The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived alde...The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining,and has become a frontier of mainstream research.This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes(5-hydroxymethylfurfural,furfural,glucose,xylose,vanillin and benzaldehyde,etc.).The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde.It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies,catalyst stability,and reaction scalability remain,but the rapid progress offers hope for future advancements.Finally,we elucidate the challenges in this domain and provide the perspectives on future developments.This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.展开更多
Addressing the contamination of antibiotics has attracted ever-increasing and imperative attention due to their widespread existence,easy-to-cause drug-resistant bacteria infection,coupled with their intrinsic toxicit...Addressing the contamination of antibiotics has attracted ever-increasing and imperative attention due to their widespread existence,easy-to-cause drug-resistant bacteria infection,coupled with their intrinsic toxicity and hazard to environments and human health.Herein,a novel CC/CoNi-LDH-10%Ce anode material was directly constructed through a simple and rapid electrodeposition strategy,serving as an efficacious electrocatalyst for removing ciprofloxacin(CIP)from aqueous solution.Such novel CC/CoNi-LDH-10%Ce anode delivered a higher charge transfer,relatively abundant oxygen vacancies,and a higher electrochemical active area.The as-fabricated CC/CoNi-LDH-10%Ce electrode achieved a substantially boosted CIP removal efficiency of 52.5%relative to that of pure CC at about 23.9%.Notably,doping an appropriate amount of Ce^(3+)can endow the pristine CC/CoNi-LDH with richer oxygen vacancies and excellent electrocatalytic performance.Additionally,the electrocatalytic oxidation of CIP was attributed to both direct oxidation on the electrode surface and indirect oxidation induced by the generated active species(superoxide radicals and hydroxyl radicals).This study provides a simple,universal and flexible tactic for other researchers in designing and manufacturing avenues of electrodes.展开更多
The organic pollutants,such as quaternary ammonium compounds,in high salinity flowback water from shale gas extraction may pose a severe risk to public health.Conventional biological technologies have limited effectiv...The organic pollutants,such as quaternary ammonium compounds,in high salinity flowback water from shale gas extraction may pose a severe risk to public health.Conventional biological technologies have limited effectiveness in the treatment of high-salt wastewaters,whereas electrocatalytic oxidation has shown potential for treating organic pollutants in high-salt flowback water.This study developed a carbon nanotubes(CNTs)doped Ru/Ir oxide coated Ti electrode CNTs-(Ru_(x)Ir_(y)O_(2))/Ti,which exhibited enhanced electrocatalytic performance for the treatment of quaternary ammonium compound in high-salt wastewater compared to the control metal oxide coated Ti anode(Ru_(x)Ir_(y)O_(2))/Ti,with pseudofirst-order reaction rate constant improved from 7.36×10^(-3) to 1.12×10^(-2) min−1.Moreover,the CNTs-(Ru_(x)Ir_(y)O_(2))/Ti anode electrocatalytic oxidation system exhibited excellent cycling stability.Mechanism studies indicated that the CNTs-(Ru_(x)Ir_(y)O_(2))/Ti electrode enhanced singlet oxygen(^(1)O_(2))generation,which played a major role in pollutant degradation.Furthermore,the formation of high concentrations of HClO and H_(2)O_(2) further facilitated the generation of ^(1)O_(2).This study may provide an efficient and green technology for the treatment of organic pollutants in high-salt shale gas flowback water.展开更多
Electrocatalytic toluene(TL)oxidation to produce benzoic acid(BAC)process is largely hindered due to sluggish kinetics associated with the transformation of the rate-determining step,because of weak TL adsorption and ...Electrocatalytic toluene(TL)oxidation to produce benzoic acid(BAC)process is largely hindered due to sluggish kinetics associated with the transformation of the rate-determining step,because of weak TL adsorption and high rate-determining step energy barrier for difficult to dehydrogenate.Herein,we report Mn_(x)Ce_(1-x)O_(2)/CNT catalyst for accelerated reaction kinetics.Theoretical and experimental studies indicate that Ce sites promote TL adsorption and polyvalent Mn modulates the electronic structure of Ce sites reducing the rate-determining step energy barrier.This results in increasing^(*)C_(6)H_(5)CH_(2)coverage and effectively accelerating TL oxidation reaction(TOR)kinetics.Excitingly,the Faraday efficiency(FE)and BAC yield of optimized Mn_(0.6)Ce_(0.4)O_(2)/CNT at 2.6 V vs.RHE could reach 85.9%and 653.9 mg h^(-1)cm^(-2),respectively.In addition,the Mn_(0.6)Ce_(0.4)O_(2)/CNT displays a high selectivity of 96.3%for BAC.Combining the TL oxidation reaction with hydrogen evolution reaction,the anion exchange membrane electrolyzer of Mn_(0.6)Ce_(0.4)O_(2)/CNT(+)||Pt/C(-)can reach 100 mA cm^(-2)at the voltage of 3.0 V,in which the BAC yield is 579.4 mg h^(-1)cm^(-2)and the FE is 83.6%.This work achieved high selectivity of TOR at industrial-relevant current densities of 100 mA cm^(-2)at the low voltage for the first time.展开更多
In this work,synthesis of Ni nanoparticles was carried out successfully by water extract of Allium jesdianum as a biochemical reducing agent in the presence of montmorillonite clay(MMT)as a natural solid support for t...In this work,synthesis of Ni nanoparticles was carried out successfully by water extract of Allium jesdianum as a biochemical reducing agent in the presence of montmorillonite clay(MMT)as a natural solid support for the first time.Then the electrochemical activity of the synthesized nanocomposite was investigated in methanol electrocatalytic oxidation.MMT with high cation exchange capacity and nano layer structure was exposed to ion exchange conditions in nickel solution.Then Ni^2+ion exchanged form was used in this process as a source of ions and also capping agent.Water extract of Allium jesdianum used as a reducing agent due to abundant availability of phenolic and flavonoid contents.The synthesized Ni/MMT nanocomposite was characterized using UV–Vis spectroscopy(UV–Vis),Fourier Transform Infrared Spectroscopy(FT-IR),X-ray diffraction(XRD),Scanning Electron Microscopy(SEM),Transmission electron microscopy(TEM)and Energy-dispersive X-ray spectroscopy(EDX).The surface of prepared modified electrode has been characterized using SEM to evaluate the morphology,showing uniform dispersion of Ni nanoparticles with mean diameter of 12 to 20 nm.The modified carbon paste electrode was then used in methanol electrocatalytic oxidation reaction.Methanol oxidation on the proposed modified electrode surface occurs at 0.6 V and 0.3 V in alkaline and acidic medium respectively.Also,the results showed the better performance of modified electrode toward methanol electrocatalytic oxidation in comparison with carbon paste electrode that is modified by ion exchanged MMT.Charge transfer coefficients and apparent charge transfer rate constant for the modified electrode in the absence of methanol in alkaline medium were respectively found as:αa=0.53,αc=0.37 and ks=1.6×10^-1 s^-1.Also,the average value of catalytic rate constant for the electrocatalytic oxidation of methanol by the prepared nano-catalyst was estimated to be about 0.9 L·mol^-1·s^-1 by chronoamperometry technique.The prepared electrode was also effective for electrocatalytic oxidation of ethanol and formaldehyde in alkaline medium.展开更多
Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepare...Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepared for electrocatalytically oxidizing gaseous toluene in an all-solid cell at ambient temperature.The complex Ti/Sb-Sn O_(2)/β-Pb O_(2)anode,which was prepared by sequentially deposing Sb-Sn O_(2)and β-Pb O_(2)on a foam Ti substrate,shows high electrocatalytic oxidation efficiency of toluene (80%) at 7 hr of reaction and high CO_(2)selectivity (94.9%) under an optimized condition,i.e.,a cell voltage of 2.0 V,relative humidity of60%and a flow rate of 100 m L/min.The better catalytic performance can be ascribed to the high production rate of·OH radicals from discharging adsorbed water and the inhibition of oxygen evolution on the surface of foam Ti/Sb-Sn O_(2)/β-Pb O_(2)anode when compared with the foam Ti/Sb-Sn O_(2)anode.Our results demonstrate that prepared complex electrodes can be potentially used for electrocatalytic removal of gaseous toluene at room temperature with a good performance.展开更多
A nickel salen complex was encapsulated in the supercages of nanozeolite NaA,LTA(linde type A)structure,using the flexible ligand method.The electrochemical behavior and electrocatalytic activity of a carbon paste ele...A nickel salen complex was encapsulated in the supercages of nanozeolite NaA,LTA(linde type A)structure,using the flexible ligand method.The electrochemical behavior and electrocatalytic activity of a carbon paste electrode(CPE)modified with Ni(II)‐Salen‐A(Ni(II)‐SalenA/CPE)for hydrazine oxidation in0.1mol/L NaOH solution were investigated by cyclic voltammetry,chronoamperometry,and chronocoulometry.First,organic‐template‐free synthesis of nanozeolite LTA was performed and the obtained material was characterized by various techniques.The average particle size of the LTA crystals was estimated to be56.1and72nm by X‐ray diffraction and particle size analysis,respectively.The electron transfer coefficient was found to be0.64and the catalytic rate constant for oxidation of hydrazine at the redox sites of Ni(II)‐SalenA/CPE was found to be1.03×105cm3/(mol·s).Investigation of the electrocatalytic mechanism suggested that oxidation of hydrazine occurred through reaction with Ni3+(Salen)O(OH)and also direct electrooxidation.The anodic peak currents revealed a linear dependence on the square root of the scan rate,indicating a diffusion‐controlled process,and the diffusion coefficient of hydrazine was found to be1.18×10?7cm2/s.The results indicated that Ni(II)‐SalenA/CPE displays good electrocatalytic activity toward hydrazine oxidation owing to the porous structure of nanozeolite LTA and the Ni(II)‐Salen complex.Finally,the general reaction mechanism for the electrooxidation of hydrazine on Ni(II)‐SalenA/CPE in alkaline solution involves the transfer of four electrons,in which the first electron transfer reaction acts as the rate‐limiting step followed by a three‐electron process to generate environmentally friendly nitrogen and water as final products.展开更多
In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small mo...In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules.The interaction between Ni and Co can optimize the electronic structure,resulting in the improved conductivity and accelerated charge transfer rate.The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process.Post-structure and catalytic characterizations confirm the surface oxidation of(Ni,Co)S_(2)during the stability test,and the in-situ formed Co(Ni)based(oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability.As a result,the optimal(Ni,Co)S_(2)solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation,in which a high conversion of benzyl alcohol(97.50%),a good selectivity to benzoic acid(93.78%)and a satisfied faraday efficiency(91.86%)can be achieved.展开更多
The promoter effects of rare earth ions on the electrocatalytic oxidation of methanol at the Pt electrode were studied using the cyclic voltammetry and stable polarization techniques. It was found for the first time ...The promoter effects of rare earth ions on the electrocatalytic oxidation of methanol at the Pt electrode were studied using the cyclic voltammetry and stable polarization techniques. It was found for the first time that Eu、Ho、Dy ions could accelerate the electrocatalytic oxidation of methanol at the Pt electrode, while Lu、Pr、Yb、Sm ions showed inhibitor effects.展开更多
To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can p...To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can promote anion movement and the generation of active species,resulting more organic compounds to be oxidized and degraded.Oxidation parameters such as treatment time,current density and initial pH of the wastewater were systematically discussed and optimized.The mineralization of organic compounds is improved by over 15% under a magnetic density of 22 mT while the current density is 50 A/m2,pH is 1.8 and the reaction time is 1.5 h.The results indicate that the magnetic field assisted electrocatalytic oxidation has considerable potential in electroplating wastewater treatment.展开更多
Platinum(Pt)/nanofibrous polyaniline(PANI) electrode was prepared by pulse galvanostatic method and characterized by scanning electron microscopy.The electrochemical behavior of L-cysteine at the Pt/nanofibrous PANI e...Platinum(Pt)/nanofibrous polyaniline(PANI) electrode was prepared by pulse galvanostatic method and characterized by scanning electron microscopy.The electrochemical behavior of L-cysteine at the Pt/nanofibrous PANI electrode was investigated by cyclic voltammetry.The results indicate that the pH value of the solution and the Pt loading of the electrode have great effect on the electrocatalytic property of the Pt /nanofibrous PANI electrode;the suitable Pt loading of the electrode is 600 μg/cm2 and the suitable pH value of the solution is 4.5 for investigating L-cysteine oxidation.The L-cysteine sensor based on the Pt/nanofibrous PANI electrode has a good selectivity,reproducibility and stability.The Pt/nanofibrous PANI electrode is highly sensitive to L-cysteine,and the linear calibration curve for the oxidation of L-cysteine can be observed in the range of 0.2-5.0 mmol/L.展开更多
The oxidation of ethanol in 1 .0 mol/L NaOH was studied on Pd/GC electrode preparedby electrodeposition. The results show that (1) Pd/GC electrode can also demonstrateclectrocatalytic activity towards the oxidation o...The oxidation of ethanol in 1 .0 mol/L NaOH was studied on Pd/GC electrode preparedby electrodeposition. The results show that (1) Pd/GC electrode can also demonstrateclectrocatalytic activity towards the oxidation of cthanolf (2) two backward anodic peaks on thecathodic branch appear when the ethanol concentration is raised up to 0.5 mol/L.展开更多
Polyaniline film was prepared by using the repeated potential cycling technique in an acidic solution at the surface of glassy carbon electrode. Then transition metal ions of Ni and Cu were incorporated to the polymer...Polyaniline film was prepared by using the repeated potential cycling technique in an acidic solution at the surface of glassy carbon electrode. Then transition metal ions of Ni and Cu were incorporated to the polymer by immersion of the modified electrode. A comparative study of the electrocatalytic oxidation of methanol is made in NaOH, on Ni and Cu on polyaniline film covered glassy carbon electrode (Ni-PANI-GC, Cu-PANI-GC) at 25℃. Catalytic activity for the oxidation of methanol was studied by using cyclic voltammetry.展开更多
With the acceleration of global industrialization,the human society has an increasing demand for high-value chemicals.Such chemicals are mostly derived from non-renewable fossil fuels,causing inevitable energy shortag...With the acceleration of global industrialization,the human society has an increasing demand for high-value chemicals.Such chemicals are mostly derived from non-renewable fossil fuels,causing inevitable energy shortage and accompanied environmental pollution issues during the conversion processes[1].Recently,biomass-derived platform molecules with abundant source,low price,and variable chemical structure have attracted tremendous attention from researchers,and their catalytic oxidation has become a promising route to reduce the dependence of fossil fuels and alleviate the harmful impact of environmental pollution for the production of high-value chemicals[2].展开更多
High-concentration phenol wastewater is pollutant of concern that pose significant risks to human health and the environment.Three-dimensional electrocatalytic oxidation is one of the most promising wastewater treatme...High-concentration phenol wastewater is pollutant of concern that pose significant risks to human health and the environment.Three-dimensional electrocatalytic oxidation is one of the most promising wastewater treatment technologies because of its high treatment efficiency,low energy consumption and low secondary pollution.Lower-cost and higher-performance particles still faces great challenges.In this work,metal oxide particle electrodes were prepared using granular activated carbon(GAC)as a substrate to study the degradation of phenol by three-dimensional electrocatalytic oxidation.GAC particle electrodes loaded with different monometallic oxides(Mn,Fe,Co,Ce)and bimetallic oxides(Fe and Ce)were prepared by the impregnation method.The effectiveness of the particle electrodes in degrading phenol was greatly improved after active components loading.Among all monometallic oxide particle electrodes,the concentration degradation efficiency was in the order of Ce/GAC>Co/GAC>Mn/GAC>Fe/GAC,and the COD degradation efficiency was Ce/GAC>Fe/GAC>Co/GAC>Mn/GAC.After optimizing the loading metal type and loading amount,it was found that the 1.1%Fe-2.7%Ce/GAC particle electrode perform the best,with a phenol degradation efficiency of 95.48%,a COD degradation rate of 94.35%,an energy consumption of 0.75 kW·h·kg^(-1)COD.This lower-cost and higher-performance particle highlights a reliable route for solving the problem of particle electrode materials limiting the efficient treatment of phenol-containing wastewater.展开更多
Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydr...Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydroxymethylfurfural(HMF),has attracted extensive attention due to the potential of replacing terephthalic acid to synthesize high-performance polymeric materials for commercialization.In the present work,the pHdependent reaction pathways and factors influencing the degree of functional group oxidation are first discussed.Then the reaction mechanism of HMF oxidation is further elucidated using the representative examples.In addition,the emerging catalyst design strategies(defects,interface engineering)used in HMF oxidation are generalized,and structure-activity relationships between the abovementioned strategies and catalysts performance are analyzed.Furthermore,cathode pairing reactions,such as hydrogen evolution reaction,CO_(2) reduction reaction(CO_(2)RR),oxygen reduction reaction,and thermodynamically favorable organic reactions to lower the cell voltage of the electrolysis system,are discussed.Finally,the challenges and prospects of the electrochemical oxidation of HMF for FDCA are presented,focusing on deeply investigated reaction mechanism,coupling reaction,reactor design,and downstream product separation/purification.展开更多
Cobalt tetra（2,4-dichloro-1,3,5-triazine）aminophthalocyanine （CoPc） was immobilized covalently on activated carbon fiber （ACF） felt to obtain CoPc-modified ACF （CoPc-ACF） catalyst, and an electrocatalytic oxid...Cobalt tetra（2,4-dichloro-1,3,5-triazine）aminophthalocyanine （CoPc） was immobilized covalently on activated carbon fiber （ACF） felt to obtain CoPc-modified ACF （CoPc-ACF） catalyst, and an electrocatalytic oxidation system using CoPc-ACF as the anode was constructed. The electrocatalytic oxidation of Acid Red 1 （ARI） was investigated in aqueous solution by an UV-vis spectrophotometer and UPLC. The results indicated that AR1 could be eliminated efficiently in this electrocatalytic oxidation system. In addition, the results of FTIR, TOC and GC-MS suggested that the electrocatalytic oxidation experienced the decoloration achieved by destroying the azo linkage and the further mineralization due to the cleavages of benzene ring and naphthalene ring. The intermediates were mainly small molecular compounds such as maleic acid and succinic acid, etc. Re- petitive tests showed that CoPc-ACF can maintain high electrocatalytic activity over several cycles. The further EPR spin-trap experiments indicated that the hydroxyl radicals did not dominate the reaction in this electrocatalytic system, which was com- pletely different from the traditional electro-Fenton system. Based on the non-radical reaction mechanism, the CoPc-modified ACF electrocatalyst has potential application in treating actual dyestuffs wastewaters, which are accompanied with high concentration of hydroxyl radical scavengers such as chlorine ions and additives in the textile printing and dyeing industry.展开更多
Carbon materials are widely used as catalysts in electrocatalytic oxidative(EO)degradation of wastewater due to their large specific surface area and low cost.Carbon materials can also be used as catalyst carriers for...Carbon materials are widely used as catalysts in electrocatalytic oxidative(EO)degradation of wastewater due to their large specific surface area and low cost.Carbon materials can also be used as catalyst carriers for EO reactions due to their ease of functionalization with other heteroatoms and metals/metal oxides.To improve the catalytic activity and current efficiency of carbon materials,modifying the structural and physicochemical properties of conventional carbon materials are common improvement method.This review briefly outlines the recent research progress of carbon materials in EO for organic pollutants degradation.It also discusses the modification strategies and corresponding electrocatalytic properties of various carbon materials(carbon nanomaterials and porous carbon materials),and explores the EO mechanism.Finally,some summaries of the remaining challenges and future developments of carbon materials in the field of electrocatalysis are given.展开更多
Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions,including the oxygen evolution reaction(OER)and glucose oxidation reaction(GOR).Herein,we prepared cobalt hydroxi...Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions,including the oxygen evolution reaction(OER)and glucose oxidation reaction(GOR).Herein,we prepared cobalt hydroxide nanoparticles(CoHP)and cobalt hydroxide nanosheets(CoHS)on nickel foam.In the electrocatalytic OER,CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm^-2.This is enhanced as compared with that of CoHP(367 mV at 10 mA·cm^-2).In addition,CoHS also exhibits an improved performance in the electrocatalytic GOR.The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer.These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.展开更多
High performance platinized-carbon electrodes have been developed for the electrocatalytic oxidation of ethanol to acetaldehyde in electrogenerative processes. A load current density of the electrode can be achieved a...High performance platinized-carbon electrodes have been developed for the electrocatalytic oxidation of ethanol to acetaldehyde in electrogenerative processes. A load current density of the electrode can be achieved as high as 600 mA per square centimeter for oxygen reducing in 3 mol/L sulfuric acid with a good stability. With these electrodes and sulfuric acid as an electrolyte in fuel cells, ethanol vapor carried by nitrogen gas can be oxidized selectively to acetaldehyde. Selectivity of acetaldehyde depends on the potential of the cell and the feed rate of ethanol vapor and it can be more than 80% under optimized conditions. The initial product of ethanol oxidized on a platinized-carbon electrode is acetaldehyde and the ethanol oxidation mechanism is discussed.展开更多
基金supported by the National Key R&D Program of China(2023YFC3905804)the National Natural Science Foundation of China(22078374,22378434,41920104003)the Scientific and Technological Planning Project of Guangzhou(202206010145)。
文摘The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining,and has become a frontier of mainstream research.This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes(5-hydroxymethylfurfural,furfural,glucose,xylose,vanillin and benzaldehyde,etc.).The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde.It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies,catalyst stability,and reaction scalability remain,but the rapid progress offers hope for future advancements.Finally,we elucidate the challenges in this domain and provide the perspectives on future developments.This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.
基金the funds granted by the Ningxia Natural Science Foundation(2023AAC05003,2024AAC03048,2024AAC03051)the National Natural Science Foundation of China(22108130,22368039)+1 种基金the Ningxia Key Research&Development Program(2023BDE03001)the Ningxia Overseas Returnee Innovation and Entrepreneurship Project for the financial support。
文摘Addressing the contamination of antibiotics has attracted ever-increasing and imperative attention due to their widespread existence,easy-to-cause drug-resistant bacteria infection,coupled with their intrinsic toxicity and hazard to environments and human health.Herein,a novel CC/CoNi-LDH-10%Ce anode material was directly constructed through a simple and rapid electrodeposition strategy,serving as an efficacious electrocatalyst for removing ciprofloxacin(CIP)from aqueous solution.Such novel CC/CoNi-LDH-10%Ce anode delivered a higher charge transfer,relatively abundant oxygen vacancies,and a higher electrochemical active area.The as-fabricated CC/CoNi-LDH-10%Ce electrode achieved a substantially boosted CIP removal efficiency of 52.5%relative to that of pure CC at about 23.9%.Notably,doping an appropriate amount of Ce^(3+)can endow the pristine CC/CoNi-LDH with richer oxygen vacancies and excellent electrocatalytic performance.Additionally,the electrocatalytic oxidation of CIP was attributed to both direct oxidation on the electrode surface and indirect oxidation induced by the generated active species(superoxide radicals and hydroxyl radicals).This study provides a simple,universal and flexible tactic for other researchers in designing and manufacturing avenues of electrodes.
基金supported by the National Natural Science Foundation of China(Nos.52200186 and 52070025)Chongqing Natural Science Foundation(No.CSTB2024NSCQ-MSX0407)+1 种基金the National Key Research and Development Program of China(No.2019YFC1805502)Chongqing Municipal Human Resources and Social Security Bureau(No.2309013519935095).
文摘The organic pollutants,such as quaternary ammonium compounds,in high salinity flowback water from shale gas extraction may pose a severe risk to public health.Conventional biological technologies have limited effectiveness in the treatment of high-salt wastewaters,whereas electrocatalytic oxidation has shown potential for treating organic pollutants in high-salt flowback water.This study developed a carbon nanotubes(CNTs)doped Ru/Ir oxide coated Ti electrode CNTs-(Ru_(x)Ir_(y)O_(2))/Ti,which exhibited enhanced electrocatalytic performance for the treatment of quaternary ammonium compound in high-salt wastewater compared to the control metal oxide coated Ti anode(Ru_(x)Ir_(y)O_(2))/Ti,with pseudofirst-order reaction rate constant improved from 7.36×10^(-3) to 1.12×10^(-2) min−1.Moreover,the CNTs-(Ru_(x)Ir_(y)O_(2))/Ti anode electrocatalytic oxidation system exhibited excellent cycling stability.Mechanism studies indicated that the CNTs-(Ru_(x)Ir_(y)O_(2))/Ti electrode enhanced singlet oxygen(^(1)O_(2))generation,which played a major role in pollutant degradation.Furthermore,the formation of high concentrations of HClO and H_(2)O_(2) further facilitated the generation of ^(1)O_(2).This study may provide an efficient and green technology for the treatment of organic pollutants in high-salt shale gas flowback water.
基金supported by the National Natural Science Foundation of China(52272222)the Taishan Scholar Young Talent Program(tsqn201909114,tsqn201909123)the University Youth Innovation Team of Shandong Province(202201010318)。
文摘Electrocatalytic toluene(TL)oxidation to produce benzoic acid(BAC)process is largely hindered due to sluggish kinetics associated with the transformation of the rate-determining step,because of weak TL adsorption and high rate-determining step energy barrier for difficult to dehydrogenate.Herein,we report Mn_(x)Ce_(1-x)O_(2)/CNT catalyst for accelerated reaction kinetics.Theoretical and experimental studies indicate that Ce sites promote TL adsorption and polyvalent Mn modulates the electronic structure of Ce sites reducing the rate-determining step energy barrier.This results in increasing^(*)C_(6)H_(5)CH_(2)coverage and effectively accelerating TL oxidation reaction(TOR)kinetics.Excitingly,the Faraday efficiency(FE)and BAC yield of optimized Mn_(0.6)Ce_(0.4)O_(2)/CNT at 2.6 V vs.RHE could reach 85.9%and 653.9 mg h^(-1)cm^(-2),respectively.In addition,the Mn_(0.6)Ce_(0.4)O_(2)/CNT displays a high selectivity of 96.3%for BAC.Combining the TL oxidation reaction with hydrogen evolution reaction,the anion exchange membrane electrolyzer of Mn_(0.6)Ce_(0.4)O_(2)/CNT(+)||Pt/C(-)can reach 100 mA cm^(-2)at the voltage of 3.0 V,in which the BAC yield is 579.4 mg h^(-1)cm^(-2)and the FE is 83.6%.This work achieved high selectivity of TOR at industrial-relevant current densities of 100 mA cm^(-2)at the low voltage for the first time.
基金supported by Science and Research and Shahr-eQods Branches of Islamic Azad University of Iran。
文摘In this work,synthesis of Ni nanoparticles was carried out successfully by water extract of Allium jesdianum as a biochemical reducing agent in the presence of montmorillonite clay(MMT)as a natural solid support for the first time.Then the electrochemical activity of the synthesized nanocomposite was investigated in methanol electrocatalytic oxidation.MMT with high cation exchange capacity and nano layer structure was exposed to ion exchange conditions in nickel solution.Then Ni^2+ion exchanged form was used in this process as a source of ions and also capping agent.Water extract of Allium jesdianum used as a reducing agent due to abundant availability of phenolic and flavonoid contents.The synthesized Ni/MMT nanocomposite was characterized using UV–Vis spectroscopy(UV–Vis),Fourier Transform Infrared Spectroscopy(FT-IR),X-ray diffraction(XRD),Scanning Electron Microscopy(SEM),Transmission electron microscopy(TEM)and Energy-dispersive X-ray spectroscopy(EDX).The surface of prepared modified electrode has been characterized using SEM to evaluate the morphology,showing uniform dispersion of Ni nanoparticles with mean diameter of 12 to 20 nm.The modified carbon paste electrode was then used in methanol electrocatalytic oxidation reaction.Methanol oxidation on the proposed modified electrode surface occurs at 0.6 V and 0.3 V in alkaline and acidic medium respectively.Also,the results showed the better performance of modified electrode toward methanol electrocatalytic oxidation in comparison with carbon paste electrode that is modified by ion exchanged MMT.Charge transfer coefficients and apparent charge transfer rate constant for the modified electrode in the absence of methanol in alkaline medium were respectively found as:αa=0.53,αc=0.37 and ks=1.6×10^-1 s^-1.Also,the average value of catalytic rate constant for the electrocatalytic oxidation of methanol by the prepared nano-catalyst was estimated to be about 0.9 L·mol^-1·s^-1 by chronoamperometry technique.The prepared electrode was also effective for electrocatalytic oxidation of ethanol and formaldehyde in alkaline medium.
基金supported by the National Natural Science Foundation of China (Nos. 22025604, 21976196, and 41877306)the Hebei Technological Innovation Center for Volatile Organic Compounds Detection and Treatment in Chemical Industry (No. ZXJJ20210403)。
文摘Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepared for electrocatalytically oxidizing gaseous toluene in an all-solid cell at ambient temperature.The complex Ti/Sb-Sn O_(2)/β-Pb O_(2)anode,which was prepared by sequentially deposing Sb-Sn O_(2)and β-Pb O_(2)on a foam Ti substrate,shows high electrocatalytic oxidation efficiency of toluene (80%) at 7 hr of reaction and high CO_(2)selectivity (94.9%) under an optimized condition,i.e.,a cell voltage of 2.0 V,relative humidity of60%and a flow rate of 100 m L/min.The better catalytic performance can be ascribed to the high production rate of·OH radicals from discharging adsorbed water and the inhibition of oxygen evolution on the surface of foam Ti/Sb-Sn O_(2)/β-Pb O_(2)anode when compared with the foam Ti/Sb-Sn O_(2)anode.Our results demonstrate that prepared complex electrodes can be potentially used for electrocatalytic removal of gaseous toluene at room temperature with a good performance.
文摘A nickel salen complex was encapsulated in the supercages of nanozeolite NaA,LTA(linde type A)structure,using the flexible ligand method.The electrochemical behavior and electrocatalytic activity of a carbon paste electrode(CPE)modified with Ni(II)‐Salen‐A(Ni(II)‐SalenA/CPE)for hydrazine oxidation in0.1mol/L NaOH solution were investigated by cyclic voltammetry,chronoamperometry,and chronocoulometry.First,organic‐template‐free synthesis of nanozeolite LTA was performed and the obtained material was characterized by various techniques.The average particle size of the LTA crystals was estimated to be56.1and72nm by X‐ray diffraction and particle size analysis,respectively.The electron transfer coefficient was found to be0.64and the catalytic rate constant for oxidation of hydrazine at the redox sites of Ni(II)‐SalenA/CPE was found to be1.03×105cm3/(mol·s).Investigation of the electrocatalytic mechanism suggested that oxidation of hydrazine occurred through reaction with Ni3+(Salen)O(OH)and also direct electrooxidation.The anodic peak currents revealed a linear dependence on the square root of the scan rate,indicating a diffusion‐controlled process,and the diffusion coefficient of hydrazine was found to be1.18×10?7cm2/s.The results indicated that Ni(II)‐SalenA/CPE displays good electrocatalytic activity toward hydrazine oxidation owing to the porous structure of nanozeolite LTA and the Ni(II)‐Salen complex.Finally,the general reaction mechanism for the electrooxidation of hydrazine on Ni(II)‐SalenA/CPE in alkaline solution involves the transfer of four electrons,in which the first electron transfer reaction acts as the rate‐limiting step followed by a three‐electron process to generate environmentally friendly nitrogen and water as final products.
基金supported by National Natural Science Foundation of China(Nos.21927811,51602182,21808129)the Natural Science Foundation of Shandong Province,China(No.ZR2021ME032)。
文摘In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules.The interaction between Ni and Co can optimize the electronic structure,resulting in the improved conductivity and accelerated charge transfer rate.The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process.Post-structure and catalytic characterizations confirm the surface oxidation of(Ni,Co)S_(2)during the stability test,and the in-situ formed Co(Ni)based(oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability.As a result,the optimal(Ni,Co)S_(2)solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation,in which a high conversion of benzyl alcohol(97.50%),a good selectivity to benzoic acid(93.78%)and a satisfied faraday efficiency(91.86%)can be achieved.
基金The authors are grateful for the financial supports of 973 Program,National Science and Technology Commission,China(G2000026408)the National Natural Science Foundation of China(20003005)+1 种基金Natural Science Foundation,Jilin Province,(20000510)Natural Science Foundation Jiangsu Province,(BQ2000009).
文摘The promoter effects of rare earth ions on the electrocatalytic oxidation of methanol at the Pt electrode were studied using the cyclic voltammetry and stable polarization techniques. It was found for the first time that Eu、Ho、Dy ions could accelerate the electrocatalytic oxidation of methanol at the Pt electrode, while Lu、Pr、Yb、Sm ions showed inhibitor effects.
基金Project(2008ZX07101-006-09) supported by the Major Science and Technology Program for Water Pollution Control and Treatment of China
文摘To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can promote anion movement and the generation of active species,resulting more organic compounds to be oxidized and degraded.Oxidation parameters such as treatment time,current density and initial pH of the wastewater were systematically discussed and optimized.The mineralization of organic compounds is improved by over 15% under a magnetic density of 22 mT while the current density is 50 A/m2,pH is 1.8 and the reaction time is 1.5 h.The results indicate that the magnetic field assisted electrocatalytic oxidation has considerable potential in electroplating wastewater treatment.
基金Project(20050532008) supported by the PhD. Program Foundation of Ministry of Education of ChinaProject(06JJ4005) supported by the Natural Science Foundation of Hunan Province+1 种基金 Project(20060400874)supported by the Postdoctoral Foundation of China Project supported by the Postdoctoral Foundation of Hunan University
文摘Platinum(Pt)/nanofibrous polyaniline(PANI) electrode was prepared by pulse galvanostatic method and characterized by scanning electron microscopy.The electrochemical behavior of L-cysteine at the Pt/nanofibrous PANI electrode was investigated by cyclic voltammetry.The results indicate that the pH value of the solution and the Pt loading of the electrode have great effect on the electrocatalytic property of the Pt /nanofibrous PANI electrode;the suitable Pt loading of the electrode is 600 μg/cm2 and the suitable pH value of the solution is 4.5 for investigating L-cysteine oxidation.The L-cysteine sensor based on the Pt/nanofibrous PANI electrode has a good selectivity,reproducibility and stability.The Pt/nanofibrous PANI electrode is highly sensitive to L-cysteine,and the linear calibration curve for the oxidation of L-cysteine can be observed in the range of 0.2-5.0 mmol/L.
文摘The oxidation of ethanol in 1 .0 mol/L NaOH was studied on Pd/GC electrode preparedby electrodeposition. The results show that (1) Pd/GC electrode can also demonstrateclectrocatalytic activity towards the oxidation of cthanolf (2) two backward anodic peaks on thecathodic branch appear when the ethanol concentration is raised up to 0.5 mol/L.
文摘Polyaniline film was prepared by using the repeated potential cycling technique in an acidic solution at the surface of glassy carbon electrode. Then transition metal ions of Ni and Cu were incorporated to the polymer by immersion of the modified electrode. A comparative study of the electrocatalytic oxidation of methanol is made in NaOH, on Ni and Cu on polyaniline film covered glassy carbon electrode (Ni-PANI-GC, Cu-PANI-GC) at 25℃. Catalytic activity for the oxidation of methanol was studied by using cyclic voltammetry.
基金supported by CAS Key Laboratory of Renewable Energy,Guangzhou Institute of Energy Conversion(E229kf1201)the National Natural Science Foundation of China(22078374,22378434,and 22309210)the Scientific and Technological Planning Project of Guangzhou(202206010145 and 2024A04J4353).
文摘With the acceleration of global industrialization,the human society has an increasing demand for high-value chemicals.Such chemicals are mostly derived from non-renewable fossil fuels,causing inevitable energy shortage and accompanied environmental pollution issues during the conversion processes[1].Recently,biomass-derived platform molecules with abundant source,low price,and variable chemical structure have attracted tremendous attention from researchers,and their catalytic oxidation has become a promising route to reduce the dependence of fossil fuels and alleviate the harmful impact of environmental pollution for the production of high-value chemicals[2].
文摘High-concentration phenol wastewater is pollutant of concern that pose significant risks to human health and the environment.Three-dimensional electrocatalytic oxidation is one of the most promising wastewater treatment technologies because of its high treatment efficiency,low energy consumption and low secondary pollution.Lower-cost and higher-performance particles still faces great challenges.In this work,metal oxide particle electrodes were prepared using granular activated carbon(GAC)as a substrate to study the degradation of phenol by three-dimensional electrocatalytic oxidation.GAC particle electrodes loaded with different monometallic oxides(Mn,Fe,Co,Ce)and bimetallic oxides(Fe and Ce)were prepared by the impregnation method.The effectiveness of the particle electrodes in degrading phenol was greatly improved after active components loading.Among all monometallic oxide particle electrodes,the concentration degradation efficiency was in the order of Ce/GAC>Co/GAC>Mn/GAC>Fe/GAC,and the COD degradation efficiency was Ce/GAC>Fe/GAC>Co/GAC>Mn/GAC.After optimizing the loading metal type and loading amount,it was found that the 1.1%Fe-2.7%Ce/GAC particle electrode perform the best,with a phenol degradation efficiency of 95.48%,a COD degradation rate of 94.35%,an energy consumption of 0.75 kW·h·kg^(-1)COD.This lower-cost and higher-performance particle highlights a reliable route for solving the problem of particle electrode materials limiting the efficient treatment of phenol-containing wastewater.
基金University of Electronic Science and Technology of China,Grant/Award Number:A1098531023601208Scientific Research Foundation,Grant/Award Number:Y030212059003045+1 种基金China Postdoctoral Science Foundation,Grant/Award Numbers:2021TQ0059,2022M710610National Natural Science Foundation of China,Grant/Award Numbers:21464015,21472235。
文摘Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydroxymethylfurfural(HMF),has attracted extensive attention due to the potential of replacing terephthalic acid to synthesize high-performance polymeric materials for commercialization.In the present work,the pHdependent reaction pathways and factors influencing the degree of functional group oxidation are first discussed.Then the reaction mechanism of HMF oxidation is further elucidated using the representative examples.In addition,the emerging catalyst design strategies(defects,interface engineering)used in HMF oxidation are generalized,and structure-activity relationships between the abovementioned strategies and catalysts performance are analyzed.Furthermore,cathode pairing reactions,such as hydrogen evolution reaction,CO_(2) reduction reaction(CO_(2)RR),oxygen reduction reaction,and thermodynamically favorable organic reactions to lower the cell voltage of the electrolysis system,are discussed.Finally,the challenges and prospects of the electrochemical oxidation of HMF for FDCA are presented,focusing on deeply investigated reaction mechanism,coupling reaction,reactor design,and downstream product separation/purification.
基金supported by the National Natural Science Foundation of China(51133006,51103133,51003096)Program for Changjiang Scholars and Innovative Research Team in University(0654)Textile Vision Science & Education Fund and Science Foundation of Zhejiang SciTech University(1001803-Y)
文摘Cobalt tetra（2,4-dichloro-1,3,5-triazine）aminophthalocyanine （CoPc） was immobilized covalently on activated carbon fiber （ACF） felt to obtain CoPc-modified ACF （CoPc-ACF） catalyst, and an electrocatalytic oxidation system using CoPc-ACF as the anode was constructed. The electrocatalytic oxidation of Acid Red 1 （ARI） was investigated in aqueous solution by an UV-vis spectrophotometer and UPLC. The results indicated that AR1 could be eliminated efficiently in this electrocatalytic oxidation system. In addition, the results of FTIR, TOC and GC-MS suggested that the electrocatalytic oxidation experienced the decoloration achieved by destroying the azo linkage and the further mineralization due to the cleavages of benzene ring and naphthalene ring. The intermediates were mainly small molecular compounds such as maleic acid and succinic acid, etc. Re- petitive tests showed that CoPc-ACF can maintain high electrocatalytic activity over several cycles. The further EPR spin-trap experiments indicated that the hydroxyl radicals did not dominate the reaction in this electrocatalytic system, which was com- pletely different from the traditional electro-Fenton system. Based on the non-radical reaction mechanism, the CoPc-modified ACF electrocatalyst has potential application in treating actual dyestuffs wastewaters, which are accompanied with high concentration of hydroxyl radical scavengers such as chlorine ions and additives in the textile printing and dyeing industry.
基金the financial support from Shanghai Pujiang Program(20PJ1404800).
文摘Carbon materials are widely used as catalysts in electrocatalytic oxidative(EO)degradation of wastewater due to their large specific surface area and low cost.Carbon materials can also be used as catalyst carriers for EO reactions due to their ease of functionalization with other heteroatoms and metals/metal oxides.To improve the catalytic activity and current efficiency of carbon materials,modifying the structural and physicochemical properties of conventional carbon materials are common improvement method.This review briefly outlines the recent research progress of carbon materials in EO for organic pollutants degradation.It also discusses the modification strategies and corresponding electrocatalytic properties of various carbon materials(carbon nanomaterials and porous carbon materials),and explores the EO mechanism.Finally,some summaries of the remaining challenges and future developments of carbon materials in the field of electrocatalysis are given.
基金the financial support from the National Natural Science Foundation of China(Grant Nos.11761141006,81822024 and 21605102)the National Key Research and Development Program of China(Grant No.2017YFC1200904).
文摘Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions,including the oxygen evolution reaction(OER)and glucose oxidation reaction(GOR).Herein,we prepared cobalt hydroxide nanoparticles(CoHP)and cobalt hydroxide nanosheets(CoHS)on nickel foam.In the electrocatalytic OER,CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm^-2.This is enhanced as compared with that of CoHP(367 mV at 10 mA·cm^-2).In addition,CoHS also exhibits an improved performance in the electrocatalytic GOR.The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer.These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.
基金Supported Partially by the Ministry of Education of China.
文摘High performance platinized-carbon electrodes have been developed for the electrocatalytic oxidation of ethanol to acetaldehyde in electrogenerative processes. A load current density of the electrode can be achieved as high as 600 mA per square centimeter for oxygen reducing in 3 mol/L sulfuric acid with a good stability. With these electrodes and sulfuric acid as an electrolyte in fuel cells, ethanol vapor carried by nitrogen gas can be oxidized selectively to acetaldehyde. Selectivity of acetaldehyde depends on the potential of the cell and the feed rate of ethanol vapor and it can be more than 80% under optimized conditions. The initial product of ethanol oxidized on a platinized-carbon electrode is acetaldehyde and the ethanol oxidation mechanism is discussed.
