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
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
To improve the specific capacitance and rate capability of electrode material for supercapacitors, a three-dimensional graphene/polyaniline （3DGN/PANI） composite is prepared via in situ polymerization on GN hydrogel...To improve the specific capacitance and rate capability of electrode material for supercapacitors, a three-dimensional graphene/polyaniline （3DGN/PANI） composite is prepared via in situ polymerization on GN hydrogel. PANI grows on the GN surface as a thin film, and its content in the composite is controlled by the concentration of the reaction monomer. The specific capacitance of the 3DGN/PANI composite containing 10 wt% PANI reaches 322.8 F.g-1 at a current density of 1 A.g-1, nearly twice as large as that of the pure 3DGN （162.8 F.g-1）. The capacitance of the composite is 307.9 F.g-1 at 30 A.g-1 （maintaining 95.4%）, and 89% retention after 500 cycles. This study demonstrates the exciting potential of 3DGN/PANI with high capacitance, excellent rate capability and long cycling life for supercapacitors.展开更多
Porous three-dimensional (3D) structures generally improve the performance of electrodes by increasing their active surface area and the diffusion speed of electrolyte ions during charging/discharging.Threedimensional...Porous three-dimensional (3D) structures generally improve the performance of electrodes by increasing their active surface area and the diffusion speed of electrolyte ions during charging/discharging.Threedimensional polypyrrole (PPy) based films were created by electrodepositing PPy in the presence of varying amounts of chloride anions (Cl^(-)) and polyanionic ribbonlike nanoparticles (carboxylated cellulose nanocrystals (CNC-COO-)) as scaffold material.The assembly mechanism of the 3D PPy electrodes combines the effect of different nucleation and growth mechanisms during electropolymerization and deposition of the formed PPy with CNC-COO-and with Cl^(-).The highest area capacitance of these electrode materials was 1.39 F cm^(-2)(150.2 F g^(-1)) at a current density of 1 m A cm^(-2)(0.1 A g^(-1)).More importantly,at a high current density of 20 m A cm^(-2)(2.2 A g^(-1)),the thick (ca.130μm),3D,and high mass loading(9.2 mg cm^(-2)) Cl^(-):CNC-COO-/PPy films exhibited an excellent areal capacitance of 0.85 F cm^(-2)(70.8 F g^(-1)),increasing about 16%over CNC-COO-/PPy films prepared without Cl^(-)present during electrodeposition.In addition,an aqueous Cl^(-):CNC-COO-/PPy (with Cl^(-):CNC-COO-=2.0) symmetric supercapacitor had an outstanding energy density of 41.15μWh cm^(-2)(4.46 Wh kg^(-1)) and excellent cycling stability,while even improving on its original areal capacitance (to 111.2%of its original capacitance) after cycling3000 cycles at 8 m A cm^(-2),indicating their potential in energy storage devices.展开更多
In this work,based on the role of pre-ionization of the non-uniform electric field and its effect of reducing the collisional ionization coefficient,a diffuse dielectric barrier discharge plasma is formed in the open ...In this work,based on the role of pre-ionization of the non-uniform electric field and its effect of reducing the collisional ionization coefficient,a diffuse dielectric barrier discharge plasma is formed in the open space outside the electrode structure at a lower voltage by constructing a three-dimensional non-uniform spatial electric field using a contact electrode structure.The air purification study is also carried out.Firstly,a contact electrode structure is constructed using a three-dimensional wire electrode.The distribution characteristics of the spatial electric field formed by this electrode structure are analyzed,and the effects of the non-uniform electric field and the different angles of the vertical wire on the generation of three-dimensional spatial diffuse discharge are investigated.Secondly,the copper foam contact electrode structure is constructed using copper foam material,and the effects of different mesh sizes on the electric field distribution are analyzed.The results show that as the mesh size of the copper foam becomes larger,a strong electric field region exists not only on the surface of the insulating layer,but also on the surface of the vertical wires inside the copper foam,i.e.,the strong electric field region shows a three-dimensional distribution.Besides,as the mesh size increases,the area of the vertical strong electric field also increases.However,the electric field strength on the surface of the insulating layer gradually decreases.Therefore,the appropriate mesh size can effectively increase the discharge area,which is conducive to improving the air purification efficiency.Finally,a highly permeable stacked electrode structure of multilayer wire-copper foam is designed.In combination with an ozone treatment catalyst,an air purification device is fabricated,and the air purification experiment is carried out.展开更多
The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transitio...The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.展开更多
High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has c...High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.展开更多
Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poi...Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.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.
基金Project supported by the National Basic Research Program of China(Grant Nos.2011CB932700 and 2011CB932703)the National Natural Science Foundation of China(Grant Nos.61335006,61378073,and 61077044)+1 种基金the Beijing Natural Science Foundation,China(Grant No.4132031)the Fundamental Research Funds for the Central Universities of Beijing Jiaotong University,China(Grant No.2014YJS136)
文摘To improve the specific capacitance and rate capability of electrode material for supercapacitors, a three-dimensional graphene/polyaniline （3DGN/PANI） composite is prepared via in situ polymerization on GN hydrogel. PANI grows on the GN surface as a thin film, and its content in the composite is controlled by the concentration of the reaction monomer. The specific capacitance of the 3DGN/PANI composite containing 10 wt% PANI reaches 322.8 F.g-1 at a current density of 1 A.g-1, nearly twice as large as that of the pure 3DGN （162.8 F.g-1）. The capacitance of the composite is 307.9 F.g-1 at 30 A.g-1 （maintaining 95.4%）, and 89% retention after 500 cycles. This study demonstrates the exciting potential of 3DGN/PANI with high capacitance, excellent rate capability and long cycling life for supercapacitors.
基金supported by the Research Foundation Flanders,Belgium(3E181170 and 12Y0319N)supported by the China Scholarship Council,China(CSC,201806220066)。
文摘Porous three-dimensional (3D) structures generally improve the performance of electrodes by increasing their active surface area and the diffusion speed of electrolyte ions during charging/discharging.Threedimensional polypyrrole (PPy) based films were created by electrodepositing PPy in the presence of varying amounts of chloride anions (Cl^(-)) and polyanionic ribbonlike nanoparticles (carboxylated cellulose nanocrystals (CNC-COO-)) as scaffold material.The assembly mechanism of the 3D PPy electrodes combines the effect of different nucleation and growth mechanisms during electropolymerization and deposition of the formed PPy with CNC-COO-and with Cl^(-).The highest area capacitance of these electrode materials was 1.39 F cm^(-2)(150.2 F g^(-1)) at a current density of 1 m A cm^(-2)(0.1 A g^(-1)).More importantly,at a high current density of 20 m A cm^(-2)(2.2 A g^(-1)),the thick (ca.130μm),3D,and high mass loading(9.2 mg cm^(-2)) Cl^(-):CNC-COO-/PPy films exhibited an excellent areal capacitance of 0.85 F cm^(-2)(70.8 F g^(-1)),increasing about 16%over CNC-COO-/PPy films prepared without Cl^(-)present during electrodeposition.In addition,an aqueous Cl^(-):CNC-COO-/PPy (with Cl^(-):CNC-COO-=2.0) symmetric supercapacitor had an outstanding energy density of 41.15μWh cm^(-2)(4.46 Wh kg^(-1)) and excellent cycling stability,while even improving on its original areal capacitance (to 111.2%of its original capacitance) after cycling3000 cycles at 8 m A cm^(-2),indicating their potential in energy storage devices.
基金supported by the Fundamental Research Funds for the Central Universities(No.2022YJS094)。
文摘In this work,based on the role of pre-ionization of the non-uniform electric field and its effect of reducing the collisional ionization coefficient,a diffuse dielectric barrier discharge plasma is formed in the open space outside the electrode structure at a lower voltage by constructing a three-dimensional non-uniform spatial electric field using a contact electrode structure.The air purification study is also carried out.Firstly,a contact electrode structure is constructed using a three-dimensional wire electrode.The distribution characteristics of the spatial electric field formed by this electrode structure are analyzed,and the effects of the non-uniform electric field and the different angles of the vertical wire on the generation of three-dimensional spatial diffuse discharge are investigated.Secondly,the copper foam contact electrode structure is constructed using copper foam material,and the effects of different mesh sizes on the electric field distribution are analyzed.The results show that as the mesh size of the copper foam becomes larger,a strong electric field region exists not only on the surface of the insulating layer,but also on the surface of the vertical wires inside the copper foam,i.e.,the strong electric field region shows a three-dimensional distribution.Besides,as the mesh size increases,the area of the vertical strong electric field also increases.However,the electric field strength on the surface of the insulating layer gradually decreases.Therefore,the appropriate mesh size can effectively increase the discharge area,which is conducive to improving the air purification efficiency.Finally,a highly permeable stacked electrode structure of multilayer wire-copper foam is designed.In combination with an ozone treatment catalyst,an air purification device is fabricated,and the air purification experiment is carried out.
基金supported by the Science and Technology Project of Southwest Petroleum University(No.2021JBGS03)the Local Science and Technology Development Fund Projects Guided by the Central Government of China(No.2021ZYD0060)+2 种基金the National Natural Science Foundation of China(Nos.22209143 and 52371241)Guangdong High-level Innovation Institute Project(Nos.2021B0909050001 and 2021CX02L365)Guangdong Basic and Applied Basic Research Foundation(No.2023B1515120095).
文摘The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.
基金supported by the National Natural Science Foundation of China(22378431,52004338,51622406,21673298)Hunan Provincial Natural Science Foundation(2023JJ40210,2022JJ20075)+3 种基金the Science and Technology Innovation Program of Hunan Province(2023RC3259)the Key R&D plan of Hunan Province(2024JK2096)Scientifc Research Fund of Hunan Provincial Education Department(23B0699)Central South University Innovation-Driven Research Programme(2023CXQD008).
文摘High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.
基金supported by National Natural Science Foundation of China(22279018)National Natural Science Foundation of China(22005055)Natural Science Foundation of Fujian Province(2022J01085).
文摘Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.
