The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commo...The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commonly employed technologies for remediating wastewater and polluted soil,their widespread adoption is hindered by their limitations,which include high costs associated with EAOPs and prolonged remediation time of biotreatments.In the review,we provided an overviewof EAOP technology and biotreatment,emphasizing the critical aspects involved in building a combined system.This review systematically evaluates recent research that combines EAOPswith bioremediation for treating wastewater or contaminated soil as pretreatment or post-treatment process.Research findings suggest that the combined treatment method represents a promising and competitive technology that can overcome some of the limitations of individual treatments.Additionally,we discussed the potential applications of this technology in varying levels of wastewater and soil pollution,as well as the underlying combination mechanisms.展开更多
Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illust...Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.展开更多
The direct difunctionalization of alkenes serves as one of the most straightforward strategies toward complex nitrogen-containing compounds.The existing approach is extensively promoted by using C/Xcentered radicals a...The direct difunctionalization of alkenes serves as one of the most straightforward strategies toward complex nitrogen-containing compounds.The existing approach is extensively promoted by using C/Xcentered radicals and N-nucleophiles to conduct 1,2-difunctional amination/azolization of alkenes.In contrast,2,1-difunctional amination/azolization of alkenes by using nitrogen-centered radicals(NCRs) and nucleophiles still remains rarely underexplored.It is possibly due to the highly active electron properties of NCRs and the relatively poor nucleophilicity of aromatic NCRs to be trapped by arylalkenes.Herein,we demonstrate an unprecedented 2,1-hydroxazolization reactions of arylalkenes through electrochemically enabled addition of NCRs from azoles and nucleophiles(NuH) in high yields and with high regioselectivity.This conversion is characterized by the fact that neither metal catalysts nor external chemical oxidants are required.This electrochemical oxidation synthesis method can also be applied for a broad range of NuH including pyridine hydrofluoride,ammonia,water,alcohols,and acids which enables the formation of C-N and C-X(X=F/N/O) bonds in one-pot fashion to furnish efficient fluoroamination,diamination and oxoamination of alkenes.展开更多
In recent years,machine learning(ML)techniques have demonstrated a strong ability to solve highly complex and non-linear problems by analyzing large datasets and learning their intrinsic patterns and relationships.Par...In recent years,machine learning(ML)techniques have demonstrated a strong ability to solve highly complex and non-linear problems by analyzing large datasets and learning their intrinsic patterns and relationships.Particularly in chemical engineering and materials science,ML can be used to discover microstructural composition,optimize chemical processes,and create novel synthetic pathways.Electrochemical processes offer the advantages of precise process control,environmental friendliness,high energy conversion efficiency and low cost.This review article provides the first systematic summary of ML in the application of electrochemical oxidation,including pollutant removal,battery remediation,substance synthesis and material characterization prediction.Hot trends at the intersection of ML and electrochemical oxidation were analyzed through bibliometrics.Common ML models were outlined.The role of ML in improving removal efficiency,optimizing experimental conditions,aiding battery diagnosis and predictive maintenance,and revealing material characterization was highlighted.In addition,current issues and future perspectives were presented in relation to the strengths and weaknesses of ML algorithms applied to electrochemical oxidation.In order to further support the sustainable growth of electrochemistry from basic research to useful applications,this review attempts to make it easier to integrate ML into electrochemical oxidation.展开更多
An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） det...An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） detection compared to the ERGO-12v （GO applied to a negative potential of-1.2 V）, GO, chemically reduced GO （CRGO）-modified glassy carbon electrode （GC） and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode （GC/ERGO-0.8v） were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared （FT-IR）, Raman, and X-ray photoelectron spectroscopies （XPS） demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.展开更多
The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different o...The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.展开更多
The treatment of biologically treated wastewater of coffee-curing industry by the electrochemical oxidation using steel anode was investigated. Bench-scale experiments were conducted for activated sludge process on ra...The treatment of biologically treated wastewater of coffee-curing industry by the electrochemical oxidation using steel anode was investigated. Bench-scale experiments were conducted for activated sludge process on raw wastewater and the treated effluents were further treated by electrochemical oxidation method for its colour and organic content removal. The efficiency of the process was determined in terms of removal percentage of COD, BOD and colour during the course of reaction. Several operating parameters like time, pH and current density were examined to ascertain their effects on the treatment efficiency. Steel anode was found to be effective for the COD and colour removal with anode efficiency of 0.118 kgCOD\5h -1\5A -1\5m -2 and energy consumption 20.61 kWh\5kg -1 of COD at pH 9. The decrease in pH from 9 to 3 found to increase the anode efficiency from 0.118 kgCOD\5h -1\5A -1\5m -2 to 0.144 kWh\5kg -1 of COD while decrease the energy consumption from 20.61 kWh\5kg -1 of COD to 12.86 kWh\5kg -1 of COD. The pH of 5 was considered an ideal from the present treatment process as it avoids the addition of chemicals for neutralization of treated effluents and also economical with respect to energy consumption. An empirical relation developed for relationship between applied current density and COD removal efficiency showed strong predictive capability with coefficient of determination of 96.5%.展开更多
A PbO2/Sb-SnO2/TiO2 nanotube array composite electrode was successfully synthesized and its electrochemical oxidation properties were investigated.Field-emission scanning electron microscopy(FE-SEM)and X-ray diffracti...A PbO2/Sb-SnO2/TiO2 nanotube array composite electrode was successfully synthesized and its electrochemical oxidation properties were investigated.Field-emission scanning electron microscopy(FE-SEM)and X-ray diffraction(XRD)results showed that the PbO2 coating was composed of anα-PbO2 inner layer and aβ-PbO2 outer layer.Accelerated life measurement indicated that the composite electrode had a lifetime of 815 h.Rhodamine B(RhB)was employed as a model pollutant to analyze the electrocatalytic activity of the electrode.The effects of initial RhB concentration,current density,initial pH,temperature,and chloride ion concentration on the electrochemical oxidation were investigated in detail.Inductively coupled plasma atomic emission spectroscopy(ICP-AES)results suggested that the concentration of leached Pb^2+in the electrolyte during the electrocatalytic oxidation process can be neglected.Finally,the degradation mechanism during the electrocatalytic oxidation process was proposed based on the results of solid-phase micro-extraction-gas chromatography-mass spectrometry(SPME-GC-MS).The high electrocatalytic performance of the composite electrode makes it a promising anode for the treatment of organic pollutants in aqueous solution.展开更多
Biologically-treated municipal solid waste （MSW） leachate still contains many kinds of bit-recalcitrant organic matter. A new plate and frame electrochemical reactor was designed to treat these materials under flow ...Biologically-treated municipal solid waste （MSW） leachate still contains many kinds of bit-recalcitrant organic matter. A new plate and frame electrochemical reactor was designed to treat these materials under flow conditions. In the electrochemical oxidation process, NH3 and color could be easily removed by means of electro-generated chlorinefaypochlorite within 20 min. The effects of major process parameters on the removal of organic pollutants were investigated systematically. Under experimental conditions, the optimum operation parameters were current density of 65 mA/cm^2, flow velocity of 2.6 cm/sec in electrode gap, and initial chloride ion concentration of 5000 mg/L. The COD in the leachate could be reduced below 100 mg/L after 1 hr of treatment. The kinetics and mechanism of COD removal were investigated by simultaneously monitoring the COD change and chlorine/hypochlorite production. The kinetics of COD removal exhibited a two-stage kinetic model, and the decrease of electro-generated chlorine/hypochlorite production was the major mechanism for the slowing down of the COD removal rate in the second stage. The narrowing of the electrode gap is beneficial for COD removal and energy consumption.展开更多
In this study,the electrochemical oxidation of reactive brilliant orange X-GN dye with a boron-doped diamond(BDD)anode was investigated.The BDD electrodes were deposited on the niobium(Nb)substrates by the hot filamen...In this study,the electrochemical oxidation of reactive brilliant orange X-GN dye with a boron-doped diamond(BDD)anode was investigated.The BDD electrodes were deposited on the niobium(Nb)substrates by the hot filament chemical vapor deposition method.The effects of processing parameters,such as film thickness,current density,supporting electrolyte concentration,initial solution pH,solution temperature,and initial dye concentration,were evaluated following the variation in the degradation efficiency.The microstructure and the electrochemical property of BDD were characterized by scanning electron microscopy,Raman spectroscopy,and electrochemical workstation;and the degradation of X-GN was estimated using UV-Vis spectrophotometry.Further,the results indicated that the film thickness of BDD had a significant impact on the electrolysis of X-GN.After 3 h of treatment,100%color and 63.2%total organic carbon removal was achieved under optimized experimental conditions:current density of 100 mA/cm2,supporting electrolyte concentration of 0.05 mol/L,initial solution pH 3.08,and solution temperature of 60°C.展开更多
The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide（F--PbO2） electrode for ...The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide（F--PbO2） electrode for the degradation of aniline was compared with that of undoped lead dioxide（PbO2） electrode by ultraviolet-visible（UV-Vis） spectroscopy,linear voltammetry and other analytical methods,such as the measurement by chemical oxygen demand analyzer,high performance liquid chromatography and scanning electron micrography.It was shown that both PbO2 electrode and F--PbO2 electrode could make aniline be mineralized completely and have the same degradation course,but F--PbO2 electrode has much higher electrocatalytic activity than undoped PbO2 electrode for the electrochemical degradation of aniline.The experimental results confirm that F--PbO2 electrode has much higher potential for oxygen evolution than undoped PbO2 electrode.展开更多
The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2...The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2 FTS were tested on the Ti/SnO2–Sb2O5–Bi2O3anode. The effects of current density,potential,and supporting electrolyte on the degradation of 6：2 FTS were evaluated. Experimental results showed that 6：2 FTS was more easily degraded than PFOS on the Ti/SnO2–Sb2O5–Bi2O3anode. At a low current density of 1.42 mA/cm2,6：2 FTS was not degraded on Ti/SnO2–Sb2O5–Bi2O3,while the degradation ratio increased when the current density ranged from 4.25 to 6.80 mA/cm2. The degradation of 6：2 FTS at current density of 6.80 mA/cm2 followed pseudo first-order kinetics with the rate constant of 0.074 hr-1. The anodic potential played an important role in the degradation of 6：2 FTS,and the pseudo first-order rate constants increased with the potential. The surface of Ti/SnO2–Sb2O5–Bi2O3was contaminated after electrolysis at constant potential of 3 V,while the fouling phenomenon was not observed at 5 V. The fouled anode could be regenerated by incinerating at 600°C. The intermediates detected by ultra-performance liquid chromatography coupled with a triple-stage quadrupole mass spectrometer（UPLC–MS/MS） were shorter chain perfluorocarboxylic acids. The 6：2 FTS was first attacked by hydroxyl radical,and then formed perfluorinated carboxylates,which decarboxylated and removed CF2 units to yield shorter-chain perfluorocarboxylic acids.展开更多
The indirect dectrechemical oxidation of 4-amino-dimethyl-aniline hydrochloride containing wastewater generated from vanillin production is presented. Experiments were conducted at a constant current density of 30 rnA...The indirect dectrechemical oxidation of 4-amino-dimethyl-aniline hydrochloride containing wastewater generated from vanillin production is presented. Experiments were conducted at a constant current density of 30 rnA/cm^2 via a Ti/Bu-Ti-Sn ternary oxide coated anode and an undivided reactor. During the various stages of the electrolysis, parameters such as the values of chemical oxygen demand（COD） and total organic carbon（TOC） were determined in order to evaluate the feasibility of the electrochemical treatment. The energy consumption and the current efficiency during the electrolysis were calculated. The present study proves the effectiveness of the electrochemical treatment for wastewater resulted from vanillin production.展开更多
In this study,the Ti/SnO_(2)-RuO_(2) electrodes with different Yb contents were prepared by sol-gel method and thermal decomposition method,and the surface morphology and crystal structure of the electrodes were chara...In this study,the Ti/SnO_(2)-RuO_(2) electrodes with different Yb contents were prepared by sol-gel method and thermal decomposition method,and the surface morphology and crystal structure of the electrodes were characterized by scanning electron microscopy(SEM),atomic force microscopy(AFM) and X-ray diffraction(XRD),the electrochemical properties of the electrodes were tested by linear sweep voltammetry(LSV) and cyclic voltammetry(CV).The electrochemical oxidation device was constructed with Yb-doped Ti/SnO_(2)-RuO_(2) electrode as the anode and titanium plate as the cathode,and the electrochemical oxidation effect and product changes of the anode on co king wastewater were investigated.The results show that the surface of the electrode is flat with high crystallinity of SnO_(2) and RuO_(2) crystals at1.5% Yb doping,and the LSV and CV curves indicate that the Yb doping of 1.5% increases the oxygen precipitation potential and electrocatalytic oxidation activity of the electrode.When the electrode with Yb doping of 1.5% is the anode with current density of 10 mA/cm^(2) electrochemical oxidation time of 30 min,the electrode can remove chemical oxygen demand(COD) up to 85.06%,total organic carbon(TOC) up to 60.59% and UV_(254) from 1.594 to 0.507 for coking wastewater.Gas chromatography(GC-MS),UV-vis and three-dimensional fluorescence results of coking wastewater before and after treatment show that large toxic substances in coking wastewater are degraded to low toxic organic substances,and most soluble organic substances are degraded and transformed.This study provides the possibility of basic research for the engineering practice of electrochemical oxidation for the treatment of coking wastewater.展开更多
The generation and transformation of radicals on the cathode of indirect electrochemical oxidation were studied by chemilumines- cence(CL)and UV-Visible spectra in the reactor with a salt bridge that connected the sep...The generation and transformation of radicals on the cathode of indirect electrochemical oxidation were studied by chemilumines- cence(CL)and UV-Visible spectra in the reactor with a salt bridge that connected the separated chambers.The CL intensity of 4×10^(-9)mol/L luminol on the cathode with bubbling oxygen was about seven times that of the intensity without it,which was because of the generation of reactive oxygen species(ROS).The existence of ROS,especially the generation of the superoxide radical,coul...展开更多
This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-...This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-multi-wailed carbon nanotubes-epoxy （AgZMWCNT） composites electrodes. The composite electrodes were obtained using two-roll mill procedure. SEM images of surfaces of the composites revealed a homogeneous distribution of the composite components within the epoxy matrix. AgZMWCNT composite electrode exhibited the better electrical conductivity and larger electroactive surface area. The electrochemical determination of ibuprofen （IBP） was achieved using AgZMWCNT by cyclic voltammetry, differential-pulsed voltammetry, square-wave voltammetry and chronoamperometry. The IBP degradation occurred on both composite electrodes under controlled electrolysis at 1.2 and 1.75 V vs. Ag/AgCl, and IBP concentration was determined comparatively by differential-pulsed voltammetry, under optimized conditions using AgZMWCNT electrode and UV-Vis spectrophotometry methods to determine the IBP degradation performance for each electrode. AgZMWCNT electrode exhibited a dual character allowing a double application in IBP degradation process and its control.展开更多
Developing highly efficient and cost-effective catalysts for electrochemically oxidizing biomass-derived 5-hydroxymethylfurfural(HMF)into value-added 2,5-furandicarboxylic acid(FDCA)is of great importance.Herein,we re...Developing highly efficient and cost-effective catalysts for electrochemically oxidizing biomass-derived 5-hydroxymethylfurfural(HMF)into value-added 2,5-furandicarboxylic acid(FDCA)is of great importance.Herein,we report a controllable nitrogen doping strategy to significantly improve the catalytic activity of Co_(3)O_(4)nanowires for highly selective electro-oxidation of HMF into FDCA.The nitrogen doping leads to the generation of defects including nitrogen dopants and oxygen vacancies in Co_(3)O_(4)nanowires,which is conducive to the formation of catalytically active sites.As a result,the electro-oxidation potential for HMF is only 1.38 V(vs.RHE)when the current density reaches 50 mA/cm^(2).More importantly,the conversion rate of HMF is as high as 99.5%,and the yield of FDCA is up to 96.4%.展开更多
The electrochemical oxidation of L-cysteine in an SDS/BA/H_2O microemulsion system was studied with the methods of ultramicroelectrode cyclic voltammetry and AC impedance. The catalytic efficiency of the microemulsion...The electrochemical oxidation of L-cysteine in an SDS/BA/H_2O microemulsion system was studied with the methods of ultramicroelectrode cyclic voltammetry and AC impedance. The catalytic efficiency of the microemulsion on the electrochemical oxidation increases with the increase of BA or SDS content, but decreases with the increase of the water content because of the effects of BA, SDS and water on the solubilization of L-cysteine in the microemulsion. Furthermore, the catalytic efficiency of the bicontinuous structure is greater than that of an O/W microemulsion system. The results derived from both the rate constant k0 and Gibbs free energy ΔG≠ accord with those from the catalytic efficiency.展开更多
The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current ...The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current densities, space sizes between the two electrodes, and amounts of added NaCl on ammonia-containing wastewater treatm.ent. It was shown that, after a 30-min treatment under the optimal conditions, which were a current density of 20 mA/cm2, a space size between the two electrodes of I cm, and an added amount of 0.5 g/L of NaC1, the COD concentration in municipal wastewater was 40 mg/L, a removal rate of 90%; and the NH3-N concentration was 7 mg/L, a removal rate of 88.3%. The effluent of municipal wastewater qualified for Class A of the Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant （GB 18918-2002）.展开更多
By using a self-made carbon/polytetrafluoroethylene （C/PTFE） O2-fed as cathode and Ti/IrO2/RuO2 as anode, the effects of electrochemical oxidation of phenol and the coal-gas wastewater containing phenol were studied...By using a self-made carbon/polytetrafluoroethylene （C/PTFE） O2-fed as cathode and Ti/IrO2/RuO2 as anode, the effects of electrochemical oxidation of phenol and the coal-gas wastewater containing phenol were studied. The terylene diaphragm which kept pH〉12 in cathodic compartment and pH〈1 in the anodic compartment was selected in the experiment in comparison with the other types of diaphragm. Furthermore, hydroxyl radical （HO·） was determined in the cathodic compartment of the diaphragm cell by electron spin resonance spectrum（ESR） and the fluorescence spectra. Compared with pH, the accumulated HzO2 and the COD removal of the no-diaphragm cell, the mechanism of electrochemical oxidation in the terylene diaphragm cell was supposed. The degradation of phenol was supposed to be cooperative oxidation by direct or indirect electrochemical oxidation at the anode and H2O2, HO· produced by oxygen reduction at the cathode. The mineralization of phenol in the diaphragm cell was better than that in the no-diaphragm cell. When the coal-gas wastewater was treated by the electrolysis system with terylene diaphragm, the average removal efficiency of the volatile phenol and COD were 100% and 79.6%, respectively.展开更多
基金supported by the National Natural Science Foundation of China(No.51709103)the Natural Science Foundation of Hunan Province,China(Nos.2018JJ3242 and 2021JJ30362)the Science and Technology Innovation Leading Plan of High Tech Industry in Hunan Province(No.2021GK4055).
文摘The global concern surrounding the advancement of methods for treating wastewater and polluted soil has markedly increased over time.While electrochemical advanced oxidation processes(EAOPs)and biotreatments are commonly employed technologies for remediating wastewater and polluted soil,their widespread adoption is hindered by their limitations,which include high costs associated with EAOPs and prolonged remediation time of biotreatments.In the review,we provided an overviewof EAOP technology and biotreatment,emphasizing the critical aspects involved in building a combined system.This review systematically evaluates recent research that combines EAOPswith bioremediation for treating wastewater or contaminated soil as pretreatment or post-treatment process.Research findings suggest that the combined treatment method represents a promising and competitive technology that can overcome some of the limitations of individual treatments.Additionally,we discussed the potential applications of this technology in varying levels of wastewater and soil pollution,as well as the underlying combination mechanisms.
基金financially supported by National Key R&D Program International Cooperation Project(2023YFE0108100)Natural Science Foundation of China(No.52170085)+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
基金the National Science Foundation of China(No.22071058)the Fundamental Research Funds for the Central Universities for financial support。
文摘The direct difunctionalization of alkenes serves as one of the most straightforward strategies toward complex nitrogen-containing compounds.The existing approach is extensively promoted by using C/Xcentered radicals and N-nucleophiles to conduct 1,2-difunctional amination/azolization of alkenes.In contrast,2,1-difunctional amination/azolization of alkenes by using nitrogen-centered radicals(NCRs) and nucleophiles still remains rarely underexplored.It is possibly due to the highly active electron properties of NCRs and the relatively poor nucleophilicity of aromatic NCRs to be trapped by arylalkenes.Herein,we demonstrate an unprecedented 2,1-hydroxazolization reactions of arylalkenes through electrochemically enabled addition of NCRs from azoles and nucleophiles(NuH) in high yields and with high regioselectivity.This conversion is characterized by the fact that neither metal catalysts nor external chemical oxidants are required.This electrochemical oxidation synthesis method can also be applied for a broad range of NuH including pyridine hydrofluoride,ammonia,water,alcohols,and acids which enables the formation of C-N and C-X(X=F/N/O) bonds in one-pot fashion to furnish efficient fluoroamination,diamination and oxoamination of alkenes.
基金funding from the National Natural Science Foundation of China(Nos.22122606,22076142,62276190)National Key Basic Research Program of China(No.2017YFA0403402)+2 种基金National Natural Science Foundation of China(No.U1932119)the Science&Technology Commission of Shanghai Municipality(No.14DZ2261100)the Fundamental Research Funds for the Central Universities。
文摘In recent years,machine learning(ML)techniques have demonstrated a strong ability to solve highly complex and non-linear problems by analyzing large datasets and learning their intrinsic patterns and relationships.Particularly in chemical engineering and materials science,ML can be used to discover microstructural composition,optimize chemical processes,and create novel synthetic pathways.Electrochemical processes offer the advantages of precise process control,environmental friendliness,high energy conversion efficiency and low cost.This review article provides the first systematic summary of ML in the application of electrochemical oxidation,including pollutant removal,battery remediation,substance synthesis and material characterization prediction.Hot trends at the intersection of ML and electrochemical oxidation were analyzed through bibliometrics.Common ML models were outlined.The role of ML in improving removal efficiency,optimizing experimental conditions,aiding battery diagnosis and predictive maintenance,and revealing material characterization was highlighted.In addition,current issues and future perspectives were presented in relation to the strengths and weaknesses of ML algorithms applied to electrochemical oxidation.In order to further support the sustainable growth of electrochemistry from basic research to useful applications,this review attempts to make it easier to integrate ML into electrochemical oxidation.
基金supported by the National Natural Science Foundation of China(21007033)the Fundamental Research Funds of Shandong University(2015JC017)~~
文摘An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） detection compared to the ERGO-12v （GO applied to a negative potential of-1.2 V）, GO, chemically reduced GO （CRGO）-modified glassy carbon electrode （GC） and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode （GC/ERGO-0.8v） were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared （FT-IR）, Raman, and X-ray photoelectron spectroscopies （XPS） demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.
基金the financial support from the National Natural Science Foundation of China(No. 51878423)Graduate Student’s Research and Innovation Fund of Sichuan University(No.2018YJSY075)
文摘The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.
文摘The treatment of biologically treated wastewater of coffee-curing industry by the electrochemical oxidation using steel anode was investigated. Bench-scale experiments were conducted for activated sludge process on raw wastewater and the treated effluents were further treated by electrochemical oxidation method for its colour and organic content removal. The efficiency of the process was determined in terms of removal percentage of COD, BOD and colour during the course of reaction. Several operating parameters like time, pH and current density were examined to ascertain their effects on the treatment efficiency. Steel anode was found to be effective for the COD and colour removal with anode efficiency of 0.118 kgCOD\5h -1\5A -1\5m -2 and energy consumption 20.61 kWh\5kg -1 of COD at pH 9. The decrease in pH from 9 to 3 found to increase the anode efficiency from 0.118 kgCOD\5h -1\5A -1\5m -2 to 0.144 kWh\5kg -1 of COD while decrease the energy consumption from 20.61 kWh\5kg -1 of COD to 12.86 kWh\5kg -1 of COD. The pH of 5 was considered an ideal from the present treatment process as it avoids the addition of chemicals for neutralization of treated effluents and also economical with respect to energy consumption. An empirical relation developed for relationship between applied current density and COD removal efficiency showed strong predictive capability with coefficient of determination of 96.5%.
基金supported by the National Natural Science Foundation of China(21507104)Natural Science Basic Research Plan in Shaanxi Province of China(2017JM2015)~~
文摘A PbO2/Sb-SnO2/TiO2 nanotube array composite electrode was successfully synthesized and its electrochemical oxidation properties were investigated.Field-emission scanning electron microscopy(FE-SEM)and X-ray diffraction(XRD)results showed that the PbO2 coating was composed of anα-PbO2 inner layer and aβ-PbO2 outer layer.Accelerated life measurement indicated that the composite electrode had a lifetime of 815 h.Rhodamine B(RhB)was employed as a model pollutant to analyze the electrocatalytic activity of the electrode.The effects of initial RhB concentration,current density,initial pH,temperature,and chloride ion concentration on the electrochemical oxidation were investigated in detail.Inductively coupled plasma atomic emission spectroscopy(ICP-AES)results suggested that the concentration of leached Pb^2+in the electrolyte during the electrocatalytic oxidation process can be neglected.Finally,the degradation mechanism during the electrocatalytic oxidation process was proposed based on the results of solid-phase micro-extraction-gas chromatography-mass spectrometry(SPME-GC-MS).The high electrocatalytic performance of the composite electrode makes it a promising anode for the treatment of organic pollutants in aqueous solution.
基金supported by the special action project "Saving energy and reducing emission" of Chongqing City( No.CSTC2010AA7060)the National Natural Science Foundation of China (No.21176273)
文摘Biologically-treated municipal solid waste （MSW） leachate still contains many kinds of bit-recalcitrant organic matter. A new plate and frame electrochemical reactor was designed to treat these materials under flow conditions. In the electrochemical oxidation process, NH3 and color could be easily removed by means of electro-generated chlorinefaypochlorite within 20 min. The effects of major process parameters on the removal of organic pollutants were investigated systematically. Under experimental conditions, the optimum operation parameters were current density of 65 mA/cm^2, flow velocity of 2.6 cm/sec in electrode gap, and initial chloride ion concentration of 5000 mg/L. The COD in the leachate could be reduced below 100 mg/L after 1 hr of treatment. The kinetics and mechanism of COD removal were investigated by simultaneously monitoring the COD change and chlorine/hypochlorite production. The kinetics of COD removal exhibited a two-stage kinetic model, and the decrease of electro-generated chlorine/hypochlorite production was the major mechanism for the slowing down of the COD removal rate in the second stage. The narrowing of the electrode gap is beneficial for COD removal and energy consumption.
基金Project(2016YEB0301402) supported by the National Key Research and Development Program of ChinaProject(51601226) supported by the National Natural Science Foundation of China+1 种基金Project supported by the Open-End Fund for the Valuable and Precision Instruments of Central South University,ChinaProject supported by State Key Laboratory of Powder Metallurgy,China
文摘In this study,the electrochemical oxidation of reactive brilliant orange X-GN dye with a boron-doped diamond(BDD)anode was investigated.The BDD electrodes were deposited on the niobium(Nb)substrates by the hot filament chemical vapor deposition method.The effects of processing parameters,such as film thickness,current density,supporting electrolyte concentration,initial solution pH,solution temperature,and initial dye concentration,were evaluated following the variation in the degradation efficiency.The microstructure and the electrochemical property of BDD were characterized by scanning electron microscopy,Raman spectroscopy,and electrochemical workstation;and the degradation of X-GN was estimated using UV-Vis spectrophotometry.Further,the results indicated that the film thickness of BDD had a significant impact on the electrolysis of X-GN.After 3 h of treatment,100%color and 63.2%total organic carbon removal was achieved under optimized experimental conditions:current density of 100 mA/cm2,supporting electrolyte concentration of 0.05 mol/L,initial solution pH 3.08,and solution temperature of 60°C.
基金Supported by the National Natural Science Foundation of China(No.20873051)the High-tech Research and Development Program of China(No.2006AA06Z321)the Natural Science Foundation of Jiangsu Province,China(No.BK2008555)
文摘The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide（F--PbO2） electrode for the degradation of aniline was compared with that of undoped lead dioxide（PbO2） electrode by ultraviolet-visible（UV-Vis） spectroscopy,linear voltammetry and other analytical methods,such as the measurement by chemical oxygen demand analyzer,high performance liquid chromatography and scanning electron micrography.It was shown that both PbO2 electrode and F--PbO2 electrode could make aniline be mineralized completely and have the same degradation course,but F--PbO2 electrode has much higher electrocatalytic activity than undoped PbO2 electrode for the electrochemical degradation of aniline.The experimental results confirm that F--PbO2 electrode has much higher potential for oxygen evolution than undoped PbO2 electrode.
基金supported by the National Natural Science Foundation of China (No.21307036)the National High-Tech Research and Development Program of China (No.2013AA062705)the National Key Scientific and Technological Project for Water Pollution Control and Management (Nos.2012ZX07206-002,2012ZX07206-003)
文摘The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2 FTS were tested on the Ti/SnO2–Sb2O5–Bi2O3anode. The effects of current density,potential,and supporting electrolyte on the degradation of 6：2 FTS were evaluated. Experimental results showed that 6：2 FTS was more easily degraded than PFOS on the Ti/SnO2–Sb2O5–Bi2O3anode. At a low current density of 1.42 mA/cm2,6：2 FTS was not degraded on Ti/SnO2–Sb2O5–Bi2O3,while the degradation ratio increased when the current density ranged from 4.25 to 6.80 mA/cm2. The degradation of 6：2 FTS at current density of 6.80 mA/cm2 followed pseudo first-order kinetics with the rate constant of 0.074 hr-1. The anodic potential played an important role in the degradation of 6：2 FTS,and the pseudo first-order rate constants increased with the potential. The surface of Ti/SnO2–Sb2O5–Bi2O3was contaminated after electrolysis at constant potential of 3 V,while the fouling phenomenon was not observed at 5 V. The fouled anode could be regenerated by incinerating at 600°C. The intermediates detected by ultra-performance liquid chromatography coupled with a triple-stage quadrupole mass spectrometer（UPLC–MS/MS） were shorter chain perfluorocarboxylic acids. The 6：2 FTS was first attacked by hydroxyl radical,and then formed perfluorinated carboxylates,which decarboxylated and removed CF2 units to yield shorter-chain perfluorocarboxylic acids.
文摘The indirect dectrechemical oxidation of 4-amino-dimethyl-aniline hydrochloride containing wastewater generated from vanillin production is presented. Experiments were conducted at a constant current density of 30 rnA/cm^2 via a Ti/Bu-Ti-Sn ternary oxide coated anode and an undivided reactor. During the various stages of the electrolysis, parameters such as the values of chemical oxygen demand（COD） and total organic carbon（TOC） were determined in order to evaluate the feasibility of the electrochemical treatment. The energy consumption and the current efficiency during the electrolysis were calculated. The present study proves the effectiveness of the electrochemical treatment for wastewater resulted from vanillin production.
基金Project supported by Natural Science Foundation of Inner Mongolia(2018LH04003,2020MS05047)Inner Mongolia Autonomous Region Science Technology Plan Project(201702100)+1 种基金Inner Mongolia Autonomous Region Results Transfer Project(2019CG075)。
文摘In this study,the Ti/SnO_(2)-RuO_(2) electrodes with different Yb contents were prepared by sol-gel method and thermal decomposition method,and the surface morphology and crystal structure of the electrodes were characterized by scanning electron microscopy(SEM),atomic force microscopy(AFM) and X-ray diffraction(XRD),the electrochemical properties of the electrodes were tested by linear sweep voltammetry(LSV) and cyclic voltammetry(CV).The electrochemical oxidation device was constructed with Yb-doped Ti/SnO_(2)-RuO_(2) electrode as the anode and titanium plate as the cathode,and the electrochemical oxidation effect and product changes of the anode on co king wastewater were investigated.The results show that the surface of the electrode is flat with high crystallinity of SnO_(2) and RuO_(2) crystals at1.5% Yb doping,and the LSV and CV curves indicate that the Yb doping of 1.5% increases the oxygen precipitation potential and electrocatalytic oxidation activity of the electrode.When the electrode with Yb doping of 1.5% is the anode with current density of 10 mA/cm^(2) electrochemical oxidation time of 30 min,the electrode can remove chemical oxygen demand(COD) up to 85.06%,total organic carbon(TOC) up to 60.59% and UV_(254) from 1.594 to 0.507 for coking wastewater.Gas chromatography(GC-MS),UV-vis and three-dimensional fluorescence results of coking wastewater before and after treatment show that large toxic substances in coking wastewater are degraded to low toxic organic substances,and most soluble organic substances are degraded and transformed.This study provides the possibility of basic research for the engineering practice of electrochemical oxidation for the treatment of coking wastewater.
文摘The generation and transformation of radicals on the cathode of indirect electrochemical oxidation were studied by chemilumines- cence(CL)and UV-Visible spectra in the reactor with a salt bridge that connected the separated chambers.The CL intensity of 4×10^(-9)mol/L luminol on the cathode with bubbling oxygen was about seven times that of the intensity without it,which was because of the generation of reactive oxygen species(ROS).The existence of ROS,especially the generation of the superoxide radical,coul...
基金supported by the strategic grant POSDRU/88/1.5/S/50783POSDRU/21/1.5/G/13798+1 种基金POSDRU/89/1.5/S/57649 co-financed by the European Social Fund - Investing in People,within the Sectoral Operational Programme Human Resources Development 2007-2013partially by the PN II-RU-PD129/2010 and PN II Ideas 165/2011
文摘This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-multi-wailed carbon nanotubes-epoxy （AgZMWCNT） composites electrodes. The composite electrodes were obtained using two-roll mill procedure. SEM images of surfaces of the composites revealed a homogeneous distribution of the composite components within the epoxy matrix. AgZMWCNT composite electrode exhibited the better electrical conductivity and larger electroactive surface area. The electrochemical determination of ibuprofen （IBP） was achieved using AgZMWCNT by cyclic voltammetry, differential-pulsed voltammetry, square-wave voltammetry and chronoamperometry. The IBP degradation occurred on both composite electrodes under controlled electrolysis at 1.2 and 1.75 V vs. Ag/AgCl, and IBP concentration was determined comparatively by differential-pulsed voltammetry, under optimized conditions using AgZMWCNT electrode and UV-Vis spectrophotometry methods to determine the IBP degradation performance for each electrode. AgZMWCNT electrode exhibited a dual character allowing a double application in IBP degradation process and its control.
基金supported by the National Natural Science Foundation of China(Nos.22075159 and 21775078)Youth Innovation Team Project of Shandong Provincial Education Department(No.2019KJC023)。
文摘Developing highly efficient and cost-effective catalysts for electrochemically oxidizing biomass-derived 5-hydroxymethylfurfural(HMF)into value-added 2,5-furandicarboxylic acid(FDCA)is of great importance.Herein,we report a controllable nitrogen doping strategy to significantly improve the catalytic activity of Co_(3)O_(4)nanowires for highly selective electro-oxidation of HMF into FDCA.The nitrogen doping leads to the generation of defects including nitrogen dopants and oxygen vacancies in Co_(3)O_(4)nanowires,which is conducive to the formation of catalytically active sites.As a result,the electro-oxidation potential for HMF is only 1.38 V(vs.RHE)when the current density reaches 50 mA/cm^(2).More importantly,the conversion rate of HMF is as high as 99.5%,and the yield of FDCA is up to 96.4%.
文摘The electrochemical oxidation of L-cysteine in an SDS/BA/H_2O microemulsion system was studied with the methods of ultramicroelectrode cyclic voltammetry and AC impedance. The catalytic efficiency of the microemulsion on the electrochemical oxidation increases with the increase of BA or SDS content, but decreases with the increase of the water content because of the effects of BA, SDS and water on the solubilization of L-cysteine in the microemulsion. Furthermore, the catalytic efficiency of the bicontinuous structure is greater than that of an O/W microemulsion system. The results derived from both the rate constant k0 and Gibbs free energy ΔG≠ accord with those from the catalytic efficiency.
基金supported by the Eleventh Five-Year Key Technology Research and Development Program in China (Grant No. 2006BAJ08B04)
文摘The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current densities, space sizes between the two electrodes, and amounts of added NaCl on ammonia-containing wastewater treatm.ent. It was shown that, after a 30-min treatment under the optimal conditions, which were a current density of 20 mA/cm2, a space size between the two electrodes of I cm, and an added amount of 0.5 g/L of NaC1, the COD concentration in municipal wastewater was 40 mg/L, a removal rate of 90%; and the NH3-N concentration was 7 mg/L, a removal rate of 88.3%. The effluent of municipal wastewater qualified for Class A of the Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant （GB 18918-2002）.
文摘By using a self-made carbon/polytetrafluoroethylene （C/PTFE） O2-fed as cathode and Ti/IrO2/RuO2 as anode, the effects of electrochemical oxidation of phenol and the coal-gas wastewater containing phenol were studied. The terylene diaphragm which kept pH〉12 in cathodic compartment and pH〈1 in the anodic compartment was selected in the experiment in comparison with the other types of diaphragm. Furthermore, hydroxyl radical （HO·） was determined in the cathodic compartment of the diaphragm cell by electron spin resonance spectrum（ESR） and the fluorescence spectra. Compared with pH, the accumulated HzO2 and the COD removal of the no-diaphragm cell, the mechanism of electrochemical oxidation in the terylene diaphragm cell was supposed. The degradation of phenol was supposed to be cooperative oxidation by direct or indirect electrochemical oxidation at the anode and H2O2, HO· produced by oxygen reduction at the cathode. The mineralization of phenol in the diaphragm cell was better than that in the no-diaphragm cell. When the coal-gas wastewater was treated by the electrolysis system with terylene diaphragm, the average removal efficiency of the volatile phenol and COD were 100% and 79.6%, respectively.
