This study focused on As(V)removal by electrosorption in a self-made three-dimensional electrode reactor,in which granular activated carbon(GAC)was used as the particle electrode.Under the optimal conditions,the remov...This study focused on As(V)removal by electrosorption in a self-made three-dimensional electrode reactor,in which granular activated carbon(GAC)was used as the particle electrode.Under the optimal conditions,the removal efficiency of As(V)was 84%,and its residual concentration in solution was 0.08 mg/L.From kinetic investigation,the rate determining steps of the entire process may involve more than two processes:membrane diffusion,material diffusion and physical/chemical adsorption processes.During the desorption process,As(V)can be desorbed from GAC,and the GAC was able to electro-adsorb As(V)again after desorption,which means that the electrode has good cycling performance.展开更多
The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode...The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.展开更多
The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research...The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research focus in this technology.They are usually in the form of particles that fill the space between the cathode and anode,and the selection of materials used is important.Carbon-based materials are widely used because of their large specific surface area,good adsorption performance,high chemical stability and low cost.The principles of 3D electrode technology are introduced and recent research on its use for degrading organic pollutants using carbon-based particle electrodes is summarized.The classification of particle electrodes is introduced and the challenges for the future development of carbon-based particle electrodes in wastewater treatment are discussed.展开更多
Degradation of o-chloronitrobenzene wastewater was experimentally investigated at a three-dimensional electrode（TDE） with granular activated carbon as the particle electrode, graphite as the anode, and stainless ste...Degradation of o-chloronitrobenzene wastewater was experimentally investigated at a three-dimensional electrode（TDE） with granular activated carbon as the particle electrode, graphite as the anode, and stainless steel plate as the cathode. The kinetic model of o-chloronitrobenzene degradation was studied, and the effects of pH, electrolysis time, particle electrode, electrolyte concentration, and initial concentration of the solution on degradation efficiency were investigated to determine the optimal operating conditions. The degradation of o-chloronitrobenzene by oxidation at the TDE was monitored by chemical oxygen demand（COD） measurements, UV-Vis absorption, and high performance liquid chromatography（HPLC）. COD degradation by electrochemical degradation followed pseudo-first order kinetics with respect to the concentration of o-chloronitrobenzene solutions. Optimal reaction conditions included 15 g of activated carbon as the particle electrode, 400 mg/L o-chloronitrobenzene solution containing 0.10 mol/L Na2SO4, pH=3, and 60 min of electrolysis. The UV-Vis absorption spectra and HPLC results illustrate that the benzene ring in o-chloronitrobenzene was rapidly broken down to form aliphatic substances through electrochemical degradation. COD degradation was approximately 98.5% at optimal conditions.展开更多
The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated cata...The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated catalytic activity and minimal energy consumption continues to pose a significant challenge.In this research,Fluorine-doped copper-carbon(F/Cu-GAC)particle electrodes were effectively synthesized through an impregnationcalcination technique,utilizing granular activated carbon as the carrier and fluorinedoped modified copper oxides as the catalytic agents.The particle electrodes were subsequently utilized to promote the degradation of 2,4,6-trichlorophenol(2,4,6-TCP)in a threedimensional electrocatalytic reactor(3DER).The F/Cu-GAC particle electrodes were polarized under the action of electric field,which promoted the heterogeneous Fenton-like reaction in which H2O2 generated by two-electron oxygen reduction reaction(2e-ORR)of O_(2) was catalytically decomposed to·OH.The 3DER equipped with F/Cu-GAC particle electrodes showed 100%removal of 2,4,6-TCP and 79.24%removal of TOC with a specific energy consumption(EC)of approximately 0.019 kWh/g·COD after 2 h of operation.The F/Cu-GAC particle electrodes exhibited an overpotential of 0.38 V and an electrochemically active surface area(ECSA)of 715 cm^(2),as determined through linear sweep voltammetry(LSV)and cyclic voltammetry(CV)assessments.These findings suggest a high level of electrocatalytic performance.Furthermore,the catalytic mechanism of the 3DER equipped with F/Cu-GAC particle electrodes was elucidated through the application of X-ray photoelectron spectroscopy(XPS),electron spin resonance(ESR),and active species capture experiments.This investigation offers a novel approach for the effective degradation of 2,4,6-TCP.展开更多
In this study,nickel foam-loaded Mn and Ce bimetallic oxide composites were successfully synthesized as particle electrodes by a hydrothermal method and synergized with ozone for the efficient degradation of alizarin ...In this study,nickel foam-loaded Mn and Ce bimetallic oxide composites were successfully synthesized as particle electrodes by a hydrothermal method and synergized with ozone for the efficient degradation of alizarin red(AR),a typical anthraquinone dye.The effects of common factors on the degradation rate of alizarin red were investigated.The optimal experimental conditions were derived as applied voltage=3.5 V,initial pH=5.5,NaCl concentration of 4.5 g/L,and initial dye concentration of 20 mg/L.The particle electrode had a high cyclic stability after five cycles.The active sites of the dye molecular structure were analyzed in combination with the Fukui function,and the degradation pathway of alizarin red was proposed on this basis.By comparing the degradation effect of alizarin red under three different systems of O3,3DER and 3DER-O3,it was confirmed that the three-dimensional electrode has a good synergistic effect in conjunction with ozone.Finally,the degradation mechanism of alizarin red under the CeO_(2)-MnO_(2)/NF synergistic ozone system was derived,in which the single linear oxygen(1O_(2))played a major role in the degradation process.展开更多
In order to increase the electrode surface area and enhance the charge storage capacity, we study the micro electro mechanical system technology to fabricate three-dimensional high aspect ratio micro-electrode structu...In order to increase the electrode surface area and enhance the charge storage capacity, we study the micro electro mechanical system technology to fabricate three-dimensional high aspect ratio micro-electrode structure based on glass. The anodic constant potential method is employed to deposit manganese oxide as electroactive substances on the micro-electrode surface. Cyclic voltammetry and constant current charge-discharge method are both used to prepare electrode electrochemical performance testing, with a two-dimensional electrode without structure for comparison. Experimental results show that three-dimensional elec- trode structure can effectively enhance the charge storage capacity. At 1.0 mA/cm2 charge- discharge density, the three-dimensional electrode shows a capacitance of 17.88 mF/cm2, seven times higher than the two-dimensional electrode.展开更多
Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of va...Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.展开更多
The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.Howeve...The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.展开更多
Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that p...Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that possess both high thermopower and rapid redox kinetics.This work addresses this challenge by leveraging our recently developed copper(Ⅰ/Ⅱ)(Cu^(+)/Cu^(2+))redox couple.We significantly enhance the performance of Cu-based liquid thermocells by integrating a thermosensitive crystallization process with etched carbon cloth electrodes,achieving synergistic improvements in thermodynamic and kinetic performance.The thermosensitive crystallization process establishes a persistent Cu^(2+)concentration gradient,boosting the thermopower from 1.47 to 2.93 mV K^(-1).Moreover,the etched carbon cloth electrodes provide a larger electroactive surface area and demonstrate a higher current density.Consequently,the optimized Cu^(+)/Cu^(2+)system achieved an exceptional normalized power density P_(max)(ΔT)^(-2)of 3.97 mW m^(-2)K^(-2).A thermocell module comprised of 20 cells directly power various electronic devices at a temperature difference of 40 K.This work successfully exhibits potential of Cu^(+)/Cu^(2+)redox couple in thermoelectric conversion and introduces a valuable redox couple for highperformance thermocells.展开更多
To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as wel...To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.展开更多
Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_...Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.展开更多
Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-...Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.展开更多
The neural interface is a key component in wireless brain–computer prostheses.In this study,we demonstrate that a unique three-dimensional(3D)microneedle electrode on a flexible mesh substrate,which can be fabricated...The neural interface is a key component in wireless brain–computer prostheses.In this study,we demonstrate that a unique three-dimensional(3D)microneedle electrode on a flexible mesh substrate,which can be fabricated without complicated micromachining techniques,is conformal to the tissues with minimal invasiveness.Furthermore,we demonstrate that it can be applied to different functional layers in the nervous system without length limitation.The microneedle electrode is fabricated using drawing lithography technology from biocompatible materials.In this approach,the profile of a 3D microneedle electrode array is determined by the design of a two-dimensional(2D)pattern on the mask,which can be used to access different functional layers in different locations of the brain.Due to the sufficient stiffness of the electrode and the excellent flexibility of the mesh substrate,the electrode can penetrate into the tissue with its bottom layer fully conformal to the curved brain surface.Then,the exposed contact at the end of the microneedle electrode can successfully acquire neural signals from the brain.展开更多
Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage...Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage of energy density is the main stumbling block for their practical applications.To solve this energy issue,constructing a three-dimensional(3D)electrode within the limited footprint area is proposed as a new solution for improving the energy storage capacity ofMSCs.In the last few years,extensive efforts have been devoted to developing 3D electrodes for MSCs,and significant progress and breakthrough have been achieved.While,there is still lack of systematic summary on the 3D electrode design strategies.To this end,it is imperative to outline the basic design conception,summarize the current states,and discuss the future research about 3D electrodes in MSCs based on the latest development.展开更多
The feasibility of decomplexation removal of typical contaminants in electroplating wastewater,complexed Cu(Ⅱ)with 1-hydroxyethylidene-1,1-diphosphonic acid(Cu-HEDP),was first performed by a three-dimensional electro...The feasibility of decomplexation removal of typical contaminants in electroplating wastewater,complexed Cu(Ⅱ)with 1-hydroxyethylidene-1,1-diphosphonic acid(Cu-HEDP),was first performed by a three-dimensional electrode reactor with activated biochar as particle electrodes.For the case of 50 mg/L Cu-HEDP,Cu(Ⅱ)removal(90.7%)and PO_(4)^(3−)conversion(34.9%)were achieved under the conditions of electric current 40 mA,initial pH 7,acid-treated almond shell biochar(AASB)addition 20 g/L,and reaction time 180 min,with second-order rate constants of 1.10×10^(−3) and 1.94×10^(−5) min^(−1) respectively.The growing chelating effect between Cu(II)and HEDP and the comprehensive actions of adsorptive accumulation,direct and indirect oxidation given by particle electrodes accounted for the enhanced removal of Cu-HEDP,even though the mineralization of HEDP was mainly dependent on anode oxidation.The performance attenuation of AASB particle electrodes was ascribed to the excessive consumption of oxygen-containing functionalities during the reaction,especially acidic carboxylic groups and quinones on particle electrodes,which decreased from 446.74 to 291.48μmol/g,and 377.55 to 247.71μmol/g,respectively.Based on the determination of adsorption behavior and indirect electrochemical oxidation mediated by in situ electrogenerated H_(2)O_(2) and reactive oxygen species(e.g.,•OH),a possible removal mechanism of Cu-HEDP by three-dimensional electrolysis was further proposed.展开更多
New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also du...New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also due to their adverse impacts on water ecological environment.Electro-Fenton technology is an effective method to remove PPCPs from water.Novel particle electrodes(MMT/rGO/Fe_(3)O_(4))were synthesized by depositing Fe3O4 nanoparticles on reduced graphene oxide modified montmorillonite and acted as catalysts to promote oxidation performance in a three-dimensional electro-Fenton(3D-EF)system.The electrodes combined the catalytic property of Fe3O4,hydrophilicity of montmorillonite and electrical conductivity of graphene oxides,and applied for the degradation of Acyclovir(ACV)with high efficiency and ease of operation.At optimal condition,the degradation rate of ACV reached 100%within 120 min,and the applicable pH range could be 3 to 11 in the 3D-EF system.The stability and reusability of MMT/rGO/Fe_(3)O_(4)particle electrodes were also studied,the removal rate of ACV remained at 92%after 10 cycles,which was just slightly lower than that of the first cycle.Potential degradation mechanisms were also proposed by methanol quenching tests and FT-ICR-MS.展开更多
As a supercapacitor electrode, the graphene/polyaniline （PANI） composite sponge with a three-dimensional （3D） porous network structure is synthesized by a simple three-step method. The three steps include an in si...As a supercapacitor electrode, the graphene/polyaniline （PANI） composite sponge with a three-dimensional （3D） porous network structure is synthesized by a simple three-step method. The three steps include an in situ polymerization, freeze-drying and reduction by hydrazine vapor. The prepared sponge has a large specific surface area and porous network structure, so it is in favor of spreading the electrolyte ion and increasing the charge transfer efficiency of the system. The process of preparation is simple, easy to operate and low cost. The composite sponge shows better electrochemical performance than the pure individual graphene sponge while PANI cannot keep the shape of a sponge. Such a composite sponge exhibits specific capacitances of 487 F.g-1 at 2 mV/s compared to pristine PANI of 397 F.g-1.展开更多
A macroscopic cell and three-dimensional fluid model have been used to investigate the discharge characteristics in ac plasma display panel cells of electrode-shaping configurations. Four kinds of non-standaxd geometr...A macroscopic cell and three-dimensional fluid model have been used to investigate the discharge characteristics in ac plasma display panel cells of electrode-shaping configurations. Four kinds of non-standaxd geometries （i.e. D-, △-, W- and U-shape electrodes） have been considered. The characteristics of the discharge current, the operating voltage and the discharge efficiency of different configurations have been discussed. It is found that the discharge efficiency can be improved by about 10%-30% compared with the standard geometry, while the operating voltage increases slightly in the non-standard geometries. There is a trade-off between improving the discharge efficiency and lowering the sustaining voltage in design of plasma display cells by electrode shaping.展开更多
Three-dimensional(3D)vertical architecture transistors represent an important technological pursuit,which have distinct advantages in device integration density,operation speed,and power consumption.However,the fabric...Three-dimensional(3D)vertical architecture transistors represent an important technological pursuit,which have distinct advantages in device integration density,operation speed,and power consumption.However,the fabrication processes of such 3D devices are complex,especially in the interconnection of electrodes.In this paper,we present a novel method which combines suspended electrodes and focused ion beam(FIB)technology to greatly simplify the electrodes interconnection in 3D devices.Based on this method,we fabricate 3D vertical core-double shell structure transistors with ZnO channel and Al_(2)O_(3) gate-oxide both grown by atomic layer deposition.Suspended top electrodes of vertical architecture could be directly connected to planar electrodes by FIB deposited Pt nanowires,which avoid cumbersome steps in the traditional 3D structure fabrication technology.Both single pillar and arrays devices show well behaved transfer characteristics with an Ion/Ioff current ratio greater than 106 and a low threshold voltage around 0 V.The ON-current of the 2×2 pillars vertical channel transistor was 1.2μA at the gate voltage of 3 V and drain voltage of 2 V,which can be also improved by increasing the number of pillars.Our method for fabricating vertical architecture transistors can be promising for device applications with high integration density and low power consumption.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 52004256)the Shanxi Provincial Science Foundation for Youths, China (No. 201901D211212)+2 种基金the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi Province, China (No. 2019L0574)the Young Academic Leader of North University of China (No. QX202004)the Postdoctoral Innovative Talent Support Program of Hunan Province, China (2021RC2010)
文摘This study focused on As(V)removal by electrosorption in a self-made three-dimensional electrode reactor,in which granular activated carbon(GAC)was used as the particle electrode.Under the optimal conditions,the removal efficiency of As(V)was 84%,and its residual concentration in solution was 0.08 mg/L.From kinetic investigation,the rate determining steps of the entire process may involve more than two processes:membrane diffusion,material diffusion and physical/chemical adsorption processes.During the desorption process,As(V)can be desorbed from GAC,and the GAC was able to electro-adsorb As(V)again after desorption,which means that the electrode has good cycling performance.
基金Project(50925417)supported by the National Natureal Science Foundation for Distinguished Young Scholar of ChinaProject(51074191)supported by the National Natural Science Foundation of China
文摘The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.
文摘The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research focus in this technology.They are usually in the form of particles that fill the space between the cathode and anode,and the selection of materials used is important.Carbon-based materials are widely used because of their large specific surface area,good adsorption performance,high chemical stability and low cost.The principles of 3D electrode technology are introduced and recent research on its use for degrading organic pollutants using carbon-based particle electrodes is summarized.The classification of particle electrodes is introduced and the challenges for the future development of carbon-based particle electrodes in wastewater treatment are discussed.
基金Supported by the National Natural Science Foundation of China(Nos.50602003, 50502004)the Beijing Science & Technology Star Plans, China(No.2007B020)
文摘Degradation of o-chloronitrobenzene wastewater was experimentally investigated at a three-dimensional electrode（TDE） with granular activated carbon as the particle electrode, graphite as the anode, and stainless steel plate as the cathode. The kinetic model of o-chloronitrobenzene degradation was studied, and the effects of pH, electrolysis time, particle electrode, electrolyte concentration, and initial concentration of the solution on degradation efficiency were investigated to determine the optimal operating conditions. The degradation of o-chloronitrobenzene by oxidation at the TDE was monitored by chemical oxygen demand（COD） measurements, UV-Vis absorption, and high performance liquid chromatography（HPLC）. COD degradation by electrochemical degradation followed pseudo-first order kinetics with respect to the concentration of o-chloronitrobenzene solutions. Optimal reaction conditions included 15 g of activated carbon as the particle electrode, 400 mg/L o-chloronitrobenzene solution containing 0.10 mol/L Na2SO4, pH=3, and 60 min of electrolysis. The UV-Vis absorption spectra and HPLC results illustrate that the benzene ring in o-chloronitrobenzene was rapidly broken down to form aliphatic substances through electrochemical degradation. COD degradation was approximately 98.5% at optimal conditions.
基金supported by Guangxi Science and Technology Major Program(No.AA23073008)Hubei Key Laboratory of Water System Science for Sponge City Construction(Wuhan University)(No.2023–05)Nanning Innovation and Entrepreneur Leading Talent Project(No.2021001).
文摘The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated catalytic activity and minimal energy consumption continues to pose a significant challenge.In this research,Fluorine-doped copper-carbon(F/Cu-GAC)particle electrodes were effectively synthesized through an impregnationcalcination technique,utilizing granular activated carbon as the carrier and fluorinedoped modified copper oxides as the catalytic agents.The particle electrodes were subsequently utilized to promote the degradation of 2,4,6-trichlorophenol(2,4,6-TCP)in a threedimensional electrocatalytic reactor(3DER).The F/Cu-GAC particle electrodes were polarized under the action of electric field,which promoted the heterogeneous Fenton-like reaction in which H2O2 generated by two-electron oxygen reduction reaction(2e-ORR)of O_(2) was catalytically decomposed to·OH.The 3DER equipped with F/Cu-GAC particle electrodes showed 100%removal of 2,4,6-TCP and 79.24%removal of TOC with a specific energy consumption(EC)of approximately 0.019 kWh/g·COD after 2 h of operation.The F/Cu-GAC particle electrodes exhibited an overpotential of 0.38 V and an electrochemically active surface area(ECSA)of 715 cm^(2),as determined through linear sweep voltammetry(LSV)and cyclic voltammetry(CV)assessments.These findings suggest a high level of electrocatalytic performance.Furthermore,the catalytic mechanism of the 3DER equipped with F/Cu-GAC particle electrodes was elucidated through the application of X-ray photoelectron spectroscopy(XPS),electron spin resonance(ESR),and active species capture experiments.This investigation offers a novel approach for the effective degradation of 2,4,6-TCP.
基金supported by the Postgraduate Innovation Fund Project by Southwest University of Science and Technology(No.24ycx2059)the National Natural Science Foundation of China(Nos.41831285 and 51974261).
文摘In this study,nickel foam-loaded Mn and Ce bimetallic oxide composites were successfully synthesized as particle electrodes by a hydrothermal method and synergized with ozone for the efficient degradation of alizarin red(AR),a typical anthraquinone dye.The effects of common factors on the degradation rate of alizarin red were investigated.The optimal experimental conditions were derived as applied voltage=3.5 V,initial pH=5.5,NaCl concentration of 4.5 g/L,and initial dye concentration of 20 mg/L.The particle electrode had a high cyclic stability after five cycles.The active sites of the dye molecular structure were analyzed in combination with the Fukui function,and the degradation pathway of alizarin red was proposed on this basis.By comparing the degradation effect of alizarin red under three different systems of O3,3DER and 3DER-O3,it was confirmed that the three-dimensional electrode has a good synergistic effect in conjunction with ozone.Finally,the degradation mechanism of alizarin red under the CeO_(2)-MnO_(2)/NF synergistic ozone system was derived,in which the single linear oxygen(1O_(2))played a major role in the degradation process.
文摘In order to increase the electrode surface area and enhance the charge storage capacity, we study the micro electro mechanical system technology to fabricate three-dimensional high aspect ratio micro-electrode structure based on glass. The anodic constant potential method is employed to deposit manganese oxide as electroactive substances on the micro-electrode surface. Cyclic voltammetry and constant current charge-discharge method are both used to prepare electrode electrochemical performance testing, with a two-dimensional electrode without structure for comparison. Experimental results show that three-dimensional elec- trode structure can effectively enhance the charge storage capacity. At 1.0 mA/cm2 charge- discharge density, the three-dimensional electrode shows a capacitance of 17.88 mF/cm2, seven times higher than the two-dimensional electrode.
基金supported by the University of Seoul’s 2025 Research Fund.
文摘Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.
基金financial support from the National Natural Science Foundation of China(52473248,52203123,52125301,22279070 and U21A20170)the State Key Laboratory of Polymer Materials Engineering(Grant No:sklpme 2023-1-05 and sklpme 2024-2-04)+2 种基金the Ministry of Science and Technology of China(No.2019YFA0705703)the Sichuan Science and Technology Program(2023NSFSC0991 and 2025ZNSFSC1411)the Fundamental Research Funds for the Central Universities.This research was partially sponsored by the Double First-Class Construction Funds of Sichuan University.
文摘The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.
基金financially supported by research grants from Innovative Research Group Project of National Natural Science Foundation of China(52021004)the National Key Research and Development Program of China(2022YFB3803300)+1 种基金the National Natural Science Foundation of China(62474026,62205140,12204071)the China Postdoctoral Science Foundation(2022M710532)。
文摘Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that possess both high thermopower and rapid redox kinetics.This work addresses this challenge by leveraging our recently developed copper(Ⅰ/Ⅱ)(Cu^(+)/Cu^(2+))redox couple.We significantly enhance the performance of Cu-based liquid thermocells by integrating a thermosensitive crystallization process with etched carbon cloth electrodes,achieving synergistic improvements in thermodynamic and kinetic performance.The thermosensitive crystallization process establishes a persistent Cu^(2+)concentration gradient,boosting the thermopower from 1.47 to 2.93 mV K^(-1).Moreover,the etched carbon cloth electrodes provide a larger electroactive surface area and demonstrate a higher current density.Consequently,the optimized Cu^(+)/Cu^(2+)system achieved an exceptional normalized power density P_(max)(ΔT)^(-2)of 3.97 mW m^(-2)K^(-2).A thermocell module comprised of 20 cells directly power various electronic devices at a temperature difference of 40 K.This work successfully exhibits potential of Cu^(+)/Cu^(2+)redox couple in thermoelectric conversion and introduces a valuable redox couple for highperformance thermocells.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2021M3H4A1A02048529)the Ministry of Trade,Industry and Energy(MOTIE)of the Korean government under grant No.RS-2022-00155854support from the DGIST Supercomputing and Big Data Center.
文摘To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.
基金funding from the National Natural Science Foundation of China(Award 91745203)supplemented by Central Universities'Basic Research Funds.We gratefully acknowledge the National Synchrotron Radiation Laboratory(NSRL,Hefei,China)for providing MCD-A and MCD-B beamlines for Soft XAS characterization.The authors are grateful to the Instrument and equipment sharing platform,College of Physics,Jilin University,for providing technical assistance in HT-XRD measurements.
文摘Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.
基金funding support from Natural Science Foundation of Shanghai(Grant No.23ZR1443900)the National Natural Science Foundation of China(Grant Nos.22178309,22476131 and 22176127)。
文摘Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.
基金This work was supported by grants from the National Research Foundation(NRF)CRP project‘Peripheral Nerve Prostheses:A Paradigm Shift in Restoring Dexterous Limb Function’(NRF-CRP10-2012-01,R-719-000-001-281)the NRF CRP project‘Self-Powered Body Sensor Network for Disease Management and Prevention Oriented Healthcare’(NRF-CRP8-2011-01,R-263-000-A27-281).
文摘The neural interface is a key component in wireless brain–computer prostheses.In this study,we demonstrate that a unique three-dimensional(3D)microneedle electrode on a flexible mesh substrate,which can be fabricated without complicated micromachining techniques,is conformal to the tissues with minimal invasiveness.Furthermore,we demonstrate that it can be applied to different functional layers in the nervous system without length limitation.The microneedle electrode is fabricated using drawing lithography technology from biocompatible materials.In this approach,the profile of a 3D microneedle electrode array is determined by the design of a two-dimensional(2D)pattern on the mask,which can be used to access different functional layers in different locations of the brain.Due to the sufficient stiffness of the electrode and the excellent flexibility of the mesh substrate,the electrode can penetrate into the tissue with its bottom layer fully conformal to the curved brain surface.Then,the exposed contact at the end of the microneedle electrode can successfully acquire neural signals from the brain.
基金China Scholarship CouncilDeutsche Forschungsgemeinschaft,Grant/Award Numbers:LE 2249/4-1,LE 2249/5-1Bundesministerium für Bildung und Forschung,Grant/Award Number:03Z1MN11。
文摘Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage of energy density is the main stumbling block for their practical applications.To solve this energy issue,constructing a three-dimensional(3D)electrode within the limited footprint area is proposed as a new solution for improving the energy storage capacity ofMSCs.In the last few years,extensive efforts have been devoted to developing 3D electrodes for MSCs,and significant progress and breakthrough have been achieved.While,there is still lack of systematic summary on the 3D electrode design strategies.To this end,it is imperative to outline the basic design conception,summarize the current states,and discuss the future research about 3D electrodes in MSCs based on the latest development.
基金supported by the support from Youth Program of National Natural Science Foundation of China (No.52000051)Initial Scientific Research Foundation of Overseas High-level Talents of Harbin Institute of Technology (Shenzhen)(No.FA11409004)Natural Science Foundation of Guangdong Province (No.2017A030310670)
文摘The feasibility of decomplexation removal of typical contaminants in electroplating wastewater,complexed Cu(Ⅱ)with 1-hydroxyethylidene-1,1-diphosphonic acid(Cu-HEDP),was first performed by a three-dimensional electrode reactor with activated biochar as particle electrodes.For the case of 50 mg/L Cu-HEDP,Cu(Ⅱ)removal(90.7%)and PO_(4)^(3−)conversion(34.9%)were achieved under the conditions of electric current 40 mA,initial pH 7,acid-treated almond shell biochar(AASB)addition 20 g/L,and reaction time 180 min,with second-order rate constants of 1.10×10^(−3) and 1.94×10^(−5) min^(−1) respectively.The growing chelating effect between Cu(II)and HEDP and the comprehensive actions of adsorptive accumulation,direct and indirect oxidation given by particle electrodes accounted for the enhanced removal of Cu-HEDP,even though the mineralization of HEDP was mainly dependent on anode oxidation.The performance attenuation of AASB particle electrodes was ascribed to the excessive consumption of oxygen-containing functionalities during the reaction,especially acidic carboxylic groups and quinones on particle electrodes,which decreased from 446.74 to 291.48μmol/g,and 377.55 to 247.71μmol/g,respectively.Based on the determination of adsorption behavior and indirect electrochemical oxidation mediated by in situ electrogenerated H_(2)O_(2) and reactive oxygen species(e.g.,•OH),a possible removal mechanism of Cu-HEDP by three-dimensional electrolysis was further proposed.
基金the GDAS’Project of Science and Technology Development(No.2020GDASYL-20200103044)Key-Area Research and Development Program of Guangdong(No.2020B1111350002)+1 种基金the National Key R&D Program of China(No.2019YFC1805305)the Project of Water Resource Department of Guangdong Province(No.2017-18).
文摘New pollutant pharmaceutical and personal care products(PPCPs),especially antiviral drugs,have received increasing attention not only due to their increase in usage after the outbreak of COVID-19 epidemics but also due to their adverse impacts on water ecological environment.Electro-Fenton technology is an effective method to remove PPCPs from water.Novel particle electrodes(MMT/rGO/Fe_(3)O_(4))were synthesized by depositing Fe3O4 nanoparticles on reduced graphene oxide modified montmorillonite and acted as catalysts to promote oxidation performance in a three-dimensional electro-Fenton(3D-EF)system.The electrodes combined the catalytic property of Fe3O4,hydrophilicity of montmorillonite and electrical conductivity of graphene oxides,and applied for the degradation of Acyclovir(ACV)with high efficiency and ease of operation.At optimal condition,the degradation rate of ACV reached 100%within 120 min,and the applicable pH range could be 3 to 11 in the 3D-EF system.The stability and reusability of MMT/rGO/Fe_(3)O_(4)particle electrodes were also studied,the removal rate of ACV remained at 92%after 10 cycles,which was just slightly lower than that of the first cycle.Potential degradation mechanisms were also proposed by methanol quenching tests and FT-ICR-MS.
基金supported by the Natural Science Foundation from Harbin University of Science and Technology and Harbin Institute of Technology
文摘As a supercapacitor electrode, the graphene/polyaniline （PANI） composite sponge with a three-dimensional （3D） porous network structure is synthesized by a simple three-step method. The three steps include an in situ polymerization, freeze-drying and reduction by hydrazine vapor. The prepared sponge has a large specific surface area and porous network structure, so it is in favor of spreading the electrolyte ion and increasing the charge transfer efficiency of the system. The process of preparation is simple, easy to operate and low cost. The composite sponge shows better electrochemical performance than the pure individual graphene sponge while PANI cannot keep the shape of a sponge. Such a composite sponge exhibits specific capacitances of 487 F.g-1 at 2 mV/s compared to pristine PANI of 397 F.g-1.
基金Project supported by the National Natural Science Foundation of China （Grant No 10475007）, the Scientific Research Foundation for the Returned 0verseas Chinese Scholars, the State Education Ministry of China （Grant No LLKYJJ200403） and Thomson . Plasma, France.
文摘A macroscopic cell and three-dimensional fluid model have been used to investigate the discharge characteristics in ac plasma display panel cells of electrode-shaping configurations. Four kinds of non-standaxd geometries （i.e. D-, △-, W- and U-shape electrodes） have been considered. The characteristics of the discharge current, the operating voltage and the discharge efficiency of different configurations have been discussed. It is found that the discharge efficiency can be improved by about 10%-30% compared with the standard geometry, while the operating voltage increases slightly in the non-standard geometries. There is a trade-off between improving the discharge efficiency and lowering the sustaining voltage in design of plasma display cells by electrode shaping.
基金the National Key Research and Development Program of China(Grant Nos.2016YFA0200400 and 2016YFA0200800)the National Natural Science Foundation of China(Grant Nos.61888102,12074420,and 11674387)+1 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB33000000)Key Research Program of Frontier Sciences,Chinese Acdemy of Sciences(Grant No.QYZDJ-SSWSLH042).
文摘Three-dimensional(3D)vertical architecture transistors represent an important technological pursuit,which have distinct advantages in device integration density,operation speed,and power consumption.However,the fabrication processes of such 3D devices are complex,especially in the interconnection of electrodes.In this paper,we present a novel method which combines suspended electrodes and focused ion beam(FIB)technology to greatly simplify the electrodes interconnection in 3D devices.Based on this method,we fabricate 3D vertical core-double shell structure transistors with ZnO channel and Al_(2)O_(3) gate-oxide both grown by atomic layer deposition.Suspended top electrodes of vertical architecture could be directly connected to planar electrodes by FIB deposited Pt nanowires,which avoid cumbersome steps in the traditional 3D structure fabrication technology.Both single pillar and arrays devices show well behaved transfer characteristics with an Ion/Ioff current ratio greater than 106 and a low threshold voltage around 0 V.The ON-current of the 2×2 pillars vertical channel transistor was 1.2μA at the gate voltage of 3 V and drain voltage of 2 V,which can be also improved by increasing the number of pillars.Our method for fabricating vertical architecture transistors can be promising for device applications with high integration density and low power consumption.
