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
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
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
Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,...Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.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
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
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
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
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
Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple ...Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.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
Flow-electrode capacitive deionization(FCDI)is an innovative technology in which an intermediate chamber plays an important role in the desalination process.However,relatively few studies have been conducted on the st...Flow-electrode capacitive deionization(FCDI)is an innovative technology in which an intermediate chamber plays an important role in the desalination process.However,relatively few studies have been conducted on the structures of these intermediate chambers.In this study,we propose a novel flow-electrode capacitive deionization device with a spindle-shaped inlet chamber(S-FCDI).The desalination rate of the S-FCDI under optimal operating conditions was 36%higher than that of the FCDI device with a conventional rectangular chamber(R-FCDI).The spindle-shaped chamber transferred 1.2μmol more ions than the rectangular chamber,based on energy per joule.Additionally,we performed a detailed analysis of different inlet chamber shapes using computational fluid dynamics software.We concluded that S-FCDI has a relatively low flow resistance and almost no stagnation zone.This provides unique insights into the development of intermediate chambers.This study may contribute to the improvement of the desalination performance in industrial applications of FCDI.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
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
Electrochemical water treatment is an attractive technology for water desalination and softening due to its low energy consumption. Especially, capacitive Deionization(CDI) is promising as a future technology for wate...Electrochemical water treatment is an attractive technology for water desalination and softening due to its low energy consumption. Especially, capacitive Deionization(CDI) is promising as a future technology for water treatment. Graphene(rGO) has been intensively studied for CDI electrode because of its advantages such as excellent electrical conductivity and high specific surface area. However, its 2D dimensional structure with small specific capacitance, high resistance between layers and hydrophobicity degrades ion adsorption efficiency. In this work, we successfully prepared uniformly dispersed Fe3O4/rGO nanocomposite by simple thermal reactions and applied it as effective electrodes for CDI. Iron oxides play a role in uniting graphene sheets, and specific capacitance and wettability of electrodes are improved significantly;hence CDI performances are enhanced. The hardness removal of Fe3O4/rGO nanocomposite electrodes can reach 4.3 mg/g at applied voltage of 1.5V, which is 3 times higher than that of separate r GO electrodes.Thus this material is a promising candidate for water softening technology.展开更多
Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this wo...Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this work, B and N co-doped porous carbon with micro-mesoporous structures is derived from sodium alginate by a carbonization, activation, and hydrothermal doping process, which exhibits large specific surface area (2587 m^(2)·g^(‒1)) and high specific capacitance (190.7 F·g^(‒1)) for adsorption of salt ions and heavy metal ions. Furthermore, the materials provide a desalination capacity of 26.9 mg·g−1 at 1.2 V in 500 mg·L^(‒1) NaCl solution as well as a high removal capacity (239.6 mg·g^(‒1)) and adsorption rate (7.99 mg·g^(‒1)·min^(‒1)) for Pb2+ with an excellent cycle stability. This work can pave the way to design low-cost porous carbon with high-performances for removal of salt ions and heavy metal ions.展开更多
Membrane capacitive deionization(MCDI)is an efficient desalination technology for brine.Penicillin fermentation residue biochar(PFRB)possesses a hierarchical porous and O/N-doped structure which could serve as a high-...Membrane capacitive deionization(MCDI)is an efficient desalination technology for brine.Penicillin fermentation residue biochar(PFRB)possesses a hierarchical porous and O/N-doped structure which could serve as a high-capacity desalination electrode in the MCDI system.Under optimal conditions(electrode weight,voltage,and concentration)and a carbonization temperature of 700℃,the maximum salt adsorption capacity of the electrode can reach 26.4 mg/g,which is higher than that of most carbon electrodes.Furthermore,the electrochemical properties of the PFRB electrode were characterized through cyclic voltammetry(CV)and electrochemical impedance spectroscopy(EIS)with a maximum specific capacitance of 212.18 F/g.Finally,biotoxicity tests have showed that PFRB was non-biotoxin against luminescent bacteria and the MCDI system with the PFRB electrode remained stable even after 27 adsorption–desorption cycles.This study provides a novel way to recycle penicillin residue and an electrode that can achieve excellent desalination.展开更多
Capacitive deionization(CDI)is a novel electrochemical water-treatment technology.The electrode material is an important factor in determining the ion separation efficiency.Activated carbon(AC)is extensively used as a...Capacitive deionization(CDI)is a novel electrochemical water-treatment technology.The electrode material is an important factor in determining the ion separation efficiency.Activated carbon(AC)is extensively used as an electrode material;however,there are still many deficiencies in commercial AC.We adopted a simple processing method,ball milling,to produce ball milled AC(BAC)to improve the physical and electrochemical properties of the original AC and desalination efficiency.The BAC was characterized in detail and used for membrane capacitive deionization(MCDI)and flow-electrode capacitive deionization(FCDI)electrode materials.After ball milling,the BAC obtained excellent pore structures and favorable surfaces for ion adsorption,which reduced electron transfer resistance and ion migration resistance in the electrodes.The optimal ball-milling time was 10 h.However,the improved effects of BAC as fixed electrodes and flow electrodes are different and the related mechanisms are discussed in detail.The average salt adsorption rates(ASAR)of FCDI and MCDI were improved by 134%and 17%,respectively,and the energy-normalized removal salt(ENRS)were enhanced by 21%and 53%,respectively.We believe that simple,low-cost,and environmentally friendly BAC has great potential for practical engineering applications of FCDI and MCDI.展开更多
Fluoride is an important pollutant in wastewater,and adsorption is an effective way to remove fluoride.Because nitrogen plays an important role in adsorbent materials,computational models were developed to understand ...Fluoride is an important pollutant in wastewater,and adsorption is an effective way to remove fluoride.Because nitrogen plays an important role in adsorbent materials,computational models were developed to understand the changes in work function resulting from nitrogen doping.La-N-C-800℃,was prepared by pyrolyzing La-MOF-NH_(2)to verify the influence on the performance of removing fluoride by electrosorption.Material and electrochemical performance tests were performed to characterize La-N-C-800℃.Adsorption kinetics,adsorption thermodynamics,initial concentrations,pH,and ions competition were investigated using La-N-C-800℃for fluoride removal.In addition,density functional theory was applied to evaluate the function of nitrogen.When nitrogen atoms were added,the density of states,partial density of states,populations,and different orbits of charge were calculated to discover deep changes.Nitrogen strengthened the carbon structure and La_(2)O_(3)structure to remove fluoride.In addition,nitrogen can also act as an adsorption site in the carbon structure.These results provide design ideas for improving the performance of adsorbent materials by doping elements.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
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supported by The National Natural Science Foundation of China(22276137,52170087)the Fundamental Research Funds for the Central Universities(XJEDU2023Z009).
文摘Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.
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We gratefully acknowledge financial supports from the National Natural Science Foundation of China(No.52202371,51905125,52102364)the Natural Science Foundation of Shandong Province(No.ZR2020QE066)+2 种基金Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2020KF08)SDUT&Zibo City Integration Development Project(No.2021SNPT0045)the fellowship of China Postdoctoral Science Foundation(No.2020M672081).
文摘Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.
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.
基金Science and Technology Project of Hebei Education Department(China)(No.QN2022038)special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control(China)(No.22K05ESPCT)。
文摘Flow-electrode capacitive deionization(FCDI)is an innovative technology in which an intermediate chamber plays an important role in the desalination process.However,relatively few studies have been conducted on the structures of these intermediate chambers.In this study,we propose a novel flow-electrode capacitive deionization device with a spindle-shaped inlet chamber(S-FCDI).The desalination rate of the S-FCDI under optimal operating conditions was 36%higher than that of the FCDI device with a conventional rectangular chamber(R-FCDI).The spindle-shaped chamber transferred 1.2μmol more ions than the rectangular chamber,based on energy per joule.Additionally,we performed a detailed analysis of different inlet chamber shapes using computational fluid dynamics software.We concluded that S-FCDI has a relatively low flow resistance and almost no stagnation zone.This provides unique insights into the development of intermediate chambers.This study may contribute to the improvement of the desalination performance in industrial applications of FCDI.
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 international cooperation program for science and technology funded by the Ministry of Science,ICT&Future Planning(NRF-2014K1A3A1A09063208)
文摘Electrochemical water treatment is an attractive technology for water desalination and softening due to its low energy consumption. Especially, capacitive Deionization(CDI) is promising as a future technology for water treatment. Graphene(rGO) has been intensively studied for CDI electrode because of its advantages such as excellent electrical conductivity and high specific surface area. However, its 2D dimensional structure with small specific capacitance, high resistance between layers and hydrophobicity degrades ion adsorption efficiency. In this work, we successfully prepared uniformly dispersed Fe3O4/rGO nanocomposite by simple thermal reactions and applied it as effective electrodes for CDI. Iron oxides play a role in uniting graphene sheets, and specific capacitance and wettability of electrodes are improved significantly;hence CDI performances are enhanced. The hardness removal of Fe3O4/rGO nanocomposite electrodes can reach 4.3 mg/g at applied voltage of 1.5V, which is 3 times higher than that of separate r GO electrodes.Thus this material is a promising candidate for water softening technology.
基金partially supported by the National Natural Science Foundation of China(Grant Nos.51472174,61604086,and 21776147)the Shandong Province Natural Science Foundation(Grant Nos.ZR2018BB066,ZR2021YQ32,and ZR2022QB164)the Taishan Scholar Project of Shandong Province(Grant No.tsqn201909117)。
文摘Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this work, B and N co-doped porous carbon with micro-mesoporous structures is derived from sodium alginate by a carbonization, activation, and hydrothermal doping process, which exhibits large specific surface area (2587 m^(2)·g^(‒1)) and high specific capacitance (190.7 F·g^(‒1)) for adsorption of salt ions and heavy metal ions. Furthermore, the materials provide a desalination capacity of 26.9 mg·g−1 at 1.2 V in 500 mg·L^(‒1) NaCl solution as well as a high removal capacity (239.6 mg·g^(‒1)) and adsorption rate (7.99 mg·g^(‒1)·min^(‒1)) for Pb2+ with an excellent cycle stability. This work can pave the way to design low-cost porous carbon with high-performances for removal of salt ions and heavy metal ions.
基金This work was supported by the Natural Science Foundation of Hebei Province(China)(Nos.B2021208035,B2020208064,and E2020208054).
文摘Membrane capacitive deionization(MCDI)is an efficient desalination technology for brine.Penicillin fermentation residue biochar(PFRB)possesses a hierarchical porous and O/N-doped structure which could serve as a high-capacity desalination electrode in the MCDI system.Under optimal conditions(electrode weight,voltage,and concentration)and a carbonization temperature of 700℃,the maximum salt adsorption capacity of the electrode can reach 26.4 mg/g,which is higher than that of most carbon electrodes.Furthermore,the electrochemical properties of the PFRB electrode were characterized through cyclic voltammetry(CV)and electrochemical impedance spectroscopy(EIS)with a maximum specific capacitance of 212.18 F/g.Finally,biotoxicity tests have showed that PFRB was non-biotoxin against luminescent bacteria and the MCDI system with the PFRB electrode remained stable even after 27 adsorption–desorption cycles.This study provides a novel way to recycle penicillin residue and an electrode that can achieve excellent desalination.
基金supported by the Science and Technology Project of Hebei Education Department(No.QN2022038)the State Key Joint Laboratory of Environment Simulation and Pollution Control(No.22K05ESPCT)the Hebei University of Science and Technology Graduate Innovation Funding Program(No.XJCXZZSS2022009).
文摘Capacitive deionization(CDI)is a novel electrochemical water-treatment technology.The electrode material is an important factor in determining the ion separation efficiency.Activated carbon(AC)is extensively used as an electrode material;however,there are still many deficiencies in commercial AC.We adopted a simple processing method,ball milling,to produce ball milled AC(BAC)to improve the physical and electrochemical properties of the original AC and desalination efficiency.The BAC was characterized in detail and used for membrane capacitive deionization(MCDI)and flow-electrode capacitive deionization(FCDI)electrode materials.After ball milling,the BAC obtained excellent pore structures and favorable surfaces for ion adsorption,which reduced electron transfer resistance and ion migration resistance in the electrodes.The optimal ball-milling time was 10 h.However,the improved effects of BAC as fixed electrodes and flow electrodes are different and the related mechanisms are discussed in detail.The average salt adsorption rates(ASAR)of FCDI and MCDI were improved by 134%and 17%,respectively,and the energy-normalized removal salt(ENRS)were enhanced by 21%and 53%,respectively.We believe that simple,low-cost,and environmentally friendly BAC has great potential for practical engineering applications of FCDI and MCDI.
基金supported by the Jointly funded project of Guangzhou City School (College)of Guangzhou Basic Research Program (No.202201020205)the Talent Cultivation Program of Guangzhou University (Nos.RP2021014 and YJ2021005)+6 种基金the Guangdong Basic and Applied Basic Research Foundation (No.2021A1515110899)the Youth Innovative Talents Project of Guangdong Province (No.2021KQNCX062)the Basic and Applied Basic Research in Guangzhou (Nos.202201010001 and 201707010256)the Guangzhou University-Hong Kong University of Science and Technology Joint Research Cooperation Fund (No.YH202102)the National Natural Science Foundation of China (No.51778156)the Pearl River S&T Nova Program of Guangzhou (No.201806010191)the Guangdong Natural Science Foundation (No.2022A1515010441)。
文摘Fluoride is an important pollutant in wastewater,and adsorption is an effective way to remove fluoride.Because nitrogen plays an important role in adsorbent materials,computational models were developed to understand the changes in work function resulting from nitrogen doping.La-N-C-800℃,was prepared by pyrolyzing La-MOF-NH_(2)to verify the influence on the performance of removing fluoride by electrosorption.Material and electrochemical performance tests were performed to characterize La-N-C-800℃.Adsorption kinetics,adsorption thermodynamics,initial concentrations,pH,and ions competition were investigated using La-N-C-800℃for fluoride removal.In addition,density functional theory was applied to evaluate the function of nitrogen.When nitrogen atoms were added,the density of states,partial density of states,populations,and different orbits of charge were calculated to discover deep changes.Nitrogen strengthened the carbon structure and La_(2)O_(3)structure to remove fluoride.In addition,nitrogen can also act as an adsorption site in the carbon structure.These results provide design ideas for improving the performance of adsorbent materials by doping elements.
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.