Low-electrode capacitive deionization(FCDI)is an emerging desalination technology with great potential for removal and/or recycling ions from a range of waters.However,it still suffers from inefficient charge transfer...Low-electrode capacitive deionization(FCDI)is an emerging desalination technology with great potential for removal and/or recycling ions from a range of waters.However,it still suffers from inefficient charge transfer and ion transport kinetics due to weak turbulence and low electric intensity in flow electrodes,both restricted by the current collectors.Herein,a new tip-array current collector(designated as T-CC)was developed to replace the conventional planar current collectors,which intensifies both the charge transfer and ion transport significantly.The effects of tip arrays on flow and electric fields were studied by both computational simulations and electrochemical impedance spectroscopy,which revealed the reduction of ion transport barrier,charge transport barrier and internal resistance.With the voltage increased from 1.0 to 1.5 and 2.0 V,the T-CC-based FCDI system(T-FCDI)exhibited average salt removal rates(ASRR)of 0.18,0.50,and 0.89μmol cm^(-2) min^(-1),respectively,which are 1.82,2.65,and 2.48 folds higher than that of the conventional serpentine current collectors,and 1.48,1.67,and 1.49 folds higher than that of the planar current collectors.Meanwhile,with the solid content in flow electrodes increased from 1 to 5 wt%,the ASRR for T-FCDI increased from 0.29 to 0.50μmol cm^(-2) min^(-1),which are 1.70 and 1.67 folds higher than that of the planar current collectors.Additionally,a salt removal efficiency of 99.89%was achieved with T-FCDI and the charge efficiency remained above 95%after 24 h of operation,thus showing its superior long-term stability.展开更多
Hybrid capacitive deionization(HCDI)shows promise for desalinating brackish and saline water by utilizing the pseudocapacitive properties of faradaic electrodes.Organic materials,with their low environmental impact an...Hybrid capacitive deionization(HCDI)shows promise for desalinating brackish and saline water by utilizing the pseudocapacitive properties of faradaic electrodes.Organic materials,with their low environmental impact and adaptable structures,are attractive for this application.However,their scarcity of active sites and tendency to dissolve in water-based solutions remain significant challenges.Herein,we synthesized a polynaphthalenequinoneimine(PCON)polymer with stable long-range ordered framework and rough three-dimensional floral surface morphology,along with high-density active sites provided by C=O and C=N functional groups,enabling efficient redox reactions and achieving a high Na^(+)capture capability.The synthesized PCON polymer showcases outstanding electroadsorption characteristics and notable structural robustness,attaining an impressive specific capacitance of 500.45 F g^(-1) at 1 A g^(-1) and maintaining 86.1%of its original capacitance following 5000 charge–discharge cycles.Benefiting from the superior pseudocapacitive properties of the PCON polymer,we have developed an HCDI system that not only exhibits exceptional salt removal capacity of 100.8 mg g^(-1) and a remarkable rapid average removal rate of 3.36 mg g^(-1) min-1 but also maintains 97%of its initial desalination capacity after 50 cycles,thereby distinguishing itself in the field of state-ofthe-art desalination technologies with its comprehensive performance that significantly surpasses reported organic capacitive deionization materials.Prospectively,the synthesis paradigm of the double active-sites PCON polymer may be extrapolated to other organic electrodes,heralding new avenues for the design of high-performance desalination systems.展开更多
Since conventional photocatalytic technology fails to achieve complete elimination of chlorophenol contaminants from aqueous environments,this study presents a synergistic photocatalysis-capacitive deionization(PC-CDI...Since conventional photocatalytic technology fails to achieve complete elimination of chlorophenol contaminants from aqueous environments,this study presents a synergistic photocatalysis-capacitive deionization(PC-CDI)system as an advanced solution for industrial chlorophenol wastewater remediation.The PC-CDI system,employing boron nitride/carbon nitride(BN/CN)heterojunction electrodes,demonstrates exceptional degradation performance toward chlorophenols.The high-surface-area porous BN/CN heterojunction facilitates electro-adsorption and charge carrier separation,thereby synergistically optimizing both photocatalytic(PC)and capacitive deionization(CDI)functionalities.Remarkably,the integrated system achieves a 2,4-DCP degradation efficiency of 97.15%and a 2,4,6-TCP degradation efficiency of 100%in 2 h.The CDI component enables spatial separation through the electro-adsorption of Cl^(-)ions at the anode,effectively mitigating their interference and suppressing chlorinated byproduct formation.Concurrently,the electro-adsorption of positively charged chlorophenol pollutants accelerates their diffusion to catalytic sites,promoting the reactive oxygen species(ROS)-driven degradation of chlorophenol pollutants.The PC-CDI system exhibits robust stability(>95%efficiency retention over five cycles)and broad applicability across various chlorophenol derivatives.By circumventing Cl^(-)-induced side reactions and inhibiting chlorine radical generation during photocatalysis,this strategy minimizes the environmental risks associated with chlorinated byproducts during chlorophenol wastewater treatment.These findings establish the PC-CDI system as a sustainable and eco-friendly technology for industrial wastewater treatment.展开更多
Flow-electrode capacitive deionization(FCDI)is a newly developed desalination technology with a high electrode loading for superior salt removal efficiency,even with high feed salinity.However,the improvement in FCDI ...Flow-electrode capacitive deionization(FCDI)is a newly developed desalination technology with a high electrode loading for superior salt removal efficiency,even with high feed salinity.However,the improvement in FCDI performance could be restricted by obstacles such as poor charge transfer in the electrode slurry and agglomeration of the electrode particles.Therefore,various FCDIelectrode materials have been studied to overcome these bottlenecks through various mechanisms.Herein,a minireview is conducted to summarize the relevant information and provide a comprehensive view of the progress in FCDI electrode materials.Flow-electrode materials can be classified into three main groups:carbon materials,metalbased materials,and carbon-metal composites.Carbonbased capacitive materials with outstanding conductivities can facilitate charge transfer in FCDI,whereas metal-based materials and carbon-metal composites with ion-intercalative behaviors exhibit high ion adsorption abilities.Additionally,carbon materials with surface function groups can enhance electrode dispersion and reach a high electrode loading by electrostatic repulsion,further upgrading the conductive network of FCDI.Moreover,magnetic carbon-metal composites can be easily separated,and the salt removal performance can be improved with magnetic fields.Different electrode materials exhibit disparate features during FCDI development.Thus,combining these materials to obtain FCDI electrodes with multiple functions may be reasonable,which could be a promising direction for FCDI research.展开更多
Chromium(Cr)is a common heavy metal that has severe impacts on the ecosystem and human health.Capacitive deionization(CDI)is an environment-friendly and energy-efficient electrochemical purification technology to remo...Chromium(Cr)is a common heavy metal that has severe impacts on the ecosystem and human health.Capacitive deionization(CDI)is an environment-friendly and energy-efficient electrochemical purification technology to remove Cr from polluted water.The performance of CDI systems relies primarily on the properties of electrodes.Carbon-nanotubes(CNTs)membranes are promising candidates in creating advanced CDI electrodes and processes.However,the low electrosorption capacity and high hydrophobicity of CNTs greatly impede their applications in water systems.In this study,we employ atomic layer deposition(ALD)to deposit TiO_(2) nanoparticulates on CNTs membranes for preparing electrodes with hydrophilicity.The TiO_(2)-deposited CNTs membranes display preferable electrosorption performance and reusability in CDI processes after only 20 ALD cycles deposition.The total Cr and Cr(VI)removal efficiencies are significantly improved to 92.1%and 93.3%,respectively.This work demonstrates that ALD is a highly controllable and simple method to produce advanced CDI electrodes,and broadens the application of metal oxide/carbon composites in the electrochemical processes.展开更多
Nitrogenization is an effective method for improving the capacitive deionization(CDI)performance of porous carbon materials.In particular,polymer organic frameworks with heteroatom doping,containing an ordered pore st...Nitrogenization is an effective method for improving the capacitive deionization(CDI)performance of porous carbon materials.In particular,polymer organic frameworks with heteroatom doping,containing an ordered pore structure and excellent electrochemical stability,are ideal precursors for carbon materials for high-performance CDI.In this study,a nitrogen-enriched micro-mesoporous carbon(NMC)electrode was fabricated by carbonizing a Schiff base network-1 at 500,600,and 700℃.Scanning electron microscopy,Fourier transform infrared spectroscopy,X-ray diffraction,N_(2) adsorption-desorption,the contact angle of water,cyclic voltammetry,and electrochemical impedance spectroscopy were used to characterize the morphological structure,wettability,Brunauer–Emmett–Teller surface areas,and electrochemical performance of the NMCs.The results showed that the NMC carbonized at 600℃ achieved the best specific capacitance(152.33 F/g),as well as a high electrosorption capacity(25.53 mg/g)because of its chemical composition(15.57%N)and surface area(312 m^(2)/g).These findings prove that NMC is viable as an electrode material for desalination by high-performance CDI applications.展开更多
Because of the low energy requirement and the environmentally safe byproducts, the capacitive deionization water desalination technology has attracted the attention of many researchers. The important requirements for ...Because of the low energy requirement and the environmentally safe byproducts, the capacitive deionization water desalination technology has attracted the attention of many researchers. The important requirements for electrode materials are good electrical conductivity, high surface area, good chemical stability and high specific capacitance. In this study, metallic nanoparticles that are encapsulated in a graphite shell(Cd doped Co/C NPs) are introduced as the new electrode material for the capacitive deionization process because they have higher specific capacitance than the pristine carbonaceous materials. Cd doped Co/C NPs perform better than graphene and the activated carbon. The introduced nanoparticles were synthesized using a simple sol gel technique. A typical sol gel composed of cadmium acetate, cobalt acetate and poly(vinyl alcohol)was prepared based on the polycondensation property of the acetates. The physiochemical characterizations that were used confirmed that the drying, grinding and calcination in an Ar atmosphere of the prepared gel produced the Cd doped Co nanoparticles, which were encapsulated in a thin graphite layer. Overall, the present study suggests a new method to effectively use the encapsulated bimetallic nanostructures in the capacitive deionization technology.展开更多
Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconduct...Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconductivity,commercial carbon fibers cloth demonstrates great potential as high-performance electrodes for ions storage.Despite this,its direct application on capacitive deionization is rarely reported in terms of limited pore structure and natural hydrophobicity.Herein,a powerful metal-organic framework-engaged structural regulation strategy is developed to boost the desalination properties of carbon fibers.The obtained porous carbon fibers features hierarchical porous structure and hydrophilic surface providing abundant ions-accessible sites,and continuous graphitized carbon core ensuring rapid electrons transport.The catalytic-etching mechanism involving oxidation of Co and subsequent carbonthermal reduction is proposed and highly relies on annealing temperature and holding time.When directly evaluated as a current collector-free capacitive deionization electrode,the porous carbon fibers demonstrates much superior desalination capability than pristine carbon fibers,and remarkable cyclic stability up to 20 h with negligible degeneration.Particularly,the PCF-1000 showcases the highest areal salt adsorption capacity of 0.037 mg cm^(−2) among carbon microfibers.Moreover,monolithic porous carbon fibers-carbon nanotubes with increased active sites and good structural integrity by in-situ growth of carbon nanotubes are further fabricated to enhance the desalination performance(0.051 mg cm^(−2)).This work demonstrates the great potential of carbon fibers in constructing high-efficient and robust monolithic electrode for capacitive deionization.展开更多
MXene materials have got great attention from researchers of environmental treatment for the great electrochemical performance.Monolayer-Ti_(3)C_(2)T_(x)(T_(x) is the surface terminal groups such as-O,-OH and/or-F spe...MXene materials have got great attention from researchers of environmental treatment for the great electrochemical performance.Monolayer-Ti_(3)C_(2)T_(x)(T_(x) is the surface terminal groups such as-O,-OH and/or-F species),as a typical structural MXene,always shows better chemical-physical characteristics than multilayer-Ti_(3)C_(2)T_(x).Thus,we prepared monolayer-Ti_(3)C_(2)T_(x) electrode by HF etching method and absolute ethyl alcohol intercalationdelamination treatment for capacitive deionization(CDI).The prepared monolay-Ti_(3)C_(2)T_(x) shows a higher specific surface area(235.6 m^(2)/g)and a thinner thickness(0.8 nm).Moreover,a series of systematic investigation demonstrated that monolayer-Ti_(3)C_(2)T_(x) has obvious promotional phenomenon on electrochemical properties(e.g.,mass specific capacitance increased from 52.1 F/g to 144.7 F/g).The NaCl adsorption capacity of monolayer-Ti_(3)C_(2)T_(x),is 30.7 mg/g in 1000 mg/L NaCl solution at 1.2 V.We concluded that the electro-sorption mechanism could be expressed as double electric layer and monolayer coverage by a good fitting of Langmuir isotherms and the pseudo-second-order kinetics equation.This work would provide a new strategy for the application of monolayer-Ti_(3)C_(2)T_(x) material in wastewater treatment in the future.展开更多
The“battery type”inorganic electrode has been demonstrated the highly efficient sodium ion intercalation capacity for capacitive deionization.In this work,the CoMn_(2)O_(4)(CMO)microspheres with porous core-shell st...The“battery type”inorganic electrode has been demonstrated the highly efficient sodium ion intercalation capacity for capacitive deionization.In this work,the CoMn_(2)O_(4)(CMO)microspheres with porous core-shell structure are prepared via co-precipitation and followed by annealing.The effects of annealing temperatures on the morphology,pore structure,valence state,and electrochemical behavior of CMO are explored.As electrode for capacitive deionization,the salt removal capacity and current efficiency of optimized AC||CMO device reaches up to 60.7 mg g^(−1) and 97.6%,respectively,and the capacity retention rate is 74.1%after 50 cycles.Remarkably,both the in-situ X-ray diffraction and ex-situ X-ray diffraction analysis features that the intercalation/de-intercalation of sodium ions are governed by(103)and(221)crystal planes of CMO.Accordingly,the density functional theory calculations realize that the adsorption energies of Na+onto(103)and(221)crystal planes are higher than that of any other crystal planes,manifesting the priorities in adsorption of sodium atoms.Furthermore,the X-ray photoelectron spectra of pristine and post-CMO electrode highlights that the reversible conversion of Mn^(3+)/Mn^(4+)couple is resulted from the intercalation/de-intercalation of Na^(+),while this is irreversible for Co^(3+)/Co^(2+)couple.Beyond that,the CMO electrode has been proven the selectivity removal of Na^(+) over K^(+)and Mg^(2+)in a multi-cation stream.展开更多
Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surf...Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surface area and mesoporous content than two other composite electrodes.Electrochemical analysis showed that D860/AC M presents higher specific capacitance and electrical double layer capacitor than the others,and significantly lower internal diffusion impedance.Thus,D860/AC M exhibits the highest adsorption capacity and rate of Ⅴ(Ⅳ)among three electrodes.The intra-particle diffusion model fits well in the initial adsorption stage,while the liquid film diffusion model is more suitable for fitting at the later stage.The pseudo-second-order kinetic model is suited for the entire adsorption process.The adsorption of Ⅴ(Ⅳ)on the composite electrode follows that of the Freundlich isotherm.Thermodynamic analysis indicates that the adsorption of Ⅴ(Ⅳ)is an exothermic process with entropy reduction,and the electric field force plays a dominant role in the CDI process.This work aims to improve our understanding of the ion adsorption behaviors and mechanisms on the composite electrodes in CDI.展开更多
Electrode materials with high desalination capacity and long-term cyclic stability are the focus of capacitive deionization(CDI) community. Understanding the causes of performance decay in traditional carbons is cruci...Electrode materials with high desalination capacity and long-term cyclic stability are the focus of capacitive deionization(CDI) community. Understanding the causes of performance decay in traditional carbons is crucial to design a high-performance material. Based on this, here, nitrogen-doped activated carbon(NAC) was prepared by pyrolyzing the blend of activated carbon powder(ACP) and melamine for the positive electrode of asymmetric CDI. By comparing the indicators changes such as conductivity, salt adsorption capacity, pH, and charge efficiency of the symmetrical ACP-ACP device to the asymmetric ACP-NAC device under different CDI cycles, as well as the changes of the electrochemical properties of anode and cathode materials after long-term operation, the reasons for the decline of the stability of the CDI performance were revealed. It was found that the carboxyl functional groups generated by the electro-oxidation of anode carbon materials make the anode zero-charge potential(E_(pzc)) shift positively,which results in the uneven distribution of potential windows of CDI units and affects the adsorption capacity. Furthermore, by understanding the electron density on C atoms surrounding the N atoms, we attribute the increased cyclic stability to the enhanced negativity of the charge of carbon atoms adjacent to quaternary-N and pyridinic-oxide-N.展开更多
Electrode materials with strong desalting ability is an important research direction of capacitive deionization.In this study,HKUST-1 was successfully synthesized by the solvothermal method,and MOFsderived porous carb...Electrode materials with strong desalting ability is an important research direction of capacitive deionization.In this study,HKUST-1 was successfully synthesized by the solvothermal method,and MOFsderived porous carbon/Cu@Cu_(2)O composites were prepared by simple pyrolysis as cathode materials for CDI.After high-temperature pyrolysis,the Cu^(+) site with unsaturated coordination is generated,and the structure changes from micropores to the coexistence of mesoporous and micropores.The complex pore structure is conducive to strengthening ion migration and diffusion.The results show that the porous carbon/Cu@Cu_(2)O materials derived from MOFs depend on the pseudocapacitance behavior for capacitive deionization and desalination.At a voltage window of-1.2V~1.2V,a current density of 40mA/g.and 5 mmol/L NaCl,the HDC-1100 exhibited the best desalting capacity of 30.9 mg/g.HDC-1100 also has good cycle stability.After 20 cycles of adsorption and desorption,the desalting capacity almost does not decrease.Therefore,MOFs derived porous carbon/Cu@Cu_(2)O composites are expected to be an excellent choice for CDI cathode materials.展开更多
Flow-electrode capacitive deionization(FCDI)represents a promising approach for ion separation from aqueous solutions.However,the optimization of spacer,particularly for nitrate-contaminated groundwa-ter systems,has o...Flow-electrode capacitive deionization(FCDI)represents a promising approach for ion separation from aqueous solutions.However,the optimization of spacer,particularly for nitrate-contaminated groundwa-ter systems,has often been overlooked.This research comprehensively investigates the influence of using a conductive(carbon cloth,CC)spacer on nitrate removal performance within FCDI system,comparing it to a non-conductive(nylon net,NN)spacer.In both CC and NN FCDI systems,it is unsurprisingly that nitrate removal efficiency improved notably with the increasing current density and hydraulic retention time(HRT).Interestingly,the specific energy consumption(SEC)for nitrate removal did not show obvious fluctuations when the current density and HRT varied in both systems.Under the auspiciously optimized process parameters,CC-FCDI attained a 20%superior nitrate removal efficiency relative to NN-FCDI,ac-companied by a notably diminished SEC for CC-FCDI,registering at a mere 28%of NN-FCDI.This great improvement can be primarily attributed to the decrement in FCDI internal resistance after using con-ductive spacer,which further confirmed by electrochemical tests such as linear sweep voltammetry(LSV)and electrochemical impedance spectroscopy(EIS).Upon prolonged continuous nitrate removal at the optimized conditions,the CC-FCDI system achieved a consistent 90%nitrate removal efficiency with a low SEC of 2.7-7.8 kWh/kg NO_(3)-N,underscoring its steady performance.Overall,this study highlights the pivotal importance of careful spacer design and optimization in realizing energy-efficient groundwater treatment via FCDI.展开更多
Water and energy shortages came due to rapid population growth, living standards and rapid development in the agriculture and industrial sectors. Desalination tends to be one of the most promising water solutions;howe...Water and energy shortages came due to rapid population growth, living standards and rapid development in the agriculture and industrial sectors. Desalination tends to be one of the most promising water solutions;however, it is a process of intense energy. Membrane Capacitive Deionization (MCDI) has received considerable interest as a promising desalination technology, and MCDI research has increased significantly over the last 10 years. In addition, there are no guidelines for the design of Capacitive Deionization (CDI) implementation strategies for individual applications. This study, therefore;provides an alternative of CDI’s recent application developments, with emphasis placed on hybrid systems to address the technological needs of different relevant fields. The MCDI’s energy consumption is compared with the reverse osmosis literature data based on experimental data from laboratory-scale system. The study demonstrates that MCDI technology is a promising technology in the next few years with an extreme competition in water recovery, energy consumption and salt removal for reverse osmosis.展开更多
Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacr...Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacrificial templates,which can afford Co^(2+)sources.After a facile solvothermal reaction and sequential cation etching,yolk-shell-structured layered double hydroxide@HMCSs(LDH@HMCSs)have been synthesized.The LDH@HMCSs nanocomposite possesses a three-dimensional(3D)hollow nanocage superstructure that effectively blocks the self-stacking of LDH nanosheets and promotes ion transport.Compared to CoFe-LDH@HMCSs,and Co-LDH@HMCSs,CoNi-LDH@HMCSs exhibit superior electrochemical performance and desalination performance due to the remarkable synergistic effect between the CoNi-LDH nanosheets and mesoporous N-doped carbon shells.The resultant CoNi-LDH@HMCSs-0.4-based capacitive deionization(CDI)device exhibits excellent salt adsorption capacity(SAC,36.41 mg·g^(-1))and good cycle stability.This work will confirm the significance of constructing superstructure and open new avenues for the practical application of CDI technology in water treatment.展开更多
Covalent organic frameworks(COFs)are highly regarded for their tunable pore structures,high specific surface areas,and functionalizable active sites,making them promising candidates for heavy metal removal through cap...Covalent organic frameworks(COFs)are highly regarded for their tunable pore structures,high specific surface areas,and functionalizable active sites,making them promising candidates for heavy metal removal through capacitive deionization(CDI).However,their application in CDI faces inherent challenges,such as low electrical conductivity and insufficient utilization of redox-active sites.To address these limitations,a high-performance COF-based electrode material was synthesized by integrating COFs with carbon nanotubes(CNTs)via in situ growth(COF@CNT).By optimizing the crystallinity,charge distribution,and accessibility of active sites in the COF@CNT framework,the resultant sulfonic acid-functionalized TpPa(Tp:1,3,5-triformylphloroglucinol and Pa:1,4-phenylenediamine)COF(S-TpPa@CNT)exhibited an exceptional Cd^(2+)adsorption capacity of 165.23 mg/g at 1.2 V with an initial concentration of 80 mg/L,representing state-of-the-art performance and the highest reported value among CDI electrodes.X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations revealed that the synergistic roles of sulfonic acid groups and theβ-ketoenamine structure within the COF framework regulated the charge distribution within the COF framework and created a lower binding energy state.These findings demonstrate the potential of functionalized COF@CNT composites as high-performance electrode materials for efficient and sustainable water purification,paving the way for next-generation CDI technologies.展开更多
Capacitive deionization(CDI)is a promising technology to satisfy the global need for fresh water,since it can be both economical and sustainable.While two-dimensional transition metal carbides/nitrides(MXenes)exhibit ...Capacitive deionization(CDI)is a promising technology to satisfy the global need for fresh water,since it can be both economical and sustainable.While two-dimensional transition metal carbides/nitrides(MXenes)exhibit great characteristics for use as CDI electrode materials,their tightly spaced layered structure renders intercalation inefficiency.In this study,the interlayer distance of MXenes is precisely modulated by inserting different quantity of one-dimensional bacterial fibers(BC),forming freestanding MXene/BC composite electrodes.Among the studied samples,MXene/BC-33%electrode with the interlayer spacing of 15.2Åcan achieve an optimized tradeoff among various desalination performance metrics and indicators.The salt adsorption capacity(SAC),the average salt adsorption rate(ASAR),the energy normalized adsorbed salt(ENAS),and the thermodynamic energy efficiency(TEE)of the MXene/BC-33%electrode are improved by 24%,46%,13%,and 66%respectively compared with those of pure MXene electrode.While the insertion of BC improves the ion diffusion pathways and facilitates the intercalation kinetics,the desalination performance decreases when the insertion amount of BC exceeds 40%.This is attributed to the overlarge resistance of the composite and the resulting increased energy consumption.This study reveals the desalination performance tradeoffs of MXene-based electrodes with different interlayer distances and also sheds light on the fundamental ion storage mechanisms of intercalation materials in a CDI desalination system.展开更多
Capacitive deionization(CDI)technology has been considered a promising desalination technique,especially for brackish water,because of its relatively low energy consumption,facile operation,and easy regeneration of el...Capacitive deionization(CDI)technology has been considered a promising desalination technique,especially for brackish water,because of its relatively low energy consumption,facile operation,and easy regeneration of electrodes.However,the desalination capacity,cost,fabrication method,electrochemical stability,and environmental unfriendliness of the electrodes have restricted the practical application of the CDI technique.Herein,we reported the one-step in situ preparation of nitrogen-doped and carbon-decorated MXene-derived TiO_(2)(termed N-TiO_(2−x)/C)through the confinement-growth strategy.The small particle size(∼25 nm)and uniform distribution of a peanut-like N-TiO_(2−x)/C material could be ascribed to the confined growth space created by the nanoporous structure of melamine foam.The defects produced by N doping provide an enhanced electrical conductivity and more adsorption sites,while wrapping with a carbon shell layer increases the conductivity and offers protection for N-TiO_(2−x) to achieve an excellent electrochemical stability.The prepared N-TiO_(2−x)/C electrode is hydrophilic due to the abundant oxygen-containing functional groups(e.g.,C-O,N-Ti-O,-NO_(x),and-OH)and exhibits a high salt removal capacity(33.4 mg·g^(−1)),desalination rate(1.5 mg·g^(−1)·min^(−1)),and remarkable cycling stability(without declining after 100 cycles),which might be ascribed to the synergistic effects of the short ion diffusion path,more active adsorption sites,enhanced conductivity,pseudocapacitive behavior,and protection of the carbon shell layer.This work provides a confined-growth strategy to develop MXene-derived oxide electrodes for electrochemical desalination.展开更多
The practical application of the capacitive deionization(CDI)enhanced ultrafiltration(CUF)technology is hampered due to low performance of electrodes.The current study demonstrated a novel super-aligned carbon nanotub...The practical application of the capacitive deionization(CDI)enhanced ultrafiltration(CUF)technology is hampered due to low performance of electrodes.The current study demonstrated a novel super-aligned carbon nanotube(SACNT)/activated carbon(AC)composite electrode,which was prepared through coating AC on a cross-stacked SACNT film.The desalination capability and water purification performance of the prepared electrode were systematically investigated at different applied voltages(0.8-1.2 V)with a CDI system and a CUF system,respectively.In the CDI tests,as compared with 5ie control AC electrode,the SACNT/AC electrode achieved an approximately 100%increase in both maximum salt adsorption capacity and average salt adsorption rate under all the applied voltage conditions,demonstrating a superior desalination capability.Meanwhile,a conspicuous increase by an average of-26%in charge efficiency was also achieved at all the voltages.In the CUF tests,as compared with the control run at 0 V,the treatment runs at 0.8,1.0,and 1.2 V achieved a 2.40-fold,2.08-fold,and 2.43-fold reduction in membrane fouling(calculated according to the final transmembrane pressure(TMP)data at the end of every purification stage),respectively.The average TMP increasing rates at 0.8,1.0,and 1.2 V were also roughly two times smaller than that at 0 V,indicating a dramatical reduction of membrane fouling.The SACNT/AC electrode also maintained its superior desalination capability in the CUF process,resulting in an overall improved water purification efficiency.展开更多
基金supported by the Shenzhen Science and Technology Program(JCYJ20230808105111022,JCYJ20220818095806013)Natural Science Foundation of Guangdong(2023A1515012267)+1 种基金the National Natural Science Foundation of China(22178223)the Royal Society/NSFC cost share program(IEC\NSFC\223372).
文摘Low-electrode capacitive deionization(FCDI)is an emerging desalination technology with great potential for removal and/or recycling ions from a range of waters.However,it still suffers from inefficient charge transfer and ion transport kinetics due to weak turbulence and low electric intensity in flow electrodes,both restricted by the current collectors.Herein,a new tip-array current collector(designated as T-CC)was developed to replace the conventional planar current collectors,which intensifies both the charge transfer and ion transport significantly.The effects of tip arrays on flow and electric fields were studied by both computational simulations and electrochemical impedance spectroscopy,which revealed the reduction of ion transport barrier,charge transport barrier and internal resistance.With the voltage increased from 1.0 to 1.5 and 2.0 V,the T-CC-based FCDI system(T-FCDI)exhibited average salt removal rates(ASRR)of 0.18,0.50,and 0.89μmol cm^(-2) min^(-1),respectively,which are 1.82,2.65,and 2.48 folds higher than that of the conventional serpentine current collectors,and 1.48,1.67,and 1.49 folds higher than that of the planar current collectors.Meanwhile,with the solid content in flow electrodes increased from 1 to 5 wt%,the ASRR for T-FCDI increased from 0.29 to 0.50μmol cm^(-2) min^(-1),which are 1.70 and 1.67 folds higher than that of the planar current collectors.Additionally,a salt removal efficiency of 99.89%was achieved with T-FCDI and the charge efficiency remained above 95%after 24 h of operation,thus showing its superior long-term stability.
基金supported by the National Key R&D Program of China(Grant Nos.2023YFC3009900)National Natural Science Foundation of China(Grant Nos.61904116)+1 种基金Natural Science Foundation of Jiangsu Province(Grant Nos.BK20211029)the young scientific talent lifting project of Jiangsu Association for Science and Technology(Grant Nos.JSTJ-2023-018).
文摘Hybrid capacitive deionization(HCDI)shows promise for desalinating brackish and saline water by utilizing the pseudocapacitive properties of faradaic electrodes.Organic materials,with their low environmental impact and adaptable structures,are attractive for this application.However,their scarcity of active sites and tendency to dissolve in water-based solutions remain significant challenges.Herein,we synthesized a polynaphthalenequinoneimine(PCON)polymer with stable long-range ordered framework and rough three-dimensional floral surface morphology,along with high-density active sites provided by C=O and C=N functional groups,enabling efficient redox reactions and achieving a high Na^(+)capture capability.The synthesized PCON polymer showcases outstanding electroadsorption characteristics and notable structural robustness,attaining an impressive specific capacitance of 500.45 F g^(-1) at 1 A g^(-1) and maintaining 86.1%of its original capacitance following 5000 charge–discharge cycles.Benefiting from the superior pseudocapacitive properties of the PCON polymer,we have developed an HCDI system that not only exhibits exceptional salt removal capacity of 100.8 mg g^(-1) and a remarkable rapid average removal rate of 3.36 mg g^(-1) min-1 but also maintains 97%of its initial desalination capacity after 50 cycles,thereby distinguishing itself in the field of state-ofthe-art desalination technologies with its comprehensive performance that significantly surpasses reported organic capacitive deionization materials.Prospectively,the synthesis paradigm of the double active-sites PCON polymer may be extrapolated to other organic electrodes,heralding new avenues for the design of high-performance desalination systems.
文摘Since conventional photocatalytic technology fails to achieve complete elimination of chlorophenol contaminants from aqueous environments,this study presents a synergistic photocatalysis-capacitive deionization(PC-CDI)system as an advanced solution for industrial chlorophenol wastewater remediation.The PC-CDI system,employing boron nitride/carbon nitride(BN/CN)heterojunction electrodes,demonstrates exceptional degradation performance toward chlorophenols.The high-surface-area porous BN/CN heterojunction facilitates electro-adsorption and charge carrier separation,thereby synergistically optimizing both photocatalytic(PC)and capacitive deionization(CDI)functionalities.Remarkably,the integrated system achieves a 2,4-DCP degradation efficiency of 97.15%and a 2,4,6-TCP degradation efficiency of 100%in 2 h.The CDI component enables spatial separation through the electro-adsorption of Cl^(-)ions at the anode,effectively mitigating their interference and suppressing chlorinated byproduct formation.Concurrently,the electro-adsorption of positively charged chlorophenol pollutants accelerates their diffusion to catalytic sites,promoting the reactive oxygen species(ROS)-driven degradation of chlorophenol pollutants.The PC-CDI system exhibits robust stability(>95%efficiency retention over five cycles)and broad applicability across various chlorophenol derivatives.By circumventing Cl^(-)-induced side reactions and inhibiting chlorine radical generation during photocatalysis,this strategy minimizes the environmental risks associated with chlorinated byproducts during chlorophenol wastewater treatment.These findings establish the PC-CDI system as a sustainable and eco-friendly technology for industrial wastewater treatment.
基金financially supported by the National Natural Science Foundation of China(No.52374423)the Science and Technology Innovation Program of Hunan Province(No.2021RC4010)the Science and Technology Major Project of Changsha(No.kh2401030)
文摘Flow-electrode capacitive deionization(FCDI)is a newly developed desalination technology with a high electrode loading for superior salt removal efficiency,even with high feed salinity.However,the improvement in FCDI performance could be restricted by obstacles such as poor charge transfer in the electrode slurry and agglomeration of the electrode particles.Therefore,various FCDIelectrode materials have been studied to overcome these bottlenecks through various mechanisms.Herein,a minireview is conducted to summarize the relevant information and provide a comprehensive view of the progress in FCDI electrode materials.Flow-electrode materials can be classified into three main groups:carbon materials,metalbased materials,and carbon-metal composites.Carbonbased capacitive materials with outstanding conductivities can facilitate charge transfer in FCDI,whereas metal-based materials and carbon-metal composites with ion-intercalative behaviors exhibit high ion adsorption abilities.Additionally,carbon materials with surface function groups can enhance electrode dispersion and reach a high electrode loading by electrostatic repulsion,further upgrading the conductive network of FCDI.Moreover,magnetic carbon-metal composites can be easily separated,and the salt removal performance can be improved with magnetic fields.Different electrode materials exhibit disparate features during FCDI development.Thus,combining these materials to obtain FCDI electrodes with multiple functions may be reasonable,which could be a promising direction for FCDI research.
基金Financial supports from the Jiangsu Natural Science Foundation(BK20190677)National Natural Science Foundation of China(21908096)+2 种基金Scientific Research Foundation of Chuzhou University(2020qd06)support from the Program of Excellent Innovation Teams of Jiangsu Higher Education Institutionsthe Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Chromium(Cr)is a common heavy metal that has severe impacts on the ecosystem and human health.Capacitive deionization(CDI)is an environment-friendly and energy-efficient electrochemical purification technology to remove Cr from polluted water.The performance of CDI systems relies primarily on the properties of electrodes.Carbon-nanotubes(CNTs)membranes are promising candidates in creating advanced CDI electrodes and processes.However,the low electrosorption capacity and high hydrophobicity of CNTs greatly impede their applications in water systems.In this study,we employ atomic layer deposition(ALD)to deposit TiO_(2) nanoparticulates on CNTs membranes for preparing electrodes with hydrophilicity.The TiO_(2)-deposited CNTs membranes display preferable electrosorption performance and reusability in CDI processes after only 20 ALD cycles deposition.The total Cr and Cr(VI)removal efficiencies are significantly improved to 92.1%and 93.3%,respectively.This work demonstrates that ALD is a highly controllable and simple method to produce advanced CDI electrodes,and broadens the application of metal oxide/carbon composites in the electrochemical processes.
基金supported by the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the National Natural Science Foundation of China(No.21577027)the 2017 Central Special Fund for Soil,Preliminary Study on Harmless Treatment and Comprehensive Utilization of Tailings in Dabao Mountain(No.18HK0108)。
文摘Nitrogenization is an effective method for improving the capacitive deionization(CDI)performance of porous carbon materials.In particular,polymer organic frameworks with heteroatom doping,containing an ordered pore structure and excellent electrochemical stability,are ideal precursors for carbon materials for high-performance CDI.In this study,a nitrogen-enriched micro-mesoporous carbon(NMC)electrode was fabricated by carbonizing a Schiff base network-1 at 500,600,and 700℃.Scanning electron microscopy,Fourier transform infrared spectroscopy,X-ray diffraction,N_(2) adsorption-desorption,the contact angle of water,cyclic voltammetry,and electrochemical impedance spectroscopy were used to characterize the morphological structure,wettability,Brunauer–Emmett–Teller surface areas,and electrochemical performance of the NMCs.The results showed that the NMC carbonized at 600℃ achieved the best specific capacitance(152.33 F/g),as well as a high electrosorption capacity(25.53 mg/g)because of its chemical composition(15.57%N)and surface area(312 m^(2)/g).These findings prove that NMC is viable as an electrode material for desalination by high-performance CDI applications.
基金financially supported by the National Plan for Science & Technology (NPST), King Saud University Project No. 11-NAN1460-02
文摘Because of the low energy requirement and the environmentally safe byproducts, the capacitive deionization water desalination technology has attracted the attention of many researchers. The important requirements for electrode materials are good electrical conductivity, high surface area, good chemical stability and high specific capacitance. In this study, metallic nanoparticles that are encapsulated in a graphite shell(Cd doped Co/C NPs) are introduced as the new electrode material for the capacitive deionization process because they have higher specific capacitance than the pristine carbonaceous materials. Cd doped Co/C NPs perform better than graphene and the activated carbon. The introduced nanoparticles were synthesized using a simple sol gel technique. A typical sol gel composed of cadmium acetate, cobalt acetate and poly(vinyl alcohol)was prepared based on the polycondensation property of the acetates. The physiochemical characterizations that were used confirmed that the drying, grinding and calcination in an Ar atmosphere of the prepared gel produced the Cd doped Co nanoparticles, which were encapsulated in a thin graphite layer. Overall, the present study suggests a new method to effectively use the encapsulated bimetallic nanostructures in the capacitive deionization technology.
基金We gratefully acknowledge financial supports from the Natural Science Founda-tion of Shandong Province (No.ZR2020QE066)Taishan Scholar Project (No.ts201511080)+1 种基金the fellowship of China Postdoctoral Science Foundation (No.2020M672081)Opening Project of State Key Laboratory of Advanced Tech-nology for Float Glass (No.2020KF08).
文摘Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconductivity,commercial carbon fibers cloth demonstrates great potential as high-performance electrodes for ions storage.Despite this,its direct application on capacitive deionization is rarely reported in terms of limited pore structure and natural hydrophobicity.Herein,a powerful metal-organic framework-engaged structural regulation strategy is developed to boost the desalination properties of carbon fibers.The obtained porous carbon fibers features hierarchical porous structure and hydrophilic surface providing abundant ions-accessible sites,and continuous graphitized carbon core ensuring rapid electrons transport.The catalytic-etching mechanism involving oxidation of Co and subsequent carbonthermal reduction is proposed and highly relies on annealing temperature and holding time.When directly evaluated as a current collector-free capacitive deionization electrode,the porous carbon fibers demonstrates much superior desalination capability than pristine carbon fibers,and remarkable cyclic stability up to 20 h with negligible degeneration.Particularly,the PCF-1000 showcases the highest areal salt adsorption capacity of 0.037 mg cm^(−2) among carbon microfibers.Moreover,monolithic porous carbon fibers-carbon nanotubes with increased active sites and good structural integrity by in-situ growth of carbon nanotubes are further fabricated to enhance the desalination performance(0.051 mg cm^(−2)).This work demonstrates the great potential of carbon fibers in constructing high-efficient and robust monolithic electrode for capacitive deionization.
基金Project(2018YFC1900300)supported by the National Key R&D Program of ChinaProject(51825403)supported by the National Science Fund for Distinguished Young Scholars,ChinaProject(2018SK2026)supported by the Key R&D Program of Hunan Province,China。
文摘MXene materials have got great attention from researchers of environmental treatment for the great electrochemical performance.Monolayer-Ti_(3)C_(2)T_(x)(T_(x) is the surface terminal groups such as-O,-OH and/or-F species),as a typical structural MXene,always shows better chemical-physical characteristics than multilayer-Ti_(3)C_(2)T_(x).Thus,we prepared monolayer-Ti_(3)C_(2)T_(x) electrode by HF etching method and absolute ethyl alcohol intercalationdelamination treatment for capacitive deionization(CDI).The prepared monolay-Ti_(3)C_(2)T_(x) shows a higher specific surface area(235.6 m^(2)/g)and a thinner thickness(0.8 nm).Moreover,a series of systematic investigation demonstrated that monolayer-Ti_(3)C_(2)T_(x) has obvious promotional phenomenon on electrochemical properties(e.g.,mass specific capacitance increased from 52.1 F/g to 144.7 F/g).The NaCl adsorption capacity of monolayer-Ti_(3)C_(2)T_(x),is 30.7 mg/g in 1000 mg/L NaCl solution at 1.2 V.We concluded that the electro-sorption mechanism could be expressed as double electric layer and monolayer coverage by a good fitting of Langmuir isotherms and the pseudo-second-order kinetics equation.This work would provide a new strategy for the application of monolayer-Ti_(3)C_(2)T_(x) material in wastewater treatment in the future.
基金This work was supported by the National Natural Science Foundation of China (No.21862016)Project of Ningxia key R&D plan (No.2017BY064).
文摘The“battery type”inorganic electrode has been demonstrated the highly efficient sodium ion intercalation capacity for capacitive deionization.In this work,the CoMn_(2)O_(4)(CMO)microspheres with porous core-shell structure are prepared via co-precipitation and followed by annealing.The effects of annealing temperatures on the morphology,pore structure,valence state,and electrochemical behavior of CMO are explored.As electrode for capacitive deionization,the salt removal capacity and current efficiency of optimized AC||CMO device reaches up to 60.7 mg g^(−1) and 97.6%,respectively,and the capacity retention rate is 74.1%after 50 cycles.Remarkably,both the in-situ X-ray diffraction and ex-situ X-ray diffraction analysis features that the intercalation/de-intercalation of sodium ions are governed by(103)and(221)crystal planes of CMO.Accordingly,the density functional theory calculations realize that the adsorption energies of Na+onto(103)and(221)crystal planes are higher than that of any other crystal planes,manifesting the priorities in adsorption of sodium atoms.Furthermore,the X-ray photoelectron spectra of pristine and post-CMO electrode highlights that the reversible conversion of Mn^(3+)/Mn^(4+)couple is resulted from the intercalation/de-intercalation of Na^(+),while this is irreversible for Co^(3+)/Co^(2+)couple.Beyond that,the CMO electrode has been proven the selectivity removal of Na^(+) over K^(+)and Mg^(2+)in a multi-cation stream.
基金financially supported by the National Natural Science Foundation of China(No.51874222).
文摘Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surface area and mesoporous content than two other composite electrodes.Electrochemical analysis showed that D860/AC M presents higher specific capacitance and electrical double layer capacitor than the others,and significantly lower internal diffusion impedance.Thus,D860/AC M exhibits the highest adsorption capacity and rate of Ⅴ(Ⅳ)among three electrodes.The intra-particle diffusion model fits well in the initial adsorption stage,while the liquid film diffusion model is more suitable for fitting at the later stage.The pseudo-second-order kinetic model is suited for the entire adsorption process.The adsorption of Ⅴ(Ⅳ)on the composite electrode follows that of the Freundlich isotherm.Thermodynamic analysis indicates that the adsorption of Ⅴ(Ⅳ)is an exothermic process with entropy reduction,and the electric field force plays a dominant role in the CDI process.This work aims to improve our understanding of the ion adsorption behaviors and mechanisms on the composite electrodes in CDI.
文摘Electrode materials with high desalination capacity and long-term cyclic stability are the focus of capacitive deionization(CDI) community. Understanding the causes of performance decay in traditional carbons is crucial to design a high-performance material. Based on this, here, nitrogen-doped activated carbon(NAC) was prepared by pyrolyzing the blend of activated carbon powder(ACP) and melamine for the positive electrode of asymmetric CDI. By comparing the indicators changes such as conductivity, salt adsorption capacity, pH, and charge efficiency of the symmetrical ACP-ACP device to the asymmetric ACP-NAC device under different CDI cycles, as well as the changes of the electrochemical properties of anode and cathode materials after long-term operation, the reasons for the decline of the stability of the CDI performance were revealed. It was found that the carboxyl functional groups generated by the electro-oxidation of anode carbon materials make the anode zero-charge potential(E_(pzc)) shift positively,which results in the uneven distribution of potential windows of CDI units and affects the adsorption capacity. Furthermore, by understanding the electron density on C atoms surrounding the N atoms, we attribute the increased cyclic stability to the enhanced negativity of the charge of carbon atoms adjacent to quaternary-N and pyridinic-oxide-N.
基金supported by The National Natural Science Foundation of China(Nos.22276137,52170087).
文摘Electrode materials with strong desalting ability is an important research direction of capacitive deionization.In this study,HKUST-1 was successfully synthesized by the solvothermal method,and MOFsderived porous carbon/Cu@Cu_(2)O composites were prepared by simple pyrolysis as cathode materials for CDI.After high-temperature pyrolysis,the Cu^(+) site with unsaturated coordination is generated,and the structure changes from micropores to the coexistence of mesoporous and micropores.The complex pore structure is conducive to strengthening ion migration and diffusion.The results show that the porous carbon/Cu@Cu_(2)O materials derived from MOFs depend on the pseudocapacitance behavior for capacitive deionization and desalination.At a voltage window of-1.2V~1.2V,a current density of 40mA/g.and 5 mmol/L NaCl,the HDC-1100 exhibited the best desalting capacity of 30.9 mg/g.HDC-1100 also has good cycle stability.After 20 cycles of adsorption and desorption,the desalting capacity almost does not decrease.Therefore,MOFs derived porous carbon/Cu@Cu_(2)O composites are expected to be an excellent choice for CDI cathode materials.
基金supported by Shanxi Province Basic Research Program(Free Exploration Category)(No.202203021221041)National Natural Science Foundation of China(No.52300016)+1 种基金China Postdoctoral Science Foundation(No.2023M733379)Students Innovation and Entrepreneurship Foundation of USTC(No.CY2022G12).
文摘Flow-electrode capacitive deionization(FCDI)represents a promising approach for ion separation from aqueous solutions.However,the optimization of spacer,particularly for nitrate-contaminated groundwa-ter systems,has often been overlooked.This research comprehensively investigates the influence of using a conductive(carbon cloth,CC)spacer on nitrate removal performance within FCDI system,comparing it to a non-conductive(nylon net,NN)spacer.In both CC and NN FCDI systems,it is unsurprisingly that nitrate removal efficiency improved notably with the increasing current density and hydraulic retention time(HRT).Interestingly,the specific energy consumption(SEC)for nitrate removal did not show obvious fluctuations when the current density and HRT varied in both systems.Under the auspiciously optimized process parameters,CC-FCDI attained a 20%superior nitrate removal efficiency relative to NN-FCDI,ac-companied by a notably diminished SEC for CC-FCDI,registering at a mere 28%of NN-FCDI.This great improvement can be primarily attributed to the decrement in FCDI internal resistance after using con-ductive spacer,which further confirmed by electrochemical tests such as linear sweep voltammetry(LSV)and electrochemical impedance spectroscopy(EIS).Upon prolonged continuous nitrate removal at the optimized conditions,the CC-FCDI system achieved a consistent 90%nitrate removal efficiency with a low SEC of 2.7-7.8 kWh/kg NO_(3)-N,underscoring its steady performance.Overall,this study highlights the pivotal importance of careful spacer design and optimization in realizing energy-efficient groundwater treatment via FCDI.
文摘Water and energy shortages came due to rapid population growth, living standards and rapid development in the agriculture and industrial sectors. Desalination tends to be one of the most promising water solutions;however, it is a process of intense energy. Membrane Capacitive Deionization (MCDI) has received considerable interest as a promising desalination technology, and MCDI research has increased significantly over the last 10 years. In addition, there are no guidelines for the design of Capacitive Deionization (CDI) implementation strategies for individual applications. This study, therefore;provides an alternative of CDI’s recent application developments, with emphasis placed on hybrid systems to address the technological needs of different relevant fields. The MCDI’s energy consumption is compared with the reverse osmosis literature data based on experimental data from laboratory-scale system. The study demonstrates that MCDI technology is a promising technology in the next few years with an extreme competition in water recovery, energy consumption and salt removal for reverse osmosis.
基金supported by the National Natural Science Foundation of China(No.52371240).
文摘Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacrificial templates,which can afford Co^(2+)sources.After a facile solvothermal reaction and sequential cation etching,yolk-shell-structured layered double hydroxide@HMCSs(LDH@HMCSs)have been synthesized.The LDH@HMCSs nanocomposite possesses a three-dimensional(3D)hollow nanocage superstructure that effectively blocks the self-stacking of LDH nanosheets and promotes ion transport.Compared to CoFe-LDH@HMCSs,and Co-LDH@HMCSs,CoNi-LDH@HMCSs exhibit superior electrochemical performance and desalination performance due to the remarkable synergistic effect between the CoNi-LDH nanosheets and mesoporous N-doped carbon shells.The resultant CoNi-LDH@HMCSs-0.4-based capacitive deionization(CDI)device exhibits excellent salt adsorption capacity(SAC,36.41 mg·g^(-1))and good cycle stability.This work will confirm the significance of constructing superstructure and open new avenues for the practical application of CDI technology in water treatment.
基金supported by the National Natural Science Foundation of China(Nos.22576103 and 52000105).
文摘Covalent organic frameworks(COFs)are highly regarded for their tunable pore structures,high specific surface areas,and functionalizable active sites,making them promising candidates for heavy metal removal through capacitive deionization(CDI).However,their application in CDI faces inherent challenges,such as low electrical conductivity and insufficient utilization of redox-active sites.To address these limitations,a high-performance COF-based electrode material was synthesized by integrating COFs with carbon nanotubes(CNTs)via in situ growth(COF@CNT).By optimizing the crystallinity,charge distribution,and accessibility of active sites in the COF@CNT framework,the resultant sulfonic acid-functionalized TpPa(Tp:1,3,5-triformylphloroglucinol and Pa:1,4-phenylenediamine)COF(S-TpPa@CNT)exhibited an exceptional Cd^(2+)adsorption capacity of 165.23 mg/g at 1.2 V with an initial concentration of 80 mg/L,representing state-of-the-art performance and the highest reported value among CDI electrodes.X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations revealed that the synergistic roles of sulfonic acid groups and theβ-ketoenamine structure within the COF framework regulated the charge distribution within the COF framework and created a lower binding energy state.These findings demonstrate the potential of functionalized COF@CNT composites as high-performance electrode materials for efficient and sustainable water purification,paving the way for next-generation CDI technologies.
基金the National Natural Science Foundation of China(Nos.52100009,51871001,and 51808251)the China Postdoctoral Science Foundation(No.2021M691337)+2 种基金Excellent Youth Fund of Anhui Province(No.2108085Y17)Hundred-Talent Program of Anhui Provincethe Innovative team project of Nanjing Institute of Environmental Sciences,MEE.
文摘Capacitive deionization(CDI)is a promising technology to satisfy the global need for fresh water,since it can be both economical and sustainable.While two-dimensional transition metal carbides/nitrides(MXenes)exhibit great characteristics for use as CDI electrode materials,their tightly spaced layered structure renders intercalation inefficiency.In this study,the interlayer distance of MXenes is precisely modulated by inserting different quantity of one-dimensional bacterial fibers(BC),forming freestanding MXene/BC composite electrodes.Among the studied samples,MXene/BC-33%electrode with the interlayer spacing of 15.2Åcan achieve an optimized tradeoff among various desalination performance metrics and indicators.The salt adsorption capacity(SAC),the average salt adsorption rate(ASAR),the energy normalized adsorbed salt(ENAS),and the thermodynamic energy efficiency(TEE)of the MXene/BC-33%electrode are improved by 24%,46%,13%,and 66%respectively compared with those of pure MXene electrode.While the insertion of BC improves the ion diffusion pathways and facilitates the intercalation kinetics,the desalination performance decreases when the insertion amount of BC exceeds 40%.This is attributed to the overlarge resistance of the composite and the resulting increased energy consumption.This study reveals the desalination performance tradeoffs of MXene-based electrodes with different interlayer distances and also sheds light on the fundamental ion storage mechanisms of intercalation materials in a CDI desalination system.
基金This research was supported by the National Natural Science Foundation of China(No.21777118).
文摘Capacitive deionization(CDI)technology has been considered a promising desalination technique,especially for brackish water,because of its relatively low energy consumption,facile operation,and easy regeneration of electrodes.However,the desalination capacity,cost,fabrication method,electrochemical stability,and environmental unfriendliness of the electrodes have restricted the practical application of the CDI technique.Herein,we reported the one-step in situ preparation of nitrogen-doped and carbon-decorated MXene-derived TiO_(2)(termed N-TiO_(2−x)/C)through the confinement-growth strategy.The small particle size(∼25 nm)and uniform distribution of a peanut-like N-TiO_(2−x)/C material could be ascribed to the confined growth space created by the nanoporous structure of melamine foam.The defects produced by N doping provide an enhanced electrical conductivity and more adsorption sites,while wrapping with a carbon shell layer increases the conductivity and offers protection for N-TiO_(2−x) to achieve an excellent electrochemical stability.The prepared N-TiO_(2−x)/C electrode is hydrophilic due to the abundant oxygen-containing functional groups(e.g.,C-O,N-Ti-O,-NO_(x),and-OH)and exhibits a high salt removal capacity(33.4 mg·g^(−1)),desalination rate(1.5 mg·g^(−1)·min^(−1)),and remarkable cycling stability(without declining after 100 cycles),which might be ascribed to the synergistic effects of the short ion diffusion path,more active adsorption sites,enhanced conductivity,pseudocapacitive behavior,and protection of the carbon shell layer.This work provides a confined-growth strategy to develop MXene-derived oxide electrodes for electrochemical desalination.
基金The authors gratefully acknowledge the financial support from the Beijing Municipal Natural Science Foundation(Nos.8192030 and L182026)Fundamental Research Funds for the Central Universities(No.2016ZCQ03)National Natural Science Foundation of China(Nos.51608038 and 21975140).
文摘The practical application of the capacitive deionization(CDI)enhanced ultrafiltration(CUF)technology is hampered due to low performance of electrodes.The current study demonstrated a novel super-aligned carbon nanotube(SACNT)/activated carbon(AC)composite electrode,which was prepared through coating AC on a cross-stacked SACNT film.The desalination capability and water purification performance of the prepared electrode were systematically investigated at different applied voltages(0.8-1.2 V)with a CDI system and a CUF system,respectively.In the CDI tests,as compared with 5ie control AC electrode,the SACNT/AC electrode achieved an approximately 100%increase in both maximum salt adsorption capacity and average salt adsorption rate under all the applied voltage conditions,demonstrating a superior desalination capability.Meanwhile,a conspicuous increase by an average of-26%in charge efficiency was also achieved at all the voltages.In the CUF tests,as compared with the control run at 0 V,the treatment runs at 0.8,1.0,and 1.2 V achieved a 2.40-fold,2.08-fold,and 2.43-fold reduction in membrane fouling(calculated according to the final transmembrane pressure(TMP)data at the end of every purification stage),respectively.The average TMP increasing rates at 0.8,1.0,and 1.2 V were also roughly two times smaller than that at 0 V,indicating a dramatical reduction of membrane fouling.The SACNT/AC electrode also maintained its superior desalination capability in the CUF process,resulting in an overall improved water purification efficiency.
