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 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
Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and ...Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and high performance electrochemical oxidation system for wastewater treatment,granular active carbon(GAC) was decorated by doping Ce,Sn,Sb to synthesize Sn-Sb-Ce/GAC using sol-gel method as particle electrode filled into a three-dimensional(3D) electrochemical reactor.Scanning electron microscopy(SEM),energy-dispersive spectroscopy(EDS) and X-ray diffraction(XRD) experiments revealed that the Sn-Sb-Ce/GAC particle electrode crystal particles were compact and uniform,and the surface structure was improved.The ten cyclic experiments indicated that the Sn-Sb-Ce/GAC particle electrode had high stability and low dissolution of the loaded active substance.The degradation mechanism of MIT was studied under the optimal working conditions of 3D electrode system with GAC of 5 g/L,current density of 20 mA/cm^(2),initial pH 5,electrolyte concentration of Na_(2)SO_(4)0.02 mol/L and reaction time of 120 min.The indirect electrochemical degradation of MIT was dominated by active substance pathway that active chlorine rather than free radicals(·OH) played the main role.Comparing with conventional two-dimensional(2D) electrode system,the 3D electrochemical system has larger active electrode area,higher treatment efficiency and lower energy consumption than the former.The 3D electrochemical system could remove 96.5% of MIT from the actual high-salt reverse osmosis concentrate wastewater in 30 min.It has a certain removal effect on UV_(254)in wastewater,but has a better removal effect on fluorescent substances.This study proposed a new strategy to develop transition metal and rare earth metal particle electrodes using carbon-based materials for high efficient electrocatalytic oxidation in the electrochemical treatment system.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
TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed ...TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed to characterize the TiNT electrodes. The linear voltammetry results under irradiation showed that the TiNT electrode annealed at 450℃ presented the highest photoelectrochemical activity. By combining photocatalytic with electrochemical process, a significantly synergetic effect on ammonia degradation was observed with Na2SO4 as supporting electrolyte at pH 10.7. Furthermore, the photoelectrocatalytic efficiency on the ammonia degradation was greatly enhanced in presence of chloride ions without the limitation ofpH. The degradation rate was improved by 14.8 times reaching 4.98 × 10^-2 min^-1 at pH 10.7 and a faster degradation rate of 6.34 × 10^-2 min^-1 was obtained at pH 3.01. The in situ photoelectrocatalytic generated active chlorine was proposed to be responsible for the improved efficiency. On the other hand, an enhanced degradation of ammonia using TiNT electrode fabricated in fluorinated organic solution was also confirmed compared to TiNT electrode anodized in fluorinated water solution and TiO2 film electrode fabricated by sol-gel method. Finally, the effect of chloride concentration was also 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
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
Cobalt phosphide(CoP) is a promising anode candidate for lithium-ion batteries(LIBs) due to its high specific capacity and low working potential.However,the poor cycling stability and rate performance,caused by low el...Cobalt phosphide(CoP) is a promising anode candidate for lithium-ion batteries(LIBs) due to its high specific capacity and low working potential.However,the poor cycling stability and rate performance,caused by low electrical conductivity and huge volume variation,impede the further practical application of CoP anode materials.Herein,we report an integrated binder-free electrode featuring needle-like CoP arrays grown on carbon fiber cloth(CC) for efficient lithium storage.The as-prepared CoP/CC electrode integrates the advantages of 1 D needle-like CoP arrays for efficient electrolyte wettability and fast cha rge transpo rtation,and 3 D CC substrate for superior mechanical stability,flexibility and high conductivity.As a result,the CoP/CC electrode delivers an initial specific capacity of 1283 mAh/g and initial Coulombic effeciencies of 85.4%,which are much higher than that of conventional CoP electrode.Notably,the Co P/CC electrode shows outstanding cycling performance up to 400 cycles at 0.5 A/cm^(2) and excellent rate performance with a discharge capacity of 549 mAh/g even at 5 A/cm^(2).This work demonstrates the great potential of integrated CoP/CC hybrid as efficient bind-free and freestanding electrode for LIBs and future flexible electronic devices.展开更多
In plane micro-supercapacitors that are miniaturized energy storage components have attracted significant attention due to their high power densities for various ubiquitous and sustainable device systems as well as th...In plane micro-supercapacitors that are miniaturized energy storage components have attracted significant attention due to their high power densities for various ubiquitous and sustainable device systems as well as their facile integration on various flexible/wearable platform.To implement the micro-supercapacitors in various practical applications that can accompany solid state or gel electrolyte and flexible substrates,ions must be readily transported to electrodes for achieving high power densities.Herein,we show large enhancement in electrochemical properties of flexible,inplane micro-supercapacitor using sharp-edged interdigitated electrode design,which was simply fabricated through direct laser scribing method.The sharp-edged electrodes allowed strong electric field to be induced at the corners of the electrode fingers which led to the greater accumulation of ions near the surface of electrode,significantly enhancing the energy storage performance of micro-supercapacitors.The electric field-enhanced in-plane micro-supercapacitor showed the volumetric energy density of 1.52 Wh L^(−1)and the excellent cyclability with capacitive retention of 95.4%after 20000 cycles.We further showed various practicability of our sharp-edged design in micro-supercapacitors by showing circuit applicability,mechanical stability,and air stability.These results present an important pathway for designing electrodes in various energy storage devices.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
A theoretical model of phase change heat sink was established in terms of thermal resistance network. The influence of different parameters on the thermal resistance was analyzed and the crucial impact factors were de...A theoretical model of phase change heat sink was established in terms of thermal resistance network. The influence of different parameters on the thermal resistance was analyzed and the crucial impact factors were determined. Subsequently, the forming methods including ploughing-extrusion and stamping method of boiling enhancement structure at evaporation surface were investigated, upon which three-dimensional microgroove structure was fabricated to improve the efficiency of evaporation. Moreover, the crucial parameters related to the fabrication of miniaturized phase change heat sink were optimized. The heat transfer performance of the heat sink was tested. Results show that the developed phase change heat sink has excellent heat transfer performance and is suitable for high power LED applications.展开更多
Transition metal oxide(TMO)nanoarrays are promising architecture designs for self-supporting oxygen electrodes to achieve high catalytic activities in lithium-oxygen(Li-O2)batteries.However,the poor conductive nature ...Transition metal oxide(TMO)nanoarrays are promising architecture designs for self-supporting oxygen electrodes to achieve high catalytic activities in lithium-oxygen(Li-O2)batteries.However,the poor conductive nature of TMOs and the confined growth of nanostructures on the limited surfaces of electrode substrates result in the low areal capacities of TMO nanoarray electrodes,which seriously deteriorates the intrinsically high energy densities of Li-O2 batteries.Herein,we propose a hybrid nanoarray architecture design that integrates the high electronic conductivity of carbon nanoflakes(CNFs)and the high catalytic activity of Co3 O4 nanosheets on carbon cloth(CC).Due to the synergistic effect of two differently featured components,the hybrid nanoarrays(Co3 O4-CNF@CC)achieve a high reversible capacity of3.14 mA h cm-2 that cannot be achieved by only single components.Further,CNFs grown on CC induce the three-dimensionally distributed growth of ultrafine Co3 O4 nanosheets to enable the efficient utilization of catalysts.Thus,with the high catalytic efficiency,hybrid Co3 O4-CNF@CC also achieves a more prolonged cycling life than pristine TMO nanoarrays.The present work provides a new strategy for improving the performance of nanoarray oxygen electrodes via the hybrid architecture design that integrates the intrinsic properties of each component and induces the three-dimensional distribution of catalysts.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
The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results s...The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.展开更多
Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electroche...Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand（COD）analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions（0.2wt%NaCl）,and a three-dimensional（3D） reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline（200 mL of 100mg·L-（-1）） and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-（-2）,pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.展开更多
A method using three-dimensional electrode is applied to treat wastewater in oil fields, which contains polyacrylamide （PAM）, for analogue. A best condition for electrolysis （I= 1.0 A, t=90 min, c=0.1%, m=980 g,φ=...A method using three-dimensional electrode is applied to treat wastewater in oil fields, which contains polyacrylamide （PAM）, for analogue. A best condition for electrolysis （I= 1.0 A, t=90 min, c=0.1%, m=980 g,φ=5 mm, d=5.0 cm） has been determined, under which the COD removal efficiency reached 96.0%, COD containing in wastewater reduced to 64.3 mg/L from 1 622.9 mg/L, the figure before treatment. Three categories of PAM-containing wastewater in production practice have been treated with the COD removal ratios being 87.5%, 82.4% and 84.7% respectively. Presence of H2O2 and ·OH are detected by means of Ti（IV）-5-Br-PADAP technique and colorimetry respectively. The concentration is positively proportional to the COD removal ratio and increases in accordance with increment of time of electrolysis and current.展开更多
A three-dimensional heterogeneous mass transfer model was proposed to investigate the enhancement of dispersed particles on gas absorption. The strategy to calculate local and overall enhancement factors is proposed. ...A three-dimensional heterogeneous mass transfer model was proposed to investigate the enhancement of dispersed particles on gas absorption. The strategy to calculate local and overall enhancement factors is proposed. Instead of a global grid, the composite overlapping grid is adopted, which simplifies the setup and solution of the three-dimensional model equations. It is found that dispersed particle hold-up, particle size, liquid-solid partition coefficient of transported component, characteristic contact time, and the shortest distance between particles and gas-liquid interface have major influence on absorption enhancement factor. The particle-particle interaction on gas absorption and the lateral diffusion of transported component in liquid film were studied with the multi-particle simulation. The proposed model predicted the experimental data from the literature reasonably well.展开更多
The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electr...The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electrochemical perromance of the coke modified with various active components was studied. The results show that the coke modified with Fe（NO3）2 has the lowest energy consumption and higher COD removal rate under the same condition, and the modified coke has better surface characteristics for the purpose of this study. In addition, the kinetic constant was also calculated. The study shows that the three-dimensional electrode system with Fe （NO3）z-modified coke can give a satisfactory solution in biologically pretreated coking wastewater.展开更多
Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, w...Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, where seven tensile/compressive stresses are designed and loaded on electrodes, thereby decoupling mechanics and electrochemistry through incremental stress loads. Four types of multi-group electrochemical tests under tensile/compressive stress loading and normal package loading are performed to quantitatively characterize the effects of tensile stress and compressive stress on cycle performance and the kinetic performance of a silicon composite electrode. Experiments show that a tensile stress improves the electrochemical performance of a silicon composite electrode, exhibiting increased specific capacity and capacity retention rate, reduced energy dissipation rate and impedances, enhanced reactivity, accelerated ion/electron migration and diffusion, and reduced polarization. Contrarily, a compressive stress has the opposite effect, inhibiting the electrochemical performance. The stress effect is nonlinear, and a more obvious suppression via compressive stress is observed than an enhancement via tensile stress. For example, a tensile stress of 675 k Pa increases diffusion coefficient by 32.5%, while a compressive stress reduces it by 35%. Based on the experimental results, the stress regulation mechanism is analyzed. Tensile stress loads increase the pores of the electrode material microstructure, providing more deformation spaces and ion/electron transport channels. This relieves contact compressive stress, strengthens diffusion/reaction, and reduces the degree of damage and energy dissipation. Thus, the essence of stress enhancement is that it improves and optimizes diffusion, reaction and stress in the microstructure of electrode material as well as their interactions via physical morphology.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the financial supports from Major Science and Technology project of China Power Engineering Consulting Group Co., Ltd. "Research on Green and digital Intelligent Technology of Sewage Treatment Plant" (No. CEEC2023-ZDYF-09)Technology Innovation Ability Improvement Project of Shandong Province, China (No. 2022TSGC1247)。
文摘Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and high performance electrochemical oxidation system for wastewater treatment,granular active carbon(GAC) was decorated by doping Ce,Sn,Sb to synthesize Sn-Sb-Ce/GAC using sol-gel method as particle electrode filled into a three-dimensional(3D) electrochemical reactor.Scanning electron microscopy(SEM),energy-dispersive spectroscopy(EDS) and X-ray diffraction(XRD) experiments revealed that the Sn-Sb-Ce/GAC particle electrode crystal particles were compact and uniform,and the surface structure was improved.The ten cyclic experiments indicated that the Sn-Sb-Ce/GAC particle electrode had high stability and low dissolution of the loaded active substance.The degradation mechanism of MIT was studied under the optimal working conditions of 3D electrode system with GAC of 5 g/L,current density of 20 mA/cm^(2),initial pH 5,electrolyte concentration of Na_(2)SO_(4)0.02 mol/L and reaction time of 120 min.The indirect electrochemical degradation of MIT was dominated by active substance pathway that active chlorine rather than free radicals(·OH) played the main role.Comparing with conventional two-dimensional(2D) electrode system,the 3D electrochemical system has larger active electrode area,higher treatment efficiency and lower energy consumption than the former.The 3D electrochemical system could remove 96.5% of MIT from the actual high-salt reverse osmosis concentrate wastewater in 30 min.It has a certain removal effect on UV_(254)in wastewater,but has a better removal effect on fluorescent substances.This study proposed a new strategy to develop transition metal and rare earth metal particle electrodes using carbon-based materials for high efficient electrocatalytic oxidation in the electrochemical treatment system.
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. 21277134, 21107103)the State Key Laboratory of Environmental, Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences
文摘TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed to characterize the TiNT electrodes. The linear voltammetry results under irradiation showed that the TiNT electrode annealed at 450℃ presented the highest photoelectrochemical activity. By combining photocatalytic with electrochemical process, a significantly synergetic effect on ammonia degradation was observed with Na2SO4 as supporting electrolyte at pH 10.7. Furthermore, the photoelectrocatalytic efficiency on the ammonia degradation was greatly enhanced in presence of chloride ions without the limitation ofpH. The degradation rate was improved by 14.8 times reaching 4.98 × 10^-2 min^-1 at pH 10.7 and a faster degradation rate of 6.34 × 10^-2 min^-1 was obtained at pH 3.01. The in situ photoelectrocatalytic generated active chlorine was proposed to be responsible for the improved efficiency. On the other hand, an enhanced degradation of ammonia using TiNT electrode fabricated in fluorinated organic solution was also confirmed compared to TiNT electrode anodized in fluorinated water solution and TiO2 film electrode fabricated by sol-gel method. Finally, the effect of chloride concentration was also 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.
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financial supported by the National Natural Science Foundation of China(Nos.51662029,21863006)Jiangxi Province Research Program of Science and Technology(No.2011BBE50023)。
文摘Cobalt phosphide(CoP) is a promising anode candidate for lithium-ion batteries(LIBs) due to its high specific capacity and low working potential.However,the poor cycling stability and rate performance,caused by low electrical conductivity and huge volume variation,impede the further practical application of CoP anode materials.Herein,we report an integrated binder-free electrode featuring needle-like CoP arrays grown on carbon fiber cloth(CC) for efficient lithium storage.The as-prepared CoP/CC electrode integrates the advantages of 1 D needle-like CoP arrays for efficient electrolyte wettability and fast cha rge transpo rtation,and 3 D CC substrate for superior mechanical stability,flexibility and high conductivity.As a result,the CoP/CC electrode delivers an initial specific capacity of 1283 mAh/g and initial Coulombic effeciencies of 85.4%,which are much higher than that of conventional CoP electrode.Notably,the Co P/CC electrode shows outstanding cycling performance up to 400 cycles at 0.5 A/cm^(2) and excellent rate performance with a discharge capacity of 549 mAh/g even at 5 A/cm^(2).This work demonstrates the great potential of integrated CoP/CC hybrid as efficient bind-free and freestanding electrode for LIBs and future flexible electronic devices.
基金supported by a National Research Foundation of Korea grant funded by the Korean government(MSIT)(2020R1A2C1101039)by Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry,and Energy(MOTIE)of the Republic of Korea(20204030200060)supported by the Soonchunhyang University Research Fund
文摘In plane micro-supercapacitors that are miniaturized energy storage components have attracted significant attention due to their high power densities for various ubiquitous and sustainable device systems as well as their facile integration on various flexible/wearable platform.To implement the micro-supercapacitors in various practical applications that can accompany solid state or gel electrolyte and flexible substrates,ions must be readily transported to electrodes for achieving high power densities.Herein,we show large enhancement in electrochemical properties of flexible,inplane micro-supercapacitor using sharp-edged interdigitated electrode design,which was simply fabricated through direct laser scribing method.The sharp-edged electrodes allowed strong electric field to be induced at the corners of the electrode fingers which led to the greater accumulation of ions near the surface of electrode,significantly enhancing the energy storage performance of micro-supercapacitors.The electric field-enhanced in-plane micro-supercapacitor showed the volumetric energy density of 1.52 Wh L^(−1)and the excellent cyclability with capacitive retention of 95.4%after 20000 cycles.We further showed various practicability of our sharp-edged design in micro-supercapacitors by showing circuit applicability,mechanical stability,and air stability.These results present an important pathway for designing electrodes in various energy storage devices.
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Projects(51575115,51775122) supported by the National Natural Science Foundation of China
文摘A theoretical model of phase change heat sink was established in terms of thermal resistance network. The influence of different parameters on the thermal resistance was analyzed and the crucial impact factors were determined. Subsequently, the forming methods including ploughing-extrusion and stamping method of boiling enhancement structure at evaporation surface were investigated, upon which three-dimensional microgroove structure was fabricated to improve the efficiency of evaporation. Moreover, the crucial parameters related to the fabrication of miniaturized phase change heat sink were optimized. The heat transfer performance of the heat sink was tested. Results show that the developed phase change heat sink has excellent heat transfer performance and is suitable for high power LED applications.
基金supported by grants from the National Natural Science Foundation of China(Nos.21673169,51672205,51972257)the National Key Research Program of China(No.2016YFA0202602)+1 种基金the Research Start-Up Fund from Wuhan University of Technologythe Fundamental Research Funds for the Central Universities(WUT:No.2019IB003)。
文摘Transition metal oxide(TMO)nanoarrays are promising architecture designs for self-supporting oxygen electrodes to achieve high catalytic activities in lithium-oxygen(Li-O2)batteries.However,the poor conductive nature of TMOs and the confined growth of nanostructures on the limited surfaces of electrode substrates result in the low areal capacities of TMO nanoarray electrodes,which seriously deteriorates the intrinsically high energy densities of Li-O2 batteries.Herein,we propose a hybrid nanoarray architecture design that integrates the high electronic conductivity of carbon nanoflakes(CNFs)and the high catalytic activity of Co3 O4 nanosheets on carbon cloth(CC).Due to the synergistic effect of two differently featured components,the hybrid nanoarrays(Co3 O4-CNF@CC)achieve a high reversible capacity of3.14 mA h cm-2 that cannot be achieved by only single components.Further,CNFs grown on CC induce the three-dimensionally distributed growth of ultrafine Co3 O4 nanosheets to enable the efficient utilization of catalysts.Thus,with the high catalytic efficiency,hybrid Co3 O4-CNF@CC also achieves a more prolonged cycling life than pristine TMO nanoarrays.The present work provides a new strategy for improving the performance of nanoarray oxygen electrodes via the hybrid architecture design that integrates the intrinsic properties of each component and induces the three-dimensional distribution of catalysts.
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.
文摘The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.
基金supported by the National Natural Science Foundation of China(21507104)the Fundamental Research Funds for the Central Universities of China
文摘Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand（COD）analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions（0.2wt%NaCl）,and a three-dimensional（3D） reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline（200 mL of 100mg·L-（-1）） and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-（-2）,pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.
基金Supported by the National High-Technology Research and Development Program(2003AA602140-2)the Important Scientific Re-search Project of Hubei Provincial Department of Education, China (2004D001)
文摘A method using three-dimensional electrode is applied to treat wastewater in oil fields, which contains polyacrylamide （PAM）, for analogue. A best condition for electrolysis （I= 1.0 A, t=90 min, c=0.1%, m=980 g,φ=5 mm, d=5.0 cm） has been determined, under which the COD removal efficiency reached 96.0%, COD containing in wastewater reduced to 64.3 mg/L from 1 622.9 mg/L, the figure before treatment. Three categories of PAM-containing wastewater in production practice have been treated with the COD removal ratios being 87.5%, 82.4% and 84.7% respectively. Presence of H2O2 and ·OH are detected by means of Ti（IV）-5-Br-PADAP technique and colorimetry respectively. The concentration is positively proportional to the COD removal ratio and increases in accordance with increment of time of electrolysis and current.
基金Supported by the National Natural Science Foundation of China (No. 20136010).
文摘A three-dimensional heterogeneous mass transfer model was proposed to investigate the enhancement of dispersed particles on gas absorption. The strategy to calculate local and overall enhancement factors is proposed. Instead of a global grid, the composite overlapping grid is adopted, which simplifies the setup and solution of the three-dimensional model equations. It is found that dispersed particle hold-up, particle size, liquid-solid partition coefficient of transported component, characteristic contact time, and the shortest distance between particles and gas-liquid interface have major influence on absorption enhancement factor. The particle-particle interaction on gas absorption and the lateral diffusion of transported component in liquid film were studied with the multi-particle simulation. The proposed model predicted the experimental data from the literature reasonably well.
文摘The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electrochemical perromance of the coke modified with various active components was studied. The results show that the coke modified with Fe（NO3）2 has the lowest energy consumption and higher COD removal rate under the same condition, and the modified coke has better surface characteristics for the purpose of this study. In addition, the kinetic constant was also calculated. The study shows that the three-dimensional electrode system with Fe （NO3）z-modified coke can give a satisfactory solution in biologically pretreated coking wastewater.
基金Project supported by the Major Program of the National Natural Science Foundation of China(Grant No.11890680)the National Natural Science Foundation of China(Grant No.12022205)。
文摘Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, where seven tensile/compressive stresses are designed and loaded on electrodes, thereby decoupling mechanics and electrochemistry through incremental stress loads. Four types of multi-group electrochemical tests under tensile/compressive stress loading and normal package loading are performed to quantitatively characterize the effects of tensile stress and compressive stress on cycle performance and the kinetic performance of a silicon composite electrode. Experiments show that a tensile stress improves the electrochemical performance of a silicon composite electrode, exhibiting increased specific capacity and capacity retention rate, reduced energy dissipation rate and impedances, enhanced reactivity, accelerated ion/electron migration and diffusion, and reduced polarization. Contrarily, a compressive stress has the opposite effect, inhibiting the electrochemical performance. The stress effect is nonlinear, and a more obvious suppression via compressive stress is observed than an enhancement via tensile stress. For example, a tensile stress of 675 k Pa increases diffusion coefficient by 32.5%, while a compressive stress reduces it by 35%. Based on the experimental results, the stress regulation mechanism is analyzed. Tensile stress loads increase the pores of the electrode material microstructure, providing more deformation spaces and ion/electron transport channels. This relieves contact compressive stress, strengthens diffusion/reaction, and reduces the degree of damage and energy dissipation. Thus, the essence of stress enhancement is that it improves and optimizes diffusion, reaction and stress in the microstructure of electrode material as well as their interactions via physical morphology.
