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
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
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
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
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
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
The oxygen evolution reaction(OER)activity of single-atom catalysts(SACs)is closely related to the coordination environment of the active site.Oxygencoordinated atomic metal species bring about unique features beyond ...The oxygen evolution reaction(OER)activity of single-atom catalysts(SACs)is closely related to the coordination environment of the active site.Oxygencoordinated atomic metal species bring about unique features beyond nitrogen-coordinated atomic metal species due to the fact that the M-O bond is weaker than the M-N bond.Herein,a series of metal-oxygen-carbon structured low-nucleus clusters(LNCs)are successfully anchored on the surface of multiwalled carbon nanotubes(M-MWCNTs,M=Ni,Co,or Fe)through a foolproof low-temperature gas transfer(300℃)method without any further treatment.The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations.The synthetic Ni-MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions,transcending the performances of Co-MWCNTs,Fe-MWCNTs and RuO_(2).Density functional theory calculations reveal that the moderate oxidation of low-nucleus Ni clusters changes the unoccupied orbital of Ni atoms,thereby lowering the energy barrier of the OER rate-limiting step and making the OER process more energy-efficient.This study demonstrates a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts.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
Selective upgrading of C=O bonds to afford carboxylic acid is significant for the petrochemical industry and biomass utilization.Here we declared the efficient electrooxidation of biomass-derived aldehydes family over...Selective upgrading of C=O bonds to afford carboxylic acid is significant for the petrochemical industry and biomass utilization.Here we declared the efficient electrooxidation of biomass-derived aldehydes family over NiV-layered double hydroxides(LDHs) thin films.Mechanistic studies confirmed the hydroxyl active intermediate(-OH*) generated on the surface of NiV-LDHs films by employing electrochemical impedance spectroscopy and the electron paramagnetic resonance spectroscopy.By using advanced techniques,e.g.,extended X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy,NiV-LDHs films with 2.6 nm could expose larger specific surface area.Taking benzaldehyde as a model,high current density of 200 mA cm^(-2)at 1.8 V vs.RHE,81.1% conversion,77.6% yield of benzoic acid and 90.8% Faradaic efficiency were reached,which was superior to most of previous studies.Theoretical DFT analysis was well matched with experimental findings and documented that NiV-LDHs had high adsorption capacity for the aldehydes to suppress the side reaction,and the aldehydes were oxidized by the electrophilic hydroxyl radicals formed on NiV-LDHs.Our findings offer a universal strategy for the robust upgrading of diverse biomass-derived platform chemicals.展开更多
This work describes the electrochemical behavior of azodicarboxamide(ACA) film immobilized on the surface of penicillamine(PNA)/Zn Se-quantum dot(Zn Se-QD) gold nanoparticle(Au NPs) Au electrode. Electrocatalytic acti...This work describes the electrochemical behavior of azodicarboxamide(ACA) film immobilized on the surface of penicillamine(PNA)/Zn Se-quantum dot(Zn Se-QD) gold nanoparticle(Au NPs) Au electrode. Electrocatalytic activity of modified electrode toward the oxidation of cysteine(Cy SH) was investigated. The surface structure and composition of the sensor were characterized by scanning electron microscopy(SEM). Oxidation of Cy SH on the surface of modified electrode was investigated with cyclic voltammetry, electrochemical impedance spectroscopy(EIS),hydrodynamic voltammetry and chronoamperometry methods. The results show that the PNA/Zn Se-QD/ACA film displays excellent electrochemical catalytic activities towards Cy SH oxidation. The modified electrode shows reproducible behavior and high level of stability during the electrochemical experiments. Also it has short response time, low detection limit, high sensitivity and low operation potential, which can be used as an amperometric sensor for monitoring of Cy SH. The proposed modified electrode was successfully used for determination of Cy SH in real sample such as human serum.展开更多
Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)como...Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)comodified Ti/PbO_(2)electrodes(Ti/PbO2CeSDBS).Ce and SDBS could greatly change the electronic structure and interface property of PbO2.Ti/PbO_(2)CeSDBS exhibited excellent electrocatalytic activity and stability in Rhodamine B(RhB)electrocatalytic oxidation reaction.The improved electrocatalytic activity associates with the synergistic effect of electronic and interface factors.In the electrochemical degradation of RhB,the removal efficiencies of RhB and COD are about 0.880 and 0.694 respectively after the electrolysis of 220 min with Ti/PbO_(2)Ce4SDBS40,which are higher than the contrast Ti/PbO_(2)electrodes.In the meantime,the accelerated lifetime of Ti/PbO_(2)Ce4SDBS40 is more than 6.2 times than that of Ti/PbO_(2).展开更多
In this paper In_2O_3 nanoshells have been synthesized via a facile hydrothermal approach.The nanoshells can be completely cracked into pony-size nanocubes by annealing,which are then used as a support of Pt catalyst ...In this paper In_2O_3 nanoshells have been synthesized via a facile hydrothermal approach.The nanoshells can be completely cracked into pony-size nanocubes by annealing,which are then used as a support of Pt catalyst for methanol and ethanol electrocatalytic oxidation.The prepared In_2O_3 and supported Pt catalysts(Pt/In_2O_3) were characterized by X-ray diffraction(XRD),energy dispersive X-ray spectroscopy(EDS),X-ray photoelectron spectroscopy(XPS),field effect scanning electron microscopy(FESEM),and transmission electron microscopy(TEM).Cyclic voltammetry(CV),linear sweep voltammetry(LSV),chronoamperometry and electrochemical impedance spectroscopy(EIS) were carried out,indicating the excellent catalytic performance for alcohol electrooxidation can be achieved on Pt/In_2O_3 nanocatalysts due to the multiple active sites,high conductivity and a mass of microchannels and micropores for reactant diffusions arising from 3D frame structures compared with that on the Pt/C catalysts.展开更多
Geopolymers have been developed to various catalysts due to their advantages.However,low conductivity restricts their application in the electrocatalysis field.In this study,anα-Fe_(2)O_(3)/circulating fluidized bed ...Geopolymers have been developed to various catalysts due to their advantages.However,low conductivity restricts their application in the electrocatalysis field.In this study,anα-Fe_(2)O_(3)/circulating fluidized bed fly ash based geopolymer(CFAG)composite anode was fabricated using a facile dip-coating method by loadingα-Fe_(2)O_(3) in the matrix of CFAG.The effects ofα-Fe_(2)O_(3) content on the composition,surface morphology and electrochemical performance ofα-Fe_(2)O_(3)/CFAG composite anode were investigated.The X-ray diffraction(XRD)and scanning electron microscope(SEM)results demonstrated thatα-Fe_(2)O_(3) was successfully inlaid with the surface of amorphous CFAG matrix.The electrochemical measurements indicated thatα-Fe_(2)O_(3)/CFAG composite anode had higher oxygen evolution potential,greater electrochemical activity area,and smaller electrochemical impedance than CFAG.The as-prepared composite anode was applied for electrocatalytic degradation of indigo carmine dye wastewater.It was discovered that the highest degradation efficiency over 10α-Fe_(2)O_(3)/CFAG reached up 92.6%,and the degradation of indigo carmine followed pseudo-first-order kinetics.Furthermore,10α-Fe_(2)O_(3)/CFAG composite anode presented excellent stability after five cycles.The active hydroxyl radical was generated over theα-Fe_(2)O_(3)/CFAG composite anode,which acted as strong oxidizing agents in the electrocatalytic degradation process.展开更多
A stable copper(hydr)oxide-modified electrode was prepared in 0.5 mol/L NaOH solution by cyclic voltammetry in the range of -250 to 1 000 mV.It can be used for electrochemical studies in the range of -250 to 1000 mV w...A stable copper(hydr)oxide-modified electrode was prepared in 0.5 mol/L NaOH solution by cyclic voltammetry in the range of -250 to 1 000 mV.It can be used for electrochemical studies in the range of -250 to 1000 mV without interfering peaks because there is no oxidation of copper.During an anodic potential sweep,the electro-oxidation of saccharose on Cu occurred by the formation of CuⅢ and this reaction also occurred in the early stages of the reversed cycle until it is stopped by the negative potentials.A mechanism based on the electro-chemical generation of CuⅢ active sites and their subsequent consumption by saccharose was proposed,and the rate law and kinetic parameters were obtained.The charge transfer resistance from theoretical and impedance studies was used to verify the mechanism.Under chronoamperometry regimes,the reaction followed Cottrellian behavior.The transfer of up to 21 electrons was observed in further investigations of the electro-oxidation of saccharose on a(hydr)oxide Cu rotating disk electrode.展开更多
Hydroxyl radicals(·OH) generated on anode play a vital role in electrochemical oxidation(EO) of organic pollutants for water treatment. Inspired by the four-electron oxygen evolution reaction(OER), we supposed an...Hydroxyl radicals(·OH) generated on anode play a vital role in electrochemical oxidation(EO) of organic pollutants for water treatment. Inspired by the four-electron oxygen evolution reaction(OER), we supposed an anode-selection strategy to stabilize deeply oxidized states(*O and*OOH) which are beneficial to generating·OH. To verify the hypothesis, a candidate anode component(MIL-101(Cr), a well-known metal-organic framework with active variable-valence transition metal centers) was used to coat Ti/TiO_(2)plate to fabricate anodes. Compared to TiO_(2)(101) plane on undecorated anode surface, fast and complete removal of aniline and phenol, and improved energy utilization were achieved on MIL-101(Cr)-coatedTi/TiO_(2)anode. Mechanism investigation, including pollutant degradation pathways, showed the predominate contribution(69.60%–75.13%) of·OH in pollutant mineralization. Density functional theory(DFT)computations indicated Cr site in MIL-101(Cr) was more conducive to stabilizing*O and*OOH, leading to thermodynamical spontaneous generation of·OH. This work opens up an exciting avenue to explore·OH production, and supplies a useful guidance to the development of anode materials for EO process.展开更多
The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising technique.Nonetheless,it remains a great challenge due to the lack o...The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising technique.Nonetheless,it remains a great challenge due to the lack of simple,cheap,highefficient electrocatalysts.Here,we successfully develop a simple and scalable electro-deposition and subsequent phosphorization route to fabricate Ni-doped Co_(2)P(Ni-Co_(2)P)nanosheets catalyst using the in-situ released Ni species from defective Ni foam as metal source.Impressively,the as-synthesized Ni-Co_(2)P catalyst exhibits excellent electrochemical 5-hydroxymethylfurfural oxidation reaction(HOR)performance with>99%2,5-furandicarboxylic acid yield and>97%Faradaic efficiency at an ultralow potential of 1.29 V vs.reversible hydrogen electrode(RHE).Experimental characterization and theoretical calculation reveal that the atomically doped Ni species can enhance the adsorption of reactant and thus lower the reaction energy barriers.By coupling the electrocatalytic HOR with HER,the employed two-electrode system using Ni-Co_(2)P and commercial Ni foam as anode and cathode,respectively,exhibits a low cell voltage of 1.53 V to drive a current density of 10 mA·cm^(−2),which is 90 mV lower than that of pure water splitting.This work provides a facile and efficient approach for the preparation of high-performance earth-abundant electrocatalysts toward the concurrent production of H_(2)and value-added chemicals.展开更多
Oxygen evolution reaction(OER)is pivotal to drive green hydrogen generation from water electrolysis,but yet is strictly overshadowed by the sluggish reaction kinetics.Earth-abundant and cut-price transitionmetal compo...Oxygen evolution reaction(OER)is pivotal to drive green hydrogen generation from water electrolysis,but yet is strictly overshadowed by the sluggish reaction kinetics.Earth-abundant and cut-price transitionmetal compounds,particularly Co Fe layered-double-hydroxides(LDHs),show the distinct superiorities in contrast to noble metals and their derivatives.In this review,we firstly underline their fundamental issues in electrocatalytic water oxidation,including Co Fe LDHs crystal structure,the surface of(hydr)oxides confined to OER and the controversial roles of Fe species,aiming at understanding the structure-related activity and catalytic mechanism.Advanced approaches for optimizing OER activity of Co Fe LDHs are then comprehensively overviewed,which will shed light on the different working mechanisms and provide a concise analysis of their unique advantages.Finally,a perspective on the future development of Co Fe LDHs electrocatalysts is offered.We hope this review can give a concise and explicit guidance for the development of transition-metal-based electrocatalysts in the energy field.展开更多
Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrop...Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.展开更多
The dye industry produces a large amount of hazardous wastewater every day worldwide,which brings potential threaten to the global environment.As an excellent method for removal of water chroma and chemical oxygen dem...The dye industry produces a large amount of hazardous wastewater every day worldwide,which brings potential threaten to the global environment.As an excellent method for removal of water chroma and chemical oxygen demand,electrocatalytic methods are currently widely used in the treatment of dye wastewater.The selection and preparation of electrode materials and electrocatalysts play an important role on the electrocatalytic treatment.The aim of this paper is to introduce the most excellent high-efficiency electrode materials and electrocatalysts in the field of dye wastewater treatment.Many electrode materials such as metal electrode materials,boron-doped diamond anode materials and three-dimensional electrode are introduced in detail.Besides,the mechanism of electrocatalytic oxidation is summarized.The composite treatment of active electrode and electrocatalyst are extensively examined.Finally,the progress of photo-assisted electrocatalytic methods of dye wastewater and the catalysts are described.展开更多
In this paper,we describe the synthesis of the AC-PtNi/G catalysts with graphene as the carrier,via the alcohol reduction and the sulfuric acid treatment.The prepared catalysts were microscopically characterized by X-...In this paper,we describe the synthesis of the AC-PtNi/G catalysts with graphene as the carrier,via the alcohol reduction and the sulfuric acid treatment.The prepared catalysts were microscopically characterized by X-ray diffractometry(XRD),X-ray photoelectron spectroscopy(XPS),scanning electron microscopy(SEM),electron spectroscopy(EDAX),and transmission electron micros-copy(TEM).We tested the electrochemical performance of the prepared catalysts using an electrochemical workstation and in situ infrared spectroscopy(FTIR).The results showed that the acid-treated AC-PtNi/G catalysts had a more uniform dispersion and with the increased of treatment time,the particle size of the catalyst became smaller.And the electrocatalytic performance of the AC-PtNi/G-48h catalyst treated with sulfuric acid for 48 h was significantly better than that of the untreated PtNi/G catalyst.Its electrochemically active surface area was 76.63 m^(2)/g,and the peak current density value for catalytic oxidation of ethanol was 1218.83 A/g,which was 10 times that of ordinary commercial Pt/C catalyst.The steady-state current density value of 1100 s was 358.77 A/g,and it has excellent anti-CO toxicity performance.It was determined that a sulfuric acid treatment controlled catalyst particle size and increased the electrocatalytic activity of the catalytic oxidation of ethanol.展开更多
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.
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 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.
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 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Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang,Grant/Award Number:2019R01006National Key R&D Program of China,Grant/Award Number:2018YFB0104300。
文摘The oxygen evolution reaction(OER)activity of single-atom catalysts(SACs)is closely related to the coordination environment of the active site.Oxygencoordinated atomic metal species bring about unique features beyond nitrogen-coordinated atomic metal species due to the fact that the M-O bond is weaker than the M-N bond.Herein,a series of metal-oxygen-carbon structured low-nucleus clusters(LNCs)are successfully anchored on the surface of multiwalled carbon nanotubes(M-MWCNTs,M=Ni,Co,or Fe)through a foolproof low-temperature gas transfer(300℃)method without any further treatment.The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations.The synthetic Ni-MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions,transcending the performances of Co-MWCNTs,Fe-MWCNTs and RuO_(2).Density functional theory calculations reveal that the moderate oxidation of low-nucleus Ni clusters changes the unoccupied orbital of Ni atoms,thereby lowering the energy barrier of the OER rate-limiting step and making the OER process more energy-efficient.This study demonstrates a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts.
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 by the National Natural Science Foundation of China(22078374,21776324)the Scientific and Technological Planning Project of Guangzhou(202206010145)+2 种基金the National Ten Thousand Talent Plan,Key-Area Research and Development Program of Guangdong Province(2019B110209003)the Guangdong Basic and Applied Basic Research Foundation(2019B1515120058,2020A1515011149)the Start-up Fund for Senior Talents in Jiangsu University(21JDG060)。
文摘Selective upgrading of C=O bonds to afford carboxylic acid is significant for the petrochemical industry and biomass utilization.Here we declared the efficient electrooxidation of biomass-derived aldehydes family over NiV-layered double hydroxides(LDHs) thin films.Mechanistic studies confirmed the hydroxyl active intermediate(-OH*) generated on the surface of NiV-LDHs films by employing electrochemical impedance spectroscopy and the electron paramagnetic resonance spectroscopy.By using advanced techniques,e.g.,extended X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy,NiV-LDHs films with 2.6 nm could expose larger specific surface area.Taking benzaldehyde as a model,high current density of 200 mA cm^(-2)at 1.8 V vs.RHE,81.1% conversion,77.6% yield of benzoic acid and 90.8% Faradaic efficiency were reached,which was superior to most of previous studies.Theoretical DFT analysis was well matched with experimental findings and documented that NiV-LDHs had high adsorption capacity for the aldehydes to suppress the side reaction,and the aldehydes were oxidized by the electrophilic hydroxyl radicals formed on NiV-LDHs.Our findings offer a universal strategy for the robust upgrading of diverse biomass-derived platform chemicals.
基金the support of this work by the Khorramabad Branch, Islamic Azad University for financial support
文摘This work describes the electrochemical behavior of azodicarboxamide(ACA) film immobilized on the surface of penicillamine(PNA)/Zn Se-quantum dot(Zn Se-QD) gold nanoparticle(Au NPs) Au electrode. Electrocatalytic activity of modified electrode toward the oxidation of cysteine(Cy SH) was investigated. The surface structure and composition of the sensor were characterized by scanning electron microscopy(SEM). Oxidation of Cy SH on the surface of modified electrode was investigated with cyclic voltammetry, electrochemical impedance spectroscopy(EIS),hydrodynamic voltammetry and chronoamperometry methods. The results show that the PNA/Zn Se-QD/ACA film displays excellent electrochemical catalytic activities towards Cy SH oxidation. The modified electrode shows reproducible behavior and high level of stability during the electrochemical experiments. Also it has short response time, low detection limit, high sensitivity and low operation potential, which can be used as an amperometric sensor for monitoring of Cy SH. The proposed modified electrode was successfully used for determination of Cy SH in real sample such as human serum.
基金Thanks to the financial support from the Science and technology project of Shaanxi Province(2017ZDXM-GY-041).
文摘Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)comodified Ti/PbO_(2)electrodes(Ti/PbO2CeSDBS).Ce and SDBS could greatly change the electronic structure and interface property of PbO2.Ti/PbO_(2)CeSDBS exhibited excellent electrocatalytic activity and stability in Rhodamine B(RhB)electrocatalytic oxidation reaction.The improved electrocatalytic activity associates with the synergistic effect of electronic and interface factors.In the electrochemical degradation of RhB,the removal efficiencies of RhB and COD are about 0.880 and 0.694 respectively after the electrolysis of 220 min with Ti/PbO_(2)Ce4SDBS40,which are higher than the contrast Ti/PbO_(2)electrodes.In the meantime,the accelerated lifetime of Ti/PbO_(2)Ce4SDBS40 is more than 6.2 times than that of Ti/PbO_(2).
基金sponsored by the National Basic Research Program of China(973 Program)under grant no.2015CB351905the National Natural Science Foundation of China(no.61504019)+3 种基金China Postdoctoral Science Foundation(no.2015M580783)Scientific Research Start-up Foundation of University of Electronic Science and Technology of China(Y02002010301082)the Technology Innovative Research Team of Sichuan Province of China(no.2015TD0005)the Fundamental Research Funds for the Central Universities of China(no.ZYGX2015J140)
文摘In this paper In_2O_3 nanoshells have been synthesized via a facile hydrothermal approach.The nanoshells can be completely cracked into pony-size nanocubes by annealing,which are then used as a support of Pt catalyst for methanol and ethanol electrocatalytic oxidation.The prepared In_2O_3 and supported Pt catalysts(Pt/In_2O_3) were characterized by X-ray diffraction(XRD),energy dispersive X-ray spectroscopy(EDS),X-ray photoelectron spectroscopy(XPS),field effect scanning electron microscopy(FESEM),and transmission electron microscopy(TEM).Cyclic voltammetry(CV),linear sweep voltammetry(LSV),chronoamperometry and electrochemical impedance spectroscopy(EIS) were carried out,indicating the excellent catalytic performance for alcohol electrooxidation can be achieved on Pt/In_2O_3 nanocatalysts due to the multiple active sites,high conductivity and a mass of microchannels and micropores for reactant diffusions arising from 3D frame structures compared with that on the Pt/C catalysts.
基金This study was supported by the National Natural Science Foundation of China(No.21676209)Key Research Development Project of Shaanxi Province(No.2019GY-137)the Cultivating Fund of Excellent Doctorate Thesis of Xi’an University of Architecture and Technology(No.6040318008).
文摘Geopolymers have been developed to various catalysts due to their advantages.However,low conductivity restricts their application in the electrocatalysis field.In this study,anα-Fe_(2)O_(3)/circulating fluidized bed fly ash based geopolymer(CFAG)composite anode was fabricated using a facile dip-coating method by loadingα-Fe_(2)O_(3) in the matrix of CFAG.The effects ofα-Fe_(2)O_(3) content on the composition,surface morphology and electrochemical performance ofα-Fe_(2)O_(3)/CFAG composite anode were investigated.The X-ray diffraction(XRD)and scanning electron microscope(SEM)results demonstrated thatα-Fe_(2)O_(3) was successfully inlaid with the surface of amorphous CFAG matrix.The electrochemical measurements indicated thatα-Fe_(2)O_(3)/CFAG composite anode had higher oxygen evolution potential,greater electrochemical activity area,and smaller electrochemical impedance than CFAG.The as-prepared composite anode was applied for electrocatalytic degradation of indigo carmine dye wastewater.It was discovered that the highest degradation efficiency over 10α-Fe_(2)O_(3)/CFAG reached up 92.6%,and the degradation of indigo carmine followed pseudo-first-order kinetics.Furthermore,10α-Fe_(2)O_(3)/CFAG composite anode presented excellent stability after five cycles.The active hydroxyl radical was generated over theα-Fe_(2)O_(3)/CFAG composite anode,which acted as strong oxidizing agents in the electrocatalytic degradation process.
文摘A stable copper(hydr)oxide-modified electrode was prepared in 0.5 mol/L NaOH solution by cyclic voltammetry in the range of -250 to 1 000 mV.It can be used for electrochemical studies in the range of -250 to 1000 mV without interfering peaks because there is no oxidation of copper.During an anodic potential sweep,the electro-oxidation of saccharose on Cu occurred by the formation of CuⅢ and this reaction also occurred in the early stages of the reversed cycle until it is stopped by the negative potentials.A mechanism based on the electro-chemical generation of CuⅢ active sites and their subsequent consumption by saccharose was proposed,and the rate law and kinetic parameters were obtained.The charge transfer resistance from theoretical and impedance studies was used to verify the mechanism.Under chronoamperometry regimes,the reaction followed Cottrellian behavior.The transfer of up to 21 electrons was observed in further investigations of the electro-oxidation of saccharose on a(hydr)oxide Cu rotating disk electrode.
基金supported by the National Natrual Science of China (NSFC, Nos. 51978341, 52070100 and 52011530433)the Natural Science Foundation of Jiangsu Province of China (No. BK20190087)Jiangsu Key Laboratory of New Power Batteries, and a project funded by the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions。
文摘Hydroxyl radicals(·OH) generated on anode play a vital role in electrochemical oxidation(EO) of organic pollutants for water treatment. Inspired by the four-electron oxygen evolution reaction(OER), we supposed an anode-selection strategy to stabilize deeply oxidized states(*O and*OOH) which are beneficial to generating·OH. To verify the hypothesis, a candidate anode component(MIL-101(Cr), a well-known metal-organic framework with active variable-valence transition metal centers) was used to coat Ti/TiO_(2)plate to fabricate anodes. Compared to TiO_(2)(101) plane on undecorated anode surface, fast and complete removal of aniline and phenol, and improved energy utilization were achieved on MIL-101(Cr)-coatedTi/TiO_(2)anode. Mechanism investigation, including pollutant degradation pathways, showed the predominate contribution(69.60%–75.13%) of·OH in pollutant mineralization. Density functional theory(DFT)computations indicated Cr site in MIL-101(Cr) was more conducive to stabilizing*O and*OOH, leading to thermodynamical spontaneous generation of·OH. This work opens up an exciting avenue to explore·OH production, and supplies a useful guidance to the development of anode materials for EO process.
基金the National Key Research and Development(R&D)Program of China(No.2020YFA0406103)the National Natural Science Foundation of China(NSFC)(Nos.21725102,51902311,22122506,91961106,22075267,and 21803002)+5 种基金Strategic Priority Research Program of the CAS(No.XDPB14)Anhui Provincial Natural Science Foundation(No.2008085J05)Youth Innovation Promotion Association of CAS(No.2019444)Open Funding Project of National Key Laboratory of Human Factors Engineering(No.SYFD062010K)Users with Excellence Program of Hefei Science Center CAS(No.2020HSCUE003)Fundamental Research Funds for the Central Universities(No.WK2060000039).
文摘The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising technique.Nonetheless,it remains a great challenge due to the lack of simple,cheap,highefficient electrocatalysts.Here,we successfully develop a simple and scalable electro-deposition and subsequent phosphorization route to fabricate Ni-doped Co_(2)P(Ni-Co_(2)P)nanosheets catalyst using the in-situ released Ni species from defective Ni foam as metal source.Impressively,the as-synthesized Ni-Co_(2)P catalyst exhibits excellent electrochemical 5-hydroxymethylfurfural oxidation reaction(HOR)performance with>99%2,5-furandicarboxylic acid yield and>97%Faradaic efficiency at an ultralow potential of 1.29 V vs.reversible hydrogen electrode(RHE).Experimental characterization and theoretical calculation reveal that the atomically doped Ni species can enhance the adsorption of reactant and thus lower the reaction energy barriers.By coupling the electrocatalytic HOR with HER,the employed two-electrode system using Ni-Co_(2)P and commercial Ni foam as anode and cathode,respectively,exhibits a low cell voltage of 1.53 V to drive a current density of 10 mA·cm^(−2),which is 90 mV lower than that of pure water splitting.This work provides a facile and efficient approach for the preparation of high-performance earth-abundant electrocatalysts toward the concurrent production of H_(2)and value-added chemicals.
基金National Natural Science Foundation of China(Nos.21773093 and 22175077)Natural Science Foundation of Guangdong Province(Nos.2021A1515012351 and 2017B030306004)Guangdong Special Support Program(No.2017TQ04N224)。
文摘Oxygen evolution reaction(OER)is pivotal to drive green hydrogen generation from water electrolysis,but yet is strictly overshadowed by the sluggish reaction kinetics.Earth-abundant and cut-price transitionmetal compounds,particularly Co Fe layered-double-hydroxides(LDHs),show the distinct superiorities in contrast to noble metals and their derivatives.In this review,we firstly underline their fundamental issues in electrocatalytic water oxidation,including Co Fe LDHs crystal structure,the surface of(hydr)oxides confined to OER and the controversial roles of Fe species,aiming at understanding the structure-related activity and catalytic mechanism.Advanced approaches for optimizing OER activity of Co Fe LDHs are then comprehensively overviewed,which will shed light on the different working mechanisms and provide a concise analysis of their unique advantages.Finally,a perspective on the future development of Co Fe LDHs electrocatalysts is offered.We hope this review can give a concise and explicit guidance for the development of transition-metal-based electrocatalysts in the energy field.
基金the National Natural Science Foundation of China(Nos.51878325,51868050,51622806,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)the Graduate Innovation Fund of Jiangxi Province(No.YC2018-S360)。
文摘Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.
基金supported by Nankai University&Cangzhou Bohai New Area Institute of Green Chemical Engineering Fund(Grant No.NCC2020FH11).
文摘The dye industry produces a large amount of hazardous wastewater every day worldwide,which brings potential threaten to the global environment.As an excellent method for removal of water chroma and chemical oxygen demand,electrocatalytic methods are currently widely used in the treatment of dye wastewater.The selection and preparation of electrode materials and electrocatalysts play an important role on the electrocatalytic treatment.The aim of this paper is to introduce the most excellent high-efficiency electrode materials and electrocatalysts in the field of dye wastewater treatment.Many electrode materials such as metal electrode materials,boron-doped diamond anode materials and three-dimensional electrode are introduced in detail.Besides,the mechanism of electrocatalytic oxidation is summarized.The composite treatment of active electrode and electrocatalyst are extensively examined.Finally,the progress of photo-assisted electrocatalytic methods of dye wastewater and the catalysts are described.
基金This work was supported by the National Natural Science Foundation of China(Nos.51864040,51974167)the Natural Science Fund of Inner Mongolia Autonomous Region,China(No.2018LH02006).
文摘In this paper,we describe the synthesis of the AC-PtNi/G catalysts with graphene as the carrier,via the alcohol reduction and the sulfuric acid treatment.The prepared catalysts were microscopically characterized by X-ray diffractometry(XRD),X-ray photoelectron spectroscopy(XPS),scanning electron microscopy(SEM),electron spectroscopy(EDAX),and transmission electron micros-copy(TEM).We tested the electrochemical performance of the prepared catalysts using an electrochemical workstation and in situ infrared spectroscopy(FTIR).The results showed that the acid-treated AC-PtNi/G catalysts had a more uniform dispersion and with the increased of treatment time,the particle size of the catalyst became smaller.And the electrocatalytic performance of the AC-PtNi/G-48h catalyst treated with sulfuric acid for 48 h was significantly better than that of the untreated PtNi/G catalyst.Its electrochemically active surface area was 76.63 m^(2)/g,and the peak current density value for catalytic oxidation of ethanol was 1218.83 A/g,which was 10 times that of ordinary commercial Pt/C catalyst.The steady-state current density value of 1100 s was 358.77 A/g,and it has excellent anti-CO toxicity performance.It was determined that a sulfuric acid treatment controlled catalyst particle size and increased the electrocatalytic activity of the catalytic oxidation of ethanol.
