Regenerative catalytic oxidizers(RCO)are widely used to remove volatile organic compounds(VOCs)due to their energy-saving and stability.In this study,a multi-component catalytic reaction model was constructed to numer...Regenerative catalytic oxidizers(RCO)are widely used to remove volatile organic compounds(VOCs)due to their energy-saving and stability.In this study,a multi-component catalytic reaction model was constructed to numerically investigate the reaction process of hydrocarbon-containing VOCs in RCO using computational fluid dynamics(CFD)simulation.To obtain the conversion characteristics of multi-component hydrocarbons,the effects of intake load,equivalence ratio,and the composition of multi-component hydrocarbons on the flow,heat transfer,and conversion rate of the reactor were analyzed.A feasibility study plan targeting the hard-to-convert components was also proposed.The results indicated that as the load increases,the conversion rates of the various components decrease,while the reaction rates increase.Moreover,increasing the flow velocity intensifies turbulence and enhances the collision frequency between the gas and the wall surfaces.This,in turn,amplifies the resistance effect of the porous medium.As the equivalence ratio of VOCs to oxygen increases,the oxygen-deficient condition leads to a decrease in the molecular weight of the hydrocarbons involved in the reaction.The reaction temperature also shows a downward trend.A comparative analysis of the catalytic combustion characteristics of multi-component VOCs and single-component gases reveals that adding ethane and propane can facilitate methane oxidation.展开更多
By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68...By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68H_(2)O(1)has been successfully obtained via one-pot method and systematically characterized by IR,XPS,solid UV spectra,PXRD pattern,and TGA analysis.The analysis of X-ray crystallography exhibits that compound 1 crystallizes in the triclinic space group P-1 and presents a novel square-shaped Zr-substituted tetrameric polyoxometalate.The catalytic oxidation of sulfides by 1 are carried out,which demonstrate that 1 exhibits a good performance for the catalytic oxidation of sulfides to sulfones with high conversion(100%)and high selectivity(100%).展开更多
A novel tetra-europium(III)-containing antimonotungstate,Na_(8.2)[H_(2)N(CH_(3))_(2)]_(9)[Na_(10.8)(tar)_(4)(H_(2)O)_(20)(Eu_(2)Sb_(2)W_(21)O_(72))_(2)]·44.5H_(2)O(EuSbW,H_(4)tar=dl-tartaric acid),has been synthe...A novel tetra-europium(III)-containing antimonotungstate,Na_(8.2)[H_(2)N(CH_(3))_(2)]_(9)[Na_(10.8)(tar)_(4)(H_(2)O)_(20)(Eu_(2)Sb_(2)W_(21)O_(72))_(2)]·44.5H_(2)O(EuSbW,H_(4)tar=dl-tartaric acid),has been synthesized and characterized.The dimeric polyoxoanion of EuSbW consists of two Dawson-like{Eu_(2)Sb_(2)W_(21)}units bridged by four dl-tartaric acid ligands.The adjacent carboxyl and hydroxy groups in each tartaric acid simultaneously chelate with W and Eu atoms from different{Eu_(2)Sb_(2)W_(21)}units,thereby forming the dimeric structure.EuSbW represents an extremely rare polyoxometalate where four tartaric acid ligands function as connectors to bridge two{Eu_(2)Sb_(2)W_(21)}units.Additionally,EuSbW exhibits excellent catalytic activity and reusability in the oxidation of thioethers and alcohols,achieving 100%conversion and>99%selectivity for various thioethers,and 85–100%conversion with 90–99%selectivity for diverse alcohols under mild conditions.展开更多
Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and re...Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.展开更多
Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction ...Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.展开更多
Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid ...Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid catalyst Co-Bent(bentonite supported cobalt)was prepared by blending method for MgSO_(3) oxidation with bentonite as the carrier and cobalt as the active component.At the calcination temperature of 550℃ and the Co loading level of 3 wt.%,the catalyst showed excellent catalytic performance for the oxidation of high concentration MgSO_(3) slurry,and the oxidation rate of MgSO_(3) was 0.13 mol/(L·h).The research indicated that the active component was uniformly distributed within porous structure of the catalyst as Co_(3)O_(4),which facilitated the oxidation of SO_(3)^(2-) catalyzed by Co_(3)O_(4).Kinetic researches indicated the oxidation rate of MgSO_(3) was influenced by the catalyst dosage,the reaction temperature,the solution pH,the airflow rate,and the SO_(3)^(2-) concentration.Additionally,after recycling experiments,the regenerated catalyst retained its high catalytic performance for the MgSO_(3) oxidation.The reaction mechanism for the catalytic oxidation of MgSO_(3) by Co-Bent catalyst was also proposed.The generation of active free radicals(OH·,SO_(4)^(-)·,SO_(3)^(-)·,SO_(5)^(-)·)accelerated the MgSO_(3) oxidation.These results provide theoretical support for the treatment of MgSO_(3) and the development of durable catalyst.展开更多
Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great c...Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great challenge.In present work,a new strategy of chloride anion intercalation in Bi_(2)O_(3)via one-pot hydrothermal process is proposed.The as-prepared Ta-BiOCl/Bi_(24)O_(31)Cl_(10)(TBB)heterojunctions are featured with Ta-Bi_(24)O_(31)Cl_(10)and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces.In this TBB heterojunctions,the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer andmultiple transfer paths,respectively,leading to enhanced visible light response and improved photogenerated charge separation.Meanwhile,a type-II heterojunction for photocharge separation has been obtained,in which photogenerated electrons are drove from the CB(conduction band)of Ta-Bi_(24)O_(31)Cl_(10)to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl,while the photogenerated holes are left on the VB(valence band)of Ta-Bi_(24)O_(31)Cl_(10),effectively hindering the recombination of photogenerated electron-hole pairs.Furthermore,the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species(·O_(2)^(−)).Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride(TCH)solution to Bi_(2)O_(3),Ta-BiOCl and Ta-Bi_(24)O_(31)Cl_(10).This work not only proposes a Ta-BiOCl/Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-Ⅱheterojunction for highly efficient photocatalytic activity,but offers a new insight into the design of highly efficient heterojunction through phasestructure synergistic transformation strategy.展开更多
Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow...Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow-loading of Ru single atoms(0.42 wt%)into Mn_(2)O_(3)matrix(0.4%Ru-Mn_(2)O_(3))greatly boosts its catalytic activity for the aerobic oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA).The FDCA productivity over the 0.4%Ru-Mn_(2)O_(3)(5.4 mmol_(FDCA)g_(cat)h^(-1))is 4.9 times higher than the Mn_(2)O_(3).Especially,this FDCAproductivity is also significantly higher than that of existing Ru and Mn-based catalysts.Experimental and theoretical investigations discovered that the Ru single atom facilitated the formation of oxygen vacancy(O_(v))in the catalyst,which synergistically weakened the Mn-O bond and promoted the activation of O_L.The co-presence of Ru single atoms and O_(v)also promote the adsorption and activation of both O_(2)and HMF.Consequently,the dehydrogenation reaction energy barrier of the rate-determining step was reduced via both the O_L and chemisorbed O_(2)dehydrogenation pathways,thus boosting the catalytic oxidation reactions.展开更多
Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the under...Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the underpinning mechanism remains elusive.Herein,the introduction of silanol nests enables the alloy formation on the SiO_(2)surface.The amination modification is disclosed to induce the electron transfer from RE to Pt and weaken the adsorption of CO on electron-rich Pt species.In situ/operando spectroscopic analyses in conjunction with density functional theory calculations demonstrate the electronic couple of Pt atoms and adjacent Ce atoms concurrently achieves the enhancement of CO oxidation and suppression of H_(2)oxidation.Additionally,CO_(2)is readily desorbed from the Pt_(5)Ce(111)surface to enhance intrinsic activity and longevity.These findings provide an atomic-level insight into the synergistic catalytic sites on regulating the electronic state of the Pt-RE alloy catalysts toward highly selective oxidation reactions.展开更多
Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by...Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by different amounts of cerium,which not only enhances the physicochemical stability but also increases the number of active sites of Ce_(x)Zr_(y)UiO-66.Furthermore,the catalysts with Co_(3)O_(4)nanoparticles supported on Ce_(x)Zr_(y)UiO-66 were successfully prepared via impregnation method.In the process of toluene degradation,the Co/Ce_(1)Zr_(2)-Ui0-66 attains a 90%conversion rate at 210℃with a space velocity of 60000 mL/(g·h)and toluene concentration at 1000×10^(-6).Meanwhile,the carbon dioxide selectivity reaches 100%at 218℃.The Co/Ce_(1)Zr_(2)-UiO-66 shows great water resistance(3 vol%H_(2)O).Multiple characterization methods were used to figure out the physicochemical properties of the catalysts.It is found that the addition of an appropriate amount of cerium can enhance stability of UiO-66 and surface lattice oxygen proportion.Additionally,the stronger electron transfer between Ce^(4+)and Co^(2+)enables the Co/Ce_(1)Zr_(2)-UiO-66 to possess more active surface oxygen species and Co_(3)+cationic species in all samples.展开更多
Volatile organic compounds(VOCs)exhausted from industrial processes are the major atmospheric pollutants,which could destroy the ecological environment and make hazards to human health seriously.Catalytic oxidation is...Volatile organic compounds(VOCs)exhausted from industrial processes are the major atmospheric pollutants,which could destroy the ecological environment and make hazards to human health seriously.Catalytic oxidation is regarded as the most competitive strategy for the efficient elimination of low-concentration VOCs.Supported noble metal catalysts are preferred catalysts due to their excellent low-temperature catalytic activity.To further lower the cost of catalysts,single atom catalysts(SAC)have been fabricated and extensively studied for application in VOCs oxidation due to their 100%atom-utilization efficiency and unique catalytic performance.In this review,we comprehensively summarize the recent advances in supported noble metal(e.g.,Pt,Pd,Au,and Ag)catalysts and SAC for VOCs oxidation since 2015.Firstly,this paper focuses on some important influencing factors that affect the activity of supported noble metal catalysts,including particle size,valence state and dispersion of noble metals,properties of the support,metal oxide/ion modification,preparation method,and pretreatment conditions of catalysts.Secondly,we briefly summarize the catalytic performance of SAC for typical VOCs.Finally,we conclude the key influencing factors and provide the prospects and challenges of VOCs oxidation.展开更多
In this work the heterogenization in polymeric membranes of decatungstate,a photocatalyst for oxidation reactions,was reported.Solid state characterization techniques confirmed that the catalyst structure was preserve...In this work the heterogenization in polymeric membranes of decatungstate,a photocatalyst for oxidation reactions,was reported.Solid state characterization techniques confirmed that the catalyst structure was preserved within the polymeric membranes.The catalytic membranes were successfully applied in the aerobic photo-oxidation of phenol,one of the main organic pollutants in wastewater,providing stable and recyclable photocatalytic systems.The dependence of the phenol degradation rate by the catalyst loading and transmembrane pressure was shown.By comparison with homogeneous reaction,the catalyst heterogenized in membrane appears to be more efficient concerning the rate of phenol photodegradation and mineralization.展开更多
Formaldehyde(HCHO)is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The developme...Formaldehyde(HCHO)is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.展开更多
Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the ...Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.展开更多
Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visi...Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light.The Er@K-C_(3)N_(4)/UiO-66-NH_(2) catalyst was synthesized using a straight-forward hydrothermal technique,and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid.The catalyst was thoroughly characterized,confirming the effective adjustment of the band gap energy of Er@K-C_(3)N_(4)/UiO-66-NH_(2).Upon the optimized reaction conditions,the conversion rate of furfural reached 89.3%,with a corresponding yield of furoic acid at 79.8%.The primary reactive oxygen species was identified as·O_(2)^(-) from ESR spectra and scavenger tests.The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate,hence increasing the separating efficiency of photogenerated electron-hole pairs.This study expands the potential applications of rare earth element doped g-C_(3)N_(4) in the photocatalytic selective oxidation of furfurans.展开更多
Because phenolic compounds are toxic for methanogenic bacteria many problems concerning the high toxicity and biodegradability of the olive oil mill wastewater (OMW) have been encountered during anaerobic treatments o...Because phenolic compounds are toxic for methanogenic bacteria many problems concerning the high toxicity and biodegradability of the olive oil mill wastewater (OMW) have been encountered during anaerobic treatments of this effluent. In this work, we try to develop a new catalytic process for the degradation of phenolic compounds, producing less toxic OMW for methanogenic bacteria, facilitating the anaerobic digestion. This process consists of an oxidative reaction using copper supported on alumina pillared clay in presence of a photocatalytic system (H2O2 with UV light). Preliminary results showed that the use of the copper supported catalyst in presence of 0.88% H2O2 (v/v) allows after 2 h colour reduction (25%), significant abatement of total organic carbon (40%), and important removal of polyphenolic compounds (63%) especially those of high molecular mass and subsequently decreases the OMW toxicity from 100% to 70%. This catalytic pre-treatment process of OMW was efficient for anaerobic digestion.展开更多
KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these cat...KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.展开更多
The MoOx/AuNPs composite film modified glassy carbon electrode was fabricated by electro-depositing simultaneously gold nanoparticles and molybdenum oxides using cyclic voltammetry. The morphology and topography of th...The MoOx/AuNPs composite film modified glassy carbon electrode was fabricated by electro-depositing simultaneously gold nanoparticles and molybdenum oxides using cyclic voltammetry. The morphology and topography of the MoOx/AuNPs composite were char-acterized by scan electron microscopy and X-ray photoelectron spectroscopy respectively, and the electrocatalytic oxidation of glucose at the MoOx/AuNPs composite film was inves-tigated and analyzed in detail. It was shown that the MoOx/AuNPs composite was of strong electrocatalytic activity towards oxidation of glucose as well as other saccharides, so that an attempt was made for direct voltammetric determination of glucose. Then the positive scan polarization reverse catalytic voltammetry was proposed for the first time. Based on this method, the pure oxidation current was extracted by subtraction of the blank current in the reverse scan. The current sensitivity was enhanced tremendously and the signal to noise ra-tio was improved adequately. The electrocatalytic oxidation of glucose at the MoOx/AuNPs modified electrode was performed in alkaline medium, a wide linear range from 0.01 mmol/L to 4.0 mmol/L of glucose, a higher current sensitivity of 2.35 mA/(mmol/L·cm2), and a lower limit of detection of 9.01 μmol/L (at signal/noise=3) were achieved. In addition, the electrocatalytic oxidation of other saccharides such as lactose, fructose and sucrose was also evaluated.展开更多
Mesoporous TiO2 ceramic films have been prepared upon the Ti alloy substrate by the micro-arc oxidation (MAO) technology. To enhance the photo-catalytic property of the films, Eu2O3 particles were added into the elect...Mesoporous TiO2 ceramic films have been prepared upon the Ti alloy substrate by the micro-arc oxidation (MAO) technology. To enhance the photo-catalytic property of the films, Eu2O3 particles were added into the electrolyte solution of Na2CO3/Na2SiO3. Scanning electron microscope (SEM), energy dispersive (EDS), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) are employed to characterize the modified films. Diffuse reflectance spectra (DRS) test, photo-generated current test and photo decomposition test are applied to evaluate the photo-catalytic property of the modified films. The results show that Eu2O3 transformed into one-dimensional (1-D) nano-wires embedded within the composite film, and the film has high photo-catalytic property.展开更多
This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hy...This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hydroxide-carbonate nanoparticles with various morphologies(i.e.,nanorods,nanosheets,and nanocubes) were successfully synthesized,and Co3O4 nanoparticles were obtained by thermal decomposition of the cobalt-hydroxide-carbonate precursors.The results suggest that the cobalt source is a key factor for controlling the morphology of cobalt-hydroxide-carbonate at relatively low hydrothermal temperatures(≤ 140℃).Nanorods can be synthesized in CoCl2 solution,while Co(NO3)2 solution promotes the formation of nanosheets.Further increasing the synthesis temperature(higher than 140 ℃) results in the formation of nanocubes in either Co(NO3)2 or CoCl2 solution.The reaction time only affects the size of the obtained nanoparticles.The presence of CTAB could improve the uniformity and dispersion of particles.Co3O4 nanosheets showed much higher catalytic activity for CO oxidation than nanorods and nanocubes because it has more abundant Co^(3+) on the surface,much higher reducibility,and better oxygen desorption capacity.展开更多
基金supported by National Key Research&Development Program of China(2022YFB4101500).
文摘Regenerative catalytic oxidizers(RCO)are widely used to remove volatile organic compounds(VOCs)due to their energy-saving and stability.In this study,a multi-component catalytic reaction model was constructed to numerically investigate the reaction process of hydrocarbon-containing VOCs in RCO using computational fluid dynamics(CFD)simulation.To obtain the conversion characteristics of multi-component hydrocarbons,the effects of intake load,equivalence ratio,and the composition of multi-component hydrocarbons on the flow,heat transfer,and conversion rate of the reactor were analyzed.A feasibility study plan targeting the hard-to-convert components was also proposed.The results indicated that as the load increases,the conversion rates of the various components decrease,while the reaction rates increase.Moreover,increasing the flow velocity intensifies turbulence and enhances the collision frequency between the gas and the wall surfaces.This,in turn,amplifies the resistance effect of the porous medium.As the equivalence ratio of VOCs to oxygen increases,the oxygen-deficient condition leads to a decrease in the molecular weight of the hydrocarbons involved in the reaction.The reaction temperature also shows a downward trend.A comparative analysis of the catalytic combustion characteristics of multi-component VOCs and single-component gases reveals that adding ethane and propane can facilitate methane oxidation.
基金financially supported by the National Natural Science Foundation of China(No.22071043).
文摘By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68H_(2)O(1)has been successfully obtained via one-pot method and systematically characterized by IR,XPS,solid UV spectra,PXRD pattern,and TGA analysis.The analysis of X-ray crystallography exhibits that compound 1 crystallizes in the triclinic space group P-1 and presents a novel square-shaped Zr-substituted tetrameric polyoxometalate.The catalytic oxidation of sulfides by 1 are carried out,which demonstrate that 1 exhibits a good performance for the catalytic oxidation of sulfides to sulfones with high conversion(100%)and high selectivity(100%).
基金supported by the Natural Science Foundation of Jiangxi Province(20232ACB213005).
文摘A novel tetra-europium(III)-containing antimonotungstate,Na_(8.2)[H_(2)N(CH_(3))_(2)]_(9)[Na_(10.8)(tar)_(4)(H_(2)O)_(20)(Eu_(2)Sb_(2)W_(21)O_(72))_(2)]·44.5H_(2)O(EuSbW,H_(4)tar=dl-tartaric acid),has been synthesized and characterized.The dimeric polyoxoanion of EuSbW consists of two Dawson-like{Eu_(2)Sb_(2)W_(21)}units bridged by four dl-tartaric acid ligands.The adjacent carboxyl and hydroxy groups in each tartaric acid simultaneously chelate with W and Eu atoms from different{Eu_(2)Sb_(2)W_(21)}units,thereby forming the dimeric structure.EuSbW represents an extremely rare polyoxometalate where four tartaric acid ligands function as connectors to bridge two{Eu_(2)Sb_(2)W_(21)}units.Additionally,EuSbW exhibits excellent catalytic activity and reusability in the oxidation of thioethers and alcohols,achieving 100%conversion and>99%selectivity for various thioethers,and 85–100%conversion with 90–99%selectivity for diverse alcohols under mild conditions.
基金supported by National Natural Science Fundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn202211012)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.
基金supported by the Beijing Nova Program(No.20220484215)National Key Research and Development Program of China(Nos.2022YFB3504100,2022YFB3506200,2021YFA1500300 and 2022YFA1500146)National Natural Science Foundation of China(Nos.22376217,22208373,22272090 and 22272106)。
文摘Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.
基金supported by the State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology (No. 2022TS10)the Taishan Industrial Experts Programthe Natural Science Foundation of Shandong Province of China (No. ZR2023ME212).
文摘Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid catalyst Co-Bent(bentonite supported cobalt)was prepared by blending method for MgSO_(3) oxidation with bentonite as the carrier and cobalt as the active component.At the calcination temperature of 550℃ and the Co loading level of 3 wt.%,the catalyst showed excellent catalytic performance for the oxidation of high concentration MgSO_(3) slurry,and the oxidation rate of MgSO_(3) was 0.13 mol/(L·h).The research indicated that the active component was uniformly distributed within porous structure of the catalyst as Co_(3)O_(4),which facilitated the oxidation of SO_(3)^(2-) catalyzed by Co_(3)O_(4).Kinetic researches indicated the oxidation rate of MgSO_(3) was influenced by the catalyst dosage,the reaction temperature,the solution pH,the airflow rate,and the SO_(3)^(2-) concentration.Additionally,after recycling experiments,the regenerated catalyst retained its high catalytic performance for the MgSO_(3) oxidation.The reaction mechanism for the catalytic oxidation of MgSO_(3) by Co-Bent catalyst was also proposed.The generation of active free radicals(OH·,SO_(4)^(-)·,SO_(3)^(-)·,SO_(5)^(-)·)accelerated the MgSO_(3) oxidation.These results provide theoretical support for the treatment of MgSO_(3) and the development of durable catalyst.
基金supported by the National Natural Science Foundation of China(Nos.22208262,52271228,52202298,52201279,51834009,and 51801151)the Natural Science Foundation of Shaanxi Province(Nos.2021JQ-468,2020JZ-47)+3 种基金the Natural Science Foundation of Shaanxi Provincial Department of Education(No.21JP086)the Postdoctoral Research Foundation of China(Nos.2020M683528 and 2018M633643XB)the Young Talent Fund of Association for Science and Technology in Shaanxi,China(No.20230625)the Hundred Talent Program of Shaanxi Province.
文摘Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great challenge.In present work,a new strategy of chloride anion intercalation in Bi_(2)O_(3)via one-pot hydrothermal process is proposed.The as-prepared Ta-BiOCl/Bi_(24)O_(31)Cl_(10)(TBB)heterojunctions are featured with Ta-Bi_(24)O_(31)Cl_(10)and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces.In this TBB heterojunctions,the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer andmultiple transfer paths,respectively,leading to enhanced visible light response and improved photogenerated charge separation.Meanwhile,a type-II heterojunction for photocharge separation has been obtained,in which photogenerated electrons are drove from the CB(conduction band)of Ta-Bi_(24)O_(31)Cl_(10)to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl,while the photogenerated holes are left on the VB(valence band)of Ta-Bi_(24)O_(31)Cl_(10),effectively hindering the recombination of photogenerated electron-hole pairs.Furthermore,the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species(·O_(2)^(−)).Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride(TCH)solution to Bi_(2)O_(3),Ta-BiOCl and Ta-Bi_(24)O_(31)Cl_(10).This work not only proposes a Ta-BiOCl/Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-Ⅱheterojunction for highly efficient photocatalytic activity,but offers a new insight into the design of highly efficient heterojunction through phasestructure synergistic transformation strategy.
基金financially supported by National Natural Science Foundation of China(22208137 and 22068022)Yunnan Fundamental Research Projects(202101BE070001-033,202401AT070825,202201BE070001007 and 202301AV070005)。
文摘Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow-loading of Ru single atoms(0.42 wt%)into Mn_(2)O_(3)matrix(0.4%Ru-Mn_(2)O_(3))greatly boosts its catalytic activity for the aerobic oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA).The FDCA productivity over the 0.4%Ru-Mn_(2)O_(3)(5.4 mmol_(FDCA)g_(cat)h^(-1))is 4.9 times higher than the Mn_(2)O_(3).Especially,this FDCAproductivity is also significantly higher than that of existing Ru and Mn-based catalysts.Experimental and theoretical investigations discovered that the Ru single atom facilitated the formation of oxygen vacancy(O_(v))in the catalyst,which synergistically weakened the Mn-O bond and promoted the activation of O_L.The co-presence of Ru single atoms and O_(v)also promote the adsorption and activation of both O_(2)and HMF.Consequently,the dehydrogenation reaction energy barrier of the rate-determining step was reduced via both the O_L and chemisorbed O_(2)dehydrogenation pathways,thus boosting the catalytic oxidation reactions.
基金financially supported by the National Natural Science Foundation of China(22468034)the Natural Science Foundation of Inner Mongolia(2021MS02008 and 2022MS02011)the Key Research and Development Project of Ordos(YF20240062)。
文摘Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the underpinning mechanism remains elusive.Herein,the introduction of silanol nests enables the alloy formation on the SiO_(2)surface.The amination modification is disclosed to induce the electron transfer from RE to Pt and weaken the adsorption of CO on electron-rich Pt species.In situ/operando spectroscopic analyses in conjunction with density functional theory calculations demonstrate the electronic couple of Pt atoms and adjacent Ce atoms concurrently achieves the enhancement of CO oxidation and suppression of H_(2)oxidation.Additionally,CO_(2)is readily desorbed from the Pt_(5)Ce(111)surface to enhance intrinsic activity and longevity.These findings provide an atomic-level insight into the synergistic catalytic sites on regulating the electronic state of the Pt-RE alloy catalysts toward highly selective oxidation reactions.
基金Project supported by National Natural Science Foundation of China(22076180)Youth Innovation Promotion Association of CAS(2019376)Chongqing Bayu Scholar Program(Young Scholar,YS2020048)。
文摘Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by different amounts of cerium,which not only enhances the physicochemical stability but also increases the number of active sites of Ce_(x)Zr_(y)UiO-66.Furthermore,the catalysts with Co_(3)O_(4)nanoparticles supported on Ce_(x)Zr_(y)UiO-66 were successfully prepared via impregnation method.In the process of toluene degradation,the Co/Ce_(1)Zr_(2)-Ui0-66 attains a 90%conversion rate at 210℃with a space velocity of 60000 mL/(g·h)and toluene concentration at 1000×10^(-6).Meanwhile,the carbon dioxide selectivity reaches 100%at 218℃.The Co/Ce_(1)Zr_(2)-UiO-66 shows great water resistance(3 vol%H_(2)O).Multiple characterization methods were used to figure out the physicochemical properties of the catalysts.It is found that the addition of an appropriate amount of cerium can enhance stability of UiO-66 and surface lattice oxygen proportion.Additionally,the stronger electron transfer between Ce^(4+)and Co^(2+)enables the Co/Ce_(1)Zr_(2)-UiO-66 to possess more active surface oxygen species and Co_(3)+cationic species in all samples.
基金supported by Beijing Natural Science Foundation(No.8244060)China Postdoctoral Science Foundation(No.2023M730143)+3 种基金the National Natural Science Foundation of China(No.22425601)the National Key R&D Program of China(No.2023YFB3810801)Beijing Nova Program(No.20240484659)the R&D Program of Beijing Municipal Education Commission(No.KZ202210005011).
文摘Volatile organic compounds(VOCs)exhausted from industrial processes are the major atmospheric pollutants,which could destroy the ecological environment and make hazards to human health seriously.Catalytic oxidation is regarded as the most competitive strategy for the efficient elimination of low-concentration VOCs.Supported noble metal catalysts are preferred catalysts due to their excellent low-temperature catalytic activity.To further lower the cost of catalysts,single atom catalysts(SAC)have been fabricated and extensively studied for application in VOCs oxidation due to their 100%atom-utilization efficiency and unique catalytic performance.In this review,we comprehensively summarize the recent advances in supported noble metal(e.g.,Pt,Pd,Au,and Ag)catalysts and SAC for VOCs oxidation since 2015.Firstly,this paper focuses on some important influencing factors that affect the activity of supported noble metal catalysts,including particle size,valence state and dispersion of noble metals,properties of the support,metal oxide/ion modification,preparation method,and pretreatment conditions of catalysts.Secondly,we briefly summarize the catalytic performance of SAC for typical VOCs.Finally,we conclude the key influencing factors and provide the prospects and challenges of VOCs oxidation.
基金Financial support from the"Ministero dell’Istruzione dell’Università e della Ricerca"(MIUR)(CEMIF.CAL-CLAB01TYEF and CAMERE-RBNE03JCR5)is gratefully acknowledged.
文摘In this work the heterogenization in polymeric membranes of decatungstate,a photocatalyst for oxidation reactions,was reported.Solid state characterization techniques confirmed that the catalyst structure was preserved within the polymeric membranes.The catalytic membranes were successfully applied in the aerobic photo-oxidation of phenol,one of the main organic pollutants in wastewater,providing stable and recyclable photocatalytic systems.The dependence of the phenol degradation rate by the catalyst loading and transmembrane pressure was shown.By comparison with homogeneous reaction,the catalyst heterogenized in membrane appears to be more efficient concerning the rate of phenol photodegradation and mineralization.
基金supported by the National Natural Science Foundation of China(21325731,51478241,21221004)~~
文摘Formaldehyde(HCHO)is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.
基金supported by the National Natural Science Foundation of China(21325731,21221004 and 51478241)~~
文摘Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.
基金supported by Natural Science Foundation of Shandong Province(ZR2022MB049)National Natural Science Foundation of China(22078174)。
文摘Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light.The Er@K-C_(3)N_(4)/UiO-66-NH_(2) catalyst was synthesized using a straight-forward hydrothermal technique,and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid.The catalyst was thoroughly characterized,confirming the effective adjustment of the band gap energy of Er@K-C_(3)N_(4)/UiO-66-NH_(2).Upon the optimized reaction conditions,the conversion rate of furfural reached 89.3%,with a corresponding yield of furoic acid at 79.8%.The primary reactive oxygen species was identified as·O_(2)^(-) from ESR spectra and scavenger tests.The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate,hence increasing the separating efficiency of photogenerated electron-hole pairs.This study expands the potential applications of rare earth element doped g-C_(3)N_(4) in the photocatalytic selective oxidation of furfurans.
文摘Because phenolic compounds are toxic for methanogenic bacteria many problems concerning the high toxicity and biodegradability of the olive oil mill wastewater (OMW) have been encountered during anaerobic treatments of this effluent. In this work, we try to develop a new catalytic process for the degradation of phenolic compounds, producing less toxic OMW for methanogenic bacteria, facilitating the anaerobic digestion. This process consists of an oxidative reaction using copper supported on alumina pillared clay in presence of a photocatalytic system (H2O2 with UV light). Preliminary results showed that the use of the copper supported catalyst in presence of 0.88% H2O2 (v/v) allows after 2 h colour reduction (25%), significant abatement of total organic carbon (40%), and important removal of polyphenolic compounds (63%) especially those of high molecular mass and subsequently decreases the OMW toxicity from 100% to 70%. This catalytic pre-treatment process of OMW was efficient for anaerobic digestion.
基金supported by the National Key Research and Development Program Foundation of China(2016YFC0209203)the National Natural Science Foundation of China(21707130,21325731)~~
文摘KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.
文摘The MoOx/AuNPs composite film modified glassy carbon electrode was fabricated by electro-depositing simultaneously gold nanoparticles and molybdenum oxides using cyclic voltammetry. The morphology and topography of the MoOx/AuNPs composite were char-acterized by scan electron microscopy and X-ray photoelectron spectroscopy respectively, and the electrocatalytic oxidation of glucose at the MoOx/AuNPs composite film was inves-tigated and analyzed in detail. It was shown that the MoOx/AuNPs composite was of strong electrocatalytic activity towards oxidation of glucose as well as other saccharides, so that an attempt was made for direct voltammetric determination of glucose. Then the positive scan polarization reverse catalytic voltammetry was proposed for the first time. Based on this method, the pure oxidation current was extracted by subtraction of the blank current in the reverse scan. The current sensitivity was enhanced tremendously and the signal to noise ra-tio was improved adequately. The electrocatalytic oxidation of glucose at the MoOx/AuNPs modified electrode was performed in alkaline medium, a wide linear range from 0.01 mmol/L to 4.0 mmol/L of glucose, a higher current sensitivity of 2.35 mA/(mmol/L·cm2), and a lower limit of detection of 9.01 μmol/L (at signal/noise=3) were achieved. In addition, the electrocatalytic oxidation of other saccharides such as lactose, fructose and sucrose was also evaluated.
文摘Mesoporous TiO2 ceramic films have been prepared upon the Ti alloy substrate by the micro-arc oxidation (MAO) technology. To enhance the photo-catalytic property of the films, Eu2O3 particles were added into the electrolyte solution of Na2CO3/Na2SiO3. Scanning electron microscope (SEM), energy dispersive (EDS), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) are employed to characterize the modified films. Diffuse reflectance spectra (DRS) test, photo-generated current test and photo decomposition test are applied to evaluate the photo-catalytic property of the modified films. The results show that Eu2O3 transformed into one-dimensional (1-D) nano-wires embedded within the composite film, and the film has high photo-catalytic property.
基金supported by the National Natural Science Foundation of China (51374004,51204083)the Candidate Talents Training Fund of Yun-nan Province (2012HB009,2014HB006)+2 种基金the Applied Basic Research Program of Yunnan Province (2014FB123)a School-Enterprise Cooperation Project from Jinchuan Corporation (Jinchuan 201115)the Talents Training Program of Kunming University of Science and Technology (KKZ3201352038)~~
文摘This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hydroxide-carbonate nanoparticles with various morphologies(i.e.,nanorods,nanosheets,and nanocubes) were successfully synthesized,and Co3O4 nanoparticles were obtained by thermal decomposition of the cobalt-hydroxide-carbonate precursors.The results suggest that the cobalt source is a key factor for controlling the morphology of cobalt-hydroxide-carbonate at relatively low hydrothermal temperatures(≤ 140℃).Nanorods can be synthesized in CoCl2 solution,while Co(NO3)2 solution promotes the formation of nanosheets.Further increasing the synthesis temperature(higher than 140 ℃) results in the formation of nanocubes in either Co(NO3)2 or CoCl2 solution.The reaction time only affects the size of the obtained nanoparticles.The presence of CTAB could improve the uniformity and dispersion of particles.Co3O4 nanosheets showed much higher catalytic activity for CO oxidation than nanorods and nanocubes because it has more abundant Co^(3+) on the surface,much higher reducibility,and better oxygen desorption capacity.