discharging ions on the electrode surfaces, enabling continuous deionization. This study aims to investigate the feasibility of using MCDI technology with Prussian blue analog (PBA)/carbon electrodes to treat highly mineralized water in oilfields. The desalination rate under different operating conditions is experimentally analyzed and compared. A comparison is made between the Capacitive De-Ionization (CDI) systems in terms of changes in conductivity, desalination rate, ion adsorption capacity, and ion adsorption rate. Results showed that compared to conventional CDI and Hybird-CDI (HCDI), MCDI demonstrates the highest desalination rate, ion adsorption capacity, and ion adsorption rate. It indicates that MCDI has significant advantages in treating highly mineralized water. At a voltage of 1.6 V, a flow rate of 30 mL·min−1, and an initial concentration of 1000 mg·L−1, the MCDI system exhibited the highest desalination efficiency. Under these conditions, the desalination rate was 43.4%, the electrosorption capacity was 54.75 mg·g−1, and the electrosorption rate was 0.018 mg·g−1·s−1. The study provides a viable solution for the treatment of highly mineralized water in oilfields and serves as a reference for further improvement and application of MCDI technology. [ABSTRACT FROM AUTHOR]

Bioelectrochemical system is a prospective strategy in organic-contaminated groundwater treatment, while few studies clearly distinguish the mechanisms of adsorption or biodegradation in this process, especially when dense biofilm is formed. This study employed a single chamber microbial electrolysis cell (MEC) with two three-dimensional electrodes for removing a typical organic contaminant, 2,4-dichlorophenol (DCP) from groundwater, which inoculated with anaerobic bacteria derived from sewage treatment plant. Compared with the single biodegradation system without electrodes, the three-dimensional electrodes with a high surface enabled an increase of alpha diversity of the microbial community (increased by 52.6% in Shannon index), and provided adaptive ecological niche for more bacteria. The application of weak voltage (0.6 V) furtherly optimized the microbial community structure, and promoted the aggregation of microorganisms with the formation of dense biofilm. Desorption experiment proved that the contaminants were removed from the groundwater mainly via adsorption by the biofilm rather than biodegradation, and compared with the reactor without electricity, the bioelectrochemical system increased the adsorption capacity from 50.0% to 74.5%. The aggregated bacteria on the surface of electrodes were mainly dominated by Delftia tsuruhatensis (85.0%), which could secrete extracellular polymers and has a high adsorption capacity (0.30 mg/g electrode material) for the contaminants. We found that a bioelectrochemical system with a three-dimensional electrode could stimulate the formation of dense biofilm and remove the organic contaminants as well as their possible more toxic degradation intermediates via adsorption. This study provides important guidance for applying bioelectrochemical system in groundwater or wastewater treatment. [Display omitted] • Bioelectrochemical system was used to treat chlorophenol-contaminated groundwater • External electricity led to the aggregated biofilm on three-dimensional electrode • The dense biofilm enhanced the adsorption of chlorophenols from 50% to 74.5% • The aggregations on electrode were dominated by Delftia tsuruhatensis (85%) • Delftia tsuruhatensis was enriched for the first time in bioelectrochemical system [ABSTRACT FROM AUTHOR]

With the continuous development of the global society, people's demand for lithium is increasing. Recovering valuable lithium from waste lithium-ion batteries and fly ash is essential for environmental protection and energy saving. We have developed a new imprinted capacitance deionization technology (N@Li+-IPDI), which can selectively recover lithium ion from acidic solution (pH = 2) under complex environment. The recovery capacity of N@Li+-IPDI electrode material was up to 20.26 mg/g. Separation of Li+ from Na+, K+, and Al3+ was achieved based on the size effect. Separation from Mg2+ was due to the higher hydration energy of Mg2+ (1940 kJ/mol) than Li+ (510 kJ/mol). After 5 regeneration cycles, recovery effect of N@Li+-IPDI was 93.42 % of original. Through density functional theory (DFT) modeling, bond length of Li+-O was 2.04–2.05 Å, and adsorption energy of 2H12C4-Li+ (−33.66 Kcal/mol) was the largest among the five ions. In addition, energy and structure of deprotonation process were studied, and the energy required for deprotonation was 6.33 kJ/mol, which was the reason Li+ adsorption is difficult in acidic environment. This research provides a new green ion recovery technology with excellent selectivity, high adsorption and conductivity for Li+ recovery in acid solution, to meet the challenge of growing demand for lithium. [Display omitted] • Ion imprinting technology and capacitive deionization technology are combined. • The maximum adsorption capacity of the N@Li+-IPDI is up to 20.26 mg/g under pH = 2. • Crown ether protonation was effectively overcome under electric field. • Adsorption energy of Li+ (−33.66 Kcal/mol) was the largest among cations. • The energy required for deprotonation was 6.33 kJ/mol. [ABSTRACT FROM AUTHOR]

Understanding the stability of the bentonite buffer when exposed to cement leachates at temperatures exceeding 100°C is crucial for optimizing the design of deep geological repositories (DGRs) for high-level radioactive wastes (HLRWs) and minimizing the required site area. Experiments were conducted under hydrothermal conditions at 150°C for 30–150 days using deionized (DI) water (pH 6) and K-rich solutions (1 mol/L KCl, pH 6 and 1 mol/L KOH, pH 13) on Ca-bentonite. The 1 mol K concentration is comparable to 15 times the cation exchange capacity (CEC) of raw bentonite. Using various analytical techniques, the mineralogical, physicochemical, swelling, and Cs adsorption characteristics of raw and reacted bentonite samples were determined. Almost no changes in the properties of bentonite reacted with DI water were found for a given reaction time. For bentonite reacted with a 1 mol/L KCl solution, the cation exchange of Ca by K was a primary alteration process, resulting in a slight decrease in swelling capacity. However, almost no mineralogical changes were observed and consequently, there was minimal change in the Cs adsorption capacity. In contrast, for the bentonite reacted with a 1 mol/L KOH solution, the dominant alteration process was the transformation of minerals in bentonite into zeolite minerals, which resulted in significant changes in physicochemical properties, in particular, a decrease in the swelling capacity. On the other hand, the Cs adsorption capacity increased up to 2 times compared with the raw bentonite. • Ca-bentonite were reacted with concentrated solutions containing K+ ions with different pHs at 150 °C for 30–150 days. • Almost no changes in properties of bentonite reacted with deionized water were found. • 1 mol/L KCl solution led to an exchange of Ca by K, but caused almost no changes in mineralogy and Cs sorption capacity. • 1 mol/L KOH solution led to formation of zeolite minerals and a decrease in swelling capacity, but an increase in Cs sorption capacity. [ABSTRACT FROM AUTHOR]

[Display omitted] • Nitric acid oxidation promotes moderate dissociation of petroleum pitch. • Preparation Multi cavity Carbon Microsheets by using NaCl and Modified pitch. • Multi cavity carbon microsheets have excellent NO 3 – removal performance of CDI. • DFT calculations indicate carbon cavity is beneficial for NO 3 – electron enrichment. Capacities deionization (CDI) denitrification technology has attracted considerable attention, and electrode materials with nitrate adsorption properties have become a research hotspot. In this study, a multi cavity carbon microsheets (MCCM-5) was prepared using a hard template method and low-cost nitrated pitch as a carbon source. The results of the electrosorption experiments showed that the material had an excellent capacity of NaNO 3 (45 mg g−1). Furthermore, although the actual specific surface area and specific capacitance of MCCM-5 are lower than those of hierarchical porous carbon materials (HPCM-1), MCCM-5 exhibit lower diffusion and charge-transfer resistances, resulting in a better denitrification performance. The adsorption capacity of MCCM-5 for NaNO 3 was twice that HPCM-1 and 11.8 times that of commercial activated carbon, which is superior to the material properties reported thus far. Our analysis indicated that the material combined the advantages of both a layered structure and hierarchical pores. First, the uniformly distributed hierarchical pores in the layered structure enhanced the ion concentration potential. Second, the layered structure provided good ion diffusion channels, thereby increasing the effective adsorption area of the material. DFT calculation shows that the carbon cavity structure enriched in the material shows a stronger adsorption capacity for NO 3 –, which can promote the electron transfer process during NO 3 – adsorption. This study shows that a precise regulation of the carbon material structure can be achieved by adjusting the size of the template material and carbonization conditions to obtain a higher adsorption capacity and provides a new idea for the structural optimization of electrode materials. [ABSTRACT FROM AUTHOR]

With the continuous development of society, industrialization, and human activities have been producing more and more pollutants. Fluoride discharge is one of the main causes of water pollution. This review summarizes various commonly used and effective fluoride removal technologies, including ion exchange technology, electrochemical technology, coagulation technology, membrane treatment, and adsorption technology, and points out the outstanding advantages of adsorption technology. Various commonly used fluoride removal techniques as well as typical adsorbent materials have been discussed in published papers, however, the relationship between different adsorbent materials and adsorption models has rarely been explored, therefore, this paper categorizes and summarizes the various models involved in static adsorption, dynamic adsorption, and electrosorption fluoride removal processes, such as pseudo-first-order and pseudo-second-order kinetic models, Langmuir and Freundlich isotherm models, Thomas and Clark dynamic adsorption models, including the mathematical equations of the corresponding models and the significance of the models are also comprehensively summarized. Furthermore, this comprehensive discussion delves into the fundamental adsorption mechanisms, quantification of maximum adsorption capacity, evaluation of resistance to anion interference, and assessment of adsorption regeneration performance exhibited by diverse adsorption materials. The selection of the best adsorption model not only predicts the adsorption performance of the adsorbent but also provides a better description and understanding of the details of each part of the adsorption process, which facilitates the adjustment of experimental conditions to optimize the adsorption process. This review may provide some guidance for the development of more cost-effective adsorbent materials and adsorption processes in the future. [Display omitted] • Overview of commonly used effective fluoride removal technologies. • The various models involved in different fluoride removal modes by adsorption are classified and summarized. • Combining models to describe the adsorption process and mechanism of different materials. • The adsorption capacity, anion resistance, and adsorption regeneration performance of different materials are discussed. [ABSTRACT FROM AUTHOR]

Transition metal oxides (TMOs) have great application potential in capacitive deionization (CDI), which can selectively extract ions from water with high charge efficiency and low contamination. Previous studies have found that cationic segregation of TMOs has adverse effects on their electrochemical performance, but its effect on CDI remains unclear. Herein, we demonstrate for the first time that Ca2+ segregation provides more sites for F− adsorption by synthesizing Ca 2 Mn 3 O 8 for CDI selective defluorination. The Ca 2 Mn 3 O 8 material has a graded porous structure, low charge transfer resistance, high specific capacitance (255.64 F/g, 1 mV/s, 0.5 M NaF solution) and good charge/discharge reversibility (about 100 % charge specific capacity retention after 50 cycles). Moreover, Ca 2 Mn 3 O 8 has a high specific adsorption capacity (SAC) for NaF (1419.07 μmol/g) and excellent cyclic stability (capacity retention rate is 96.69 % after 100 cycles). The Ca2+ segregation from lattice to surface provides more sites for F− adsorption and greatly shortens ion transport paths. Density functional theory (DFT) calculation further suggests that the adsorption energy of Ca 2 Mn 3 O 8 for F− is much greater than that of Cl−. As a result, the removal rate of F− by Ca 2 Mn 3 O 8 in mixed solutions is up to 20 times higher than that of Cl−. [Display omitted] • It is proved that cationic segregation on the surface provides additional sites for ion adsorption. • Ca 2 Mn 3 O 8 electrode delivers outstanding fluoride removal performance and cycle stability. • Ca 2 Mn 3 O 8 electrode is much more selective for F− than for Cl−. [ABSTRACT FROM AUTHOR]

[Display omitted] • Divergent/convergent CDI cells are established and compared with straight ones. • The spacer geometry shifts the location of the initial adsorption and the depletion zone. • The channel slope mainly affects the desalination output rate. • Convergent channels show a faster ASAR than the regular straight geometry. • Steeper slopes give larger benefits. This research aims to explore the impact of tilted channel configurations of CDI cells on desalination performance. The results reveal that the titled convergent channels have a faster average salt adsorption rate (ASAR) than the regular straight geometry. For desalination operations that end at a quarter of the equilibrium salt adsorption capacity (SAC), the convergent spacer with a slight slope of 1.5 degrees has a 20 % higher ASAR than the typical straight geometry (0.15 mg/g/min for convergent and 0.12 mg/g/min for straight). This gain increases to about 24, 29.5, and 33%, respectively, for slopes of 3.5, 5.5, and 7 degrees, compared to the straight geometry with the same spacer thickness. By looking at the underlying mechanisms, the spacer geometry is found to shift the location of the initial adsorption. This affects how quickly the device outputs the cleaned water. Interestingly, the geometry angle can also affect the location of the depletion zone, so tilted spacers can also affect the behavior during electrode starvation. Specifically, the convergent geometry has the depletion zone in the middle of the electrode instead of the corner near the outlet, as seen for straight and divergent channels. Together, these findings indicate how to construct tilted spacers to enhance CDI performance. [ABSTRACT FROM AUTHOR]

[Display omitted] • Charging time plays a decisive role in CDI performance improvement. • UQ analysis quantitively provides guidance for CDI optimization. • The pore distribution and connectivity are highlighted. Capacitive deionization (CDI) is considered to be one of the most promising technologies to deionize water with low/medium concentration. Great attention has been paid to improve its performance by optimizing electrode architectures and operation conditions. However, no guidelines are built for developing such strategies due to the nonlinear impact of the parameters concerning electrodes and operations. Therefore, our work quantitatively reveals the influence of some key parameters involving electrode characteristics, operation conditions and ion properties using the statistical analysis based on uncertainty quantification. We find the porosity solely has a small influence on all the performance metrics. But the pore might play a significant role by the pore size distribution and connectivity that greatly determine the effective diffusion coefficient of salt ions. The high diffusion coefficient obviously raises the salt adsorption by facilitating ion transport, which also reduces the energy consumption while most of the consumed energy could even be recovered. The current exerts an opposite influence by shortening the charging period in the constant current (CC) mode. The salt concentration in the inflow water increases the adsorption capacity but decreases the removal efficiency. The decreased removal efficiency requires less external energy, enabling the usage of CDI as an economic pre-treatment unit. We highlight the ion transport resistance and its influence on CDI performance by acting upon charging time in the CC mode. We also suggest the application of the constant voltage mode to the low-salinity wastewater instead of the CC mode due to the high resistance. Our work addressed the importance of proper electrode and operation condition for high desalination performance and energy efficiency. [ABSTRACT FROM AUTHOR]

In the present work, a novel, floral-like, magnetic sodalite microsphere (SODM) was synthesized in situ by using fly ash (FA) and metakaolin (MK) as raw materials and was used to remove Cd(II) from water. Its magnetism can solve the problems of adsorbent recovery and possible secondary pollution. During the static adsorption, SODM shows a maximum adsorption capacity of 245.17 mg/g. The adsorption of Cd(II) on the SODM surface is spontaneous, exothermic, and physicochemical adsorption, which was evaluated by thermodynamics, kinetics, and isotherm studies. During dynamic adsorption, SODM shows a maximum adsorption capacity of 342.74 mg/g in the simulated solution prepared by the deionized water, compared to 215.88 mg/g in the simulated solution prepared using Xiangsi Lake water from Guangxi Minzu University. At 0.5 g SODM dosage in the dynamic adsorption, the adsorption capacity could rise to 632.81 mg/g. These results demonstrated the excellent Cd (II) adsorption performance of the SODM. The adsorption of cadmium on the SODM surface includes the synergistic effects of electrostatic attraction, ion exchange, and surface coordination reaction. Besides, the SODM shows good regeneration performance in both the deionized water and Xiangsi Lake water. The present study explores SODM as an adsorbent for the Cd (II) removal from wastewater and unbolts the industrial applicability of the SODM in the field of wastewater purification. [Display omitted] • The sodalite zeolite synthesized in situ by adjusting the content ratio of fly ash to metakaolin. • The SODM which contained low-cost raw materials exhibits magnetism and a flower-like morphology. • The adsorption capacities were 245.17 and 342.72～632.81 mg/g in the static, dynamic adsorption respectively. • The adsorption mechanisms included ion exchange, electrostatic interaction and surface coordination. • After 5 cycles, SODM has good regeneration performance in both lake water and deionized water. [ABSTRACT FROM AUTHOR]

[Display omitted] • EDTA grafted MXene was designed and fabricated as CDI electrode for treating simulant nuclear wastewater. • EDTA grafted MXene demonstrates high selectivity of Cs+ from concentrated HNO 3 solutions. • Cs+ can be concentrated to form an enriched waste stream that can be further utilized or disposed as a small waste package. • Stripping of adsorbed Cs+ by simple reverse of applied voltage led to easy regeneration with outstanding performance over 320 cycles. A capacitive deionization (CDI) electrode comprising ethylenediamine triacetic acid (EDTA) and 2D MXene (EDTA-MXene) is fabricated to separate Cs+ from strongly acidic process water. The method provides new direction for an advanced aqueous recycle process to separate fission products from spent fuel liquor. Grafting EDTA on MXene has no detrimental effect on its structure but does diversify the modes of ion interaction and increase the number of binding sites. The composite CDI electrode has a Cs+ adsorption capacity of 2.07 mmol g−1 at 1.2 V with 97.3% removal efficiency within 15 min. Step-wise adsorption and desorption cycling of the electrode highlights the chemisorption effect of EDTA which immobilizes the ions as the applied voltage is lowered, although almost all ions can be stripped by reversing the voltage to −1.4 V and without the need for chemical treatment. The EDTA-MXene electrode demonstrates outstanding cyclic performance with a capacity retention of >80% after 320 cycles. Furthermore, the electrode maintains its performance in strongly acidic solution, removing 0.66 mmol g−1 Cs+ at 1.2 V, as well as being stable after immersing in 3 mol L−1 HNO 3 for 7 days. Through continuous cycling it is possible to enrich the Cs+ into a highly concentrated solution for element recovery or safe disposal. The EDTA-MXene material is robust and maintains good performance in harsh chemical environments, levering its multiple binding sites to successfully isolate Cs+ from strongly acidic solutions and in the presence of competing ions, Sr2+ and Ce(IV). [ABSTRACT FROM AUTHOR]

Polysaccharide-based hydrogel adsorbents become popular because of their high adsorption capacity and fast adsorption rate, but their low removal rate and poor pH resistance have always been fatal shortcomings. Herein, a feasible strategy was proposed to strengthen the ability of hydrogel adsorbent to remove organic pollutants (i.e., dye) by incorporating natural rectorite (REC) into chitosan- g -poly (2-acrylamido-2-methyl-propane-sulfonic-acid) hydrogel network to form a rectorite-in-polymer network structure. The introduction of less dosage of REC (1.2 wt%) into the hydrogel facilitates to improve its adsorption capacities toward methylene blue (MB) in deionized water, tap water, seawater, Yangtze River water, and Yellow River water (1083.39–1303.49 mg/g); while incorporating higher content of REC (15.8 wt% REC) helps to improve the removal rate (99.6% for MB in real waters), which are greatly superior to commercial activated carbons. The adsorbent keeps high adsorption efficiency in a broad pH range (2–11), and can be reused for >4 times. [Display omitted] • Synthesized chitosan-based hydrogel has a rectorite-in-polymer composite network. • The hydrogel shows high adsorption capacity (1303.49 mg/g) and removal rate (99.6 %). • Removal efficiency keeps high in real waters (Yangtze River, Yellow River, seawater). • The hydrogel's adsorption capacity far exceeds that of commercial activated carbon. • This method is universal to enhance the removal efficiency of hydrogel adsorbent. [ABSTRACT FROM AUTHOR]

• Novel MoSe 2 /MCHS composite with unique 2D/3D interconnected structure was synthesized. • The MoSe 2 /MCHS electrode exhibited excellent HCDI water desalination performance. • Excellent performance came from synergy of intercalation pseudocapacitance and EDLC. • The MoSe 2 /MCHS electrode exhibited great recyclability and low energy consumption. Transition-metal dichalcogenides can be used for capacitive deionization (CDI) via pseudocapacitive ion intercalation/de-intercalation due to their unique two-dimensional (2D) laminar structure. MoS 2 has been extensively studied in the hybrid capacitive deionization (HCDI), but the desalination performance of MoS 2 -based electrodes remains only 20–35 mg g−1 on average. Benefiting from the higher conductivity and larger layer spacing of MoSe 2 than MoS 2 , it is expected that MoSe 2 would exhibit a superior HCDI desalination performance. Herein, for the first time, we explored the use of MoSe 2 in HCDI and synthesized a novel MoSe 2 /MCHS composite material by utilizing mesoporous carbon hollow spheres (MCHS) as the growth substrate to inhibit the aggregation and improve the conductivity of MoSe 2. The as-obtained MoSe 2 /MCHS presented unique 2D/3D interconnected architectures, allowing for synergistic effects of intercalation pseudocapacitance and electrical double layer capacitance (EDLC). An excellent salt adsorption capacity of 45.25 mg g−1 and a high salt removal rate of 7.75 mg g−1 min−1 were achieved in 500 mg L−1 NaCl feed solution at an applied voltage of 1.2 V in batch-mode tests. Moreover, the MoSe 2 /MCHS electrode exhibited outstanding cycling performance and low energy consumption, making it suitable for practical applications. This work demonstrates the promising application of selenides in CDI and provides new insights for ration design of high-performance composite electrode materials. [Display omitted] [ABSTRACT FROM AUTHOR]

As an indispensable element in the field of nuclear energy, uranium (U (VI)) is widely concerned because it is abundant and easy to obtain from seawater. Herein, we report a promising dual-template strategy to prepare heteroatom-doped carbon materials with hierarchical micro−/ meso −/macroporous from low-cost biomass precursors. The carbon materials with hierarchical porosity nitrogen/oxygen are synthesized through freeze-drying, high-temperature thermal treatment and subsequent HF etching treatment by in-situ growth of SiO 2 on the precursor with ethyl silicate as silicon source and introduction of ZnCl 2 as hard template and starch/ammonia as carbon and nitrogen source. Based on the advantages of three-dimensional interconnected hierarchical porous heteroatom doping, the electrosorption capacity reaches 67.25 mg/g, and the removal efficiency is as high as 98.45%, when the initial UO 2 (NO 3) 2 concentration is 80 mg/L in capacitive deionization. The isothermal adsorption of nitrogen doped hierarchical porous carbon (NHPC) is consistent with the Langmuir model, with a maximum electrosorption capacity of 152.43 mg/g, good cycle stability and high charge efficiency (energy consumption is only 0.77 kg-U kWh−1). Fascinatingly, the initial UO 2 (NO 3) 2 concentration is 80 mg/L and it also has a high adsorption capacity in 3.5 wt% NaCl solution, and the U (VI) removal efficiency could reach 42.5% after 8 h of continuous adsorption, with high selectivity. The prepared adsorbent NHPC shows good selectivity for U (VI) in the solution of 11 metal ions co-existing, and the effective selectivity K d value of U (VI) is 1620.84 mL/g. Finally, X-ray photoelectron spectroscopy analysis reveals that in addition to Coulomb interaction and chelation during the adsorption process, there is also a synergistic effect of the conversion of U (VI) to UO 2 under electric drive to improve the adsorption capacity of U (VI). • Dual-template synthesis of biomass-derived hierarchical porous heteroatom-doped carbon materials. • The removal efficiency of the NHPC electrode for U (VI) in 3.5 wt% NaCl solution is 42.5%. • The synergistic effect between UO 2 2+ and NHPC through coulomb interaction and reduction reaction makes it selective for UO 2 2+. [ABSTRACT FROM AUTHOR]

Prussian blue analogue (PBA) as a typical Faraday electrode material has important application value in capacitive deionization (CDI) for its rigid open framework and unique ion storage properties. But poor electrical conductivity and deformation of crystal structure during the desalination process restrict its development. To enhance the stability of PBA and provide rapid charge transfer, a new composite hollow core-shell polyaniline-encapsuled Ni-Prussian blue analogue (H-NP@PANI) is constructed. Experiments illustrate that PANI formed an omnidirectional uniform and highly conductive layer on the crystal surface, which tremendously improved the electrochemical capacity of H-NP@PANI (242.24 F·g−1). In constant voltage mode, the adsorption capacity of AC║H-NP@PANI cell is 35.86 mg·g−1, which was the highest to H-NP (20.82 mg·g−1) and pure Ni-PBA (16.08 mg·g−1). The retention rate remains 96.1 % after 50 cycles. XRD tests show that superior cycle stability is due to the hollow structure and buffer space provided by PANI shell, which can effectively inhibit the degree of crystal transformation. Furthermore, DFT calculation confirms the existence of a highly stable tight electron coupling between H-NP and PANI, and the electron aggregation center around Fe atom facilitates the Fe3+/Fe2+ redox cycle. Hence, this work can provide a feasible strategy for designing stable and efficient electrodes. [Display omitted] • Hollow core-shell PANI-encapsuled Ni-PBA (H-NP@PANI) with omni-directional conductive layer was constructed. • H-NP@PANI electrode showed superior electrochemical performance with high specific capacity of 242.24 F·g-1. • H-NP@PANI electrode had remarkable desalination performance of 35.86 mg·g-1 with superior desalination cycle stability. • Both DFT calculation and experimental analysis revealed the synergistic effect between PANI shell and H-NP in CDI process. [ABSTRACT FROM AUTHOR]

[Display omitted] • A low-carbon strategy was proposed for discarded mask recycling. • High Cr(VI) removal (358.68 mg g−1) was achieved using low-cost CPM/PDA/PPy. • Excellent desalination performance was obtained via capacitive deionization. • It has shown excellent reusability in Cr(VI) adsorption and desalination. The global mask consumption has been exacerbated because of the coronavirus disease 2019 (COVID-19) pandemic. Simultaneously, the traditional mask disposal methods (incineration and landfill) have caused serious environmental pollution and waste of resources. Herein, a simple and green mass-production method has been proposed to recycle carbon protective mask (CPM) into the carbon protective mask/polydopamine/polypyrrole (CPM/PDA/PPy) composite by in situ polymerization of PPy. The CPM/PDA/PPy composite was used for the removal of Cr(VI) and salt ions to produce clean water. The synergistic effect of PPy and the CPM improved the removal capability of Cr(VI). The CPM/PDA/PPy composite provided high adsorption capacity (358.68 mg g−1) and economic value (811.42 mg $−1). Consequently, the CPM/PDA/PPy (cathode) was combined with MnO 2 (anode) for desalination in CDI cells, demonstrated excellent desalination capacity (26.65 mg g−1) and ultrafast salt adsorption rate (6.96 mg g−1 min−1), which was higher than conventional CDI cells. Our work proposes a new low-carbon strategy to recycle discarded masks and demonstrates their utilization in Cr(VI) removal and seawater desalination. [ABSTRACT FROM AUTHOR]

Polyethersulfone (PES) is a widely used polymer for ultrafiltration (UF) membrane fabrication. In the current study, carbide-derived carbon (CDC) oxidized by acid treatment was utilized as a filler to fabricate a novel PES composites UF membranes. The successful oxidation of CDC was validated from presence of oxygen containing functional groups and improved oxygen content, from 5.08 at.% for CDC to 26.22 at.% for oxidized CDC (OCDC). The OCDC PES UF membranes were prepared at different loadings of OCDC between 0.5 and 3.0 wt%. The membrane porosity, pore size and surface free energy found to be improved while a noticeable reduction in water contact angle was observed with OCDC loading implying the improved hydrophilicity of PES membranes. Consequently, the pure water flux found to improve from 151.6 to 569.6 (L/(m2. h)) for the 3.0 wt% modified OCDC membrane (M−3) which is 3.8 folds of the bare PES membrane. The antifouling characteristics were evaluated by humic acid (HA) filtration. The results revealed a significant enhancement in HA rejection with OCDC loading, the highest rejection was 96.8% for M−3 membrane. Additionally, the adsorption capacity of OCDC modified membranes found to decrease with OCDC loading indicating improved rejection of HA from the membrane surface. Moreover, M−3 demonstrated the maximum flux recovery ratio (FRR) of 92.3%. Reusability of the fabricated membranes was evaluated by deionized water/humic acid cycling filtration. The FRR was higher than 86.7% over three cycles of pure water/HA filtration for 140 min, indicated the excellent stability and reusability of the membranes. Overall, the OCDC was an effective filler for enhancing the PES UF membranes antifouling and permeability properties. [Display omitted] • Oxidized carbide-derived carbon (OCDC) was synthesized by acid treatment. • PES UF membrane porosity, contact angle and hydrophilicity were improved with OCDC addition. • Humic acid rejection and antifouling properties were improved with OCDC loading. • Long term filtration experiments of pure water and humic acid were considered. • The OCDC found to be an effective and compatible filler for PES UF membranes. [ABSTRACT FROM AUTHOR]

Fluorine pollution has been recognized as one of the major problems of global concern. Metal-organic frameworks (MOFs), as potential fluoride adsorbents, possess unique chemical reactivity and broad functionalities. However, their application is restricted by instability in fluoride or acid/base solution and difficult separation. Here, lotus flower-like Al/N-doped porous carbon composite was prepared by a simple pyrolysis method using Al-based MOF as a precursor and used for capacitive deionization (CDI) defluorination. Through pyrolysis, MOF-derived carbon not only obtained a larger specific surface area and N-rich structure, but also possessed multiple F− capture sites. These carbon substrate enabled the metal centers to be uniformly dispersed and contributed to enhanced electrical conductivity and chemical stability of electrode material. Through the CDI defluorination system, F− migrate rapidly with the aid of the electric field and was captured under the synergistic effect of metal sites and carbon substrate. According to the Langmuir isotherm, the maximum F− removal capacity was 76.28 mg g−1 at 1.2 V, and the adsorption kinetics followed pseudo-second-order model. The electroenhanced adsorption method exhibits high adsorption capacity and selectivity for F− due to combining the advantages of adsorbent adsorption and electrosorption, which already exceeds the capacities of most electrode material. [Display omitted] • MOF-derived Al/N-doped porous carbon composite (AlNC) is firstly proposed in Capacitive deionization defluorination. • The F− removal capacity reached 76.28 mg g-1 at 1.2 V. • Presented a possible mechanism for the elctrosorption of F- on AlNC. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) has been considered as the most promising and environmentally friendly electrical desalination technology owing to its low energy consumption and no secondary pollution. CDI is based on the principle of electric double layer for salt ion adsorption, but the existence of co-ions repulsion reduce the charge efficiency, leading to the low salt adsorption capacity. To prevent the intrinsic "co-ion effect" inside the porous carbon electrodes, membrane capacitive deionization (MCDI) by applying an ion-exchange membrane (IEM) to the surface of electrode is of increasing interest. However, MCDI brings various resistances, such as the internal and interface resistances of membrane, as well as the contact resistance between membrane and carbon electrode. More recently, by integrating "membrane" with carbon electrode without the introduction of free-standing IEM, integrated-MCDI has shown great merits to enhance counter-ion selectivity of electrode and decrease resistance, resulting in improving adsorption rate and reducing energy consumption. In this review, the preparation methods of innovative electrodes, the working mechanisms and performances of integrated-MCDIs, and the advanced advantages are summarized. It is hoped that this work will provide insight into integrated-MCDI and shed light on the future direction of water desalination based on CDI technology. [Display omitted] • Integrated-MCDI has been developed without using free-standing IEM on electrode. • Integrated-MCDI outperforms MCDI on energy consumption, cost, and kinetic rate. • Integrated-MCDI has the potential of anti-organic pollution and ion-selective removal. • Review summarized current status of integrated-MCDI for water desalination. • The mechanisms of integrated-MCDI with different fabrication methods are analyzed. [ABSTRACT FROM AUTHOR]

[Display omitted] • The universal low carbon mass loading was used in capacitive deionization (CDI) for efficient deionized (DI) water production. • Partial desalination performance weakened with increasing carbon mass loading. • CDI cells using YEC-8–5.81 as electrodes produced DI water with a low conductivity of 1.89 μS/cm. • Carbons with a suitable micro- meso pore distribution and high specific capacitance may be a better choice. • 82.2% DI water recovery was achieved under stopped flow (SF) discharge mode. High-purity deionized (DI) water can be widely used in high-end manufacturing fields, but its efficient and energy-saving production is a huge challenge. Here, simple carbon mass loading control was developed for efficient DI water production via advanced capacitive deionization (CDI). Supercapacitor carbon (YEC-8) electrodes with diverse mass loading of 2.50, 5.81, 12.63 and 24.72 mg/cm2 were prepared for desalination. As expected, YEC-8–2.50 acquired the optimal CDI performance. High mass loading of 12.63 and 24.72 mg/cm2 not only caused an overt property drop but also serious wasted materials. Competitively, YEC-8–5.81 achieved a similar volumetric adsorption capacity (VAC) to YEC-8–2.50 as well as made up for the lack of total mass of YEC-8–2.50 and the resultant solution conductivity was as low as 1.89 μS/cm (grade III DI water). This strategy has been successfully extended to other carbon materials and carbons with suitable micro- meso pore distribution and high specific capacitance may be a better choice. Besides, the reverse effect of acetylene black (AB) mass on desalination was verified. To gain a high water recovery (W R), stopped flow (SF) discharge was introduced and realized a high W R of 82.2 %. Meanwhile, cycling tests indicated its splendid cycling stability. This study provides a universal direction for using low mass loading strategy for efficient DI water production. [ABSTRACT FROM AUTHOR]

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]

[Display omitted] • Nitrogen-doped porous carbon is synthesized via a dual-salt template approach. • The carbon exhibits high ion adsorption capacity and ultrafast adsorption rate. • Ion adsorption proceeds via electrocapacitive and pseudocapacitive mechanisms. • The electrocapacitive mechanism plays a dominant role in the ion adsorption. Porous carbon materials hold tremendous potential for capacitive deionization (CDI). However, realizing high specific surface area (SSA), suitable pore size distribution, and hierarchical porosity in carbons with facile and sustainable techniques is still challenging. In this work, we prepare hierarchical porous carbons (HPCs) with high SSA, abundant pore structures, and N-self doping via a versatile and sustainable modified salt-template approach. The optimized electrode gives a high SSA of 1639.9 m2/g, a large pore volume (2.7 cm3/g), and hierarchical porous structures (micro-meso-macro pores). For applications, the symmetric CDI electrode assembly delivers a salt adsorption capacity (SAC) of up to 17.67 mg/g in a 500 mg/L NaCl at 1.2 V together with ultrafast salt adsorption kinetics. We systematically study their associated desalination mechanism by combining several electrochemical experiments with the in-situ Raman spectroscopy technique, which revealed that the total salt storage is from the synergistic effect of both electrical double-layer (EDL) storage and pseudocapacitive mechanisms, with the EDL storage being dominant. This work paves the way to design economical and eco-friendly porous carbon materials for high-performance CDI desalination. [ABSTRACT FROM AUTHOR]

Integration of membrane and nanomaterial is a forward-looking research orientation, which can effectively overcome the permeability-selectivity trade-off relationship and improve anti-fouling performance. However, the current combination methods usually suffer from defects due to the aggregation and embedding of nanomaterials, resulting in serious performance deterioration of membrane during continuous operation process. Herein, "graphdiyne-like" Tetrabromobisphenol A molecularly imprinted membranes with uniform and dense SiO 2 layer, namely TB-MIMs, are successfully prepared by delayed phase inversion method (DPIM). We found that the membrane prepared by DPIM exhibits both promoted pure water flux (405 L m−2 h−1) and enhanced adsorption capacity (83.476 mg g−1) by comparing with the membranes prepared by blending and grafting methods. The role of molecularly imprinting technique contributes to improving the selectivity of TB-MIMs toward TBBPA, leading to a high selectivity factor of 3.39, 3.27 and 3.05 for bisphenol A, paratert-butyl phenol and 4, 4'-dihydroxybiphenyl, respectively. Moreover, the flux of TB-MIMs is nearly recovered to an original level after washing the bovine serum albumin fouled membrane surface with deionized water. Notably, the TB-MIMs presents a high rejection rate for bovine serum albumin (94%), humic acid (92%) and alginic acid (91%) in natural water, indicating its bright actual application value. These superior performances highlight the advantage of DPIM strategy over traditional methods in terms of combination between membrane and nanomaterials. A "graphdiyne-like" molecularly imprinted membrane with high selectivity and lasting anti-fouling performance was first proposed and developed by delayed phase inversion method for selective recognition and separation of Tetrabromobisphenol A. [Display omitted] • A"graphdiyne-like" membrane was synthesized by delayed phase inversion method. • The SiO 2 sphere had a dense and uniform distribution on the membrane surface. • The TB-MIMs possessed a superior selectivity and water permeability. • A lasting anti-fouling stability was realized. [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) is an emerging technology in brackish water desalination. Several types of CDI electrodes have been fabricated and tested throughout the years and most, if not all, require hours of CDI performance testing to assess their capability. In this study, a model was created to predict the salt adsorption capacity of different carbon-based CDI electrodes. Random forest, a statistical classification method, was utilized in the making of the model. Based on the results, the generated models had high accuracy and precision in estimating the salt adsorption capacity, representing R2 values mostly over 0.9. Furthermore, feature importance analysis showed that specific capacitance at higher scan rates can reduce the performance of the model. Therefore, it is recommended that low scan rate specific capacitance be used in creating any kind of CDI model. This study also illustrated that a universal model is possible for CDI with a minor sacrifice in precision. Depending on the goal of the end user, individual and universal models can be used in the prediction of salt adsorption capacity of various CDI electrodes. • The SAC of different CDI electrodes was predicted by the RF model. • Carbon electrodes doped with heteroatom and metal/metal-heteroatom were examined. • Variable importance of operational condition and electrode property was explored. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ppy grafted CMC carbon aerogels are applied in CDI for the first time. • Ppy/CA-2 shows excellent electrochemical and electrosorption performance. • The salt adsorption capacity of Ppy/CA-2 reaches 34.03 mg g−1. • Ppy could capture Cl− via surface redox reaction during CDI. Capacitive deionization (CDI) has been identified as a prospective desalination technology. There has been increasing interest in the exploration of electrodes with high electrochemical properties and salt adsorption capacity. Here, polypyrrole (Ppy)/CA electrodes were prepared by grafting Ppy on carbon aerogel (CA) via in-situ polymerization and applied in CDI desalination. Compared with CA, the Ppy/CA samples display higher specific capacitance, lower charge transfer resistance as well as enhanced ion diffusion rate. Particularly, Ppy/CA shows enhanced pseudocapacitance generation and the synergistic effect of the diffusion-controlled dominating process and capacitive process by Ppy introduction, conducive to the desalination performance. The optimal Ppy/CA-2 CDI system exhibits high adsorption capacity (34.03 mg g−1 with 500 mg L−1 solution), fast salt adsorption rate (0.053 mg g−1 s−1 with 500 mg L−1 solution) together with reasonable long-term stability. The outstanding desalination performance is principally on account of the positively charged nitrogen atoms of Ppy could capture Cl− well through the surface redox reaction in CDI and the most positively charged nitrogen in Ppy/CA-2 contribute its best adsorption capacity. The simple preparation method, excellent electrochemical properties, outstanding adsorption performance, and good cycling stability render Ppy/CA-2 a potential CDI electrode material. [ABSTRACT FROM AUTHOR]