Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short life...Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short lifetime of reactive oxygen species(ROS)and uncontrollable oxidation pathways.Herein,we show that single-atom Co supported on carbon nitride enables the high-valent-oxo cobalt species(Co(IV)O)mediated oxidation of glucose into value-added products in acetonitrile.This photocatalytic Fenton-like system achieved an overall selectivity of gluconic acid,glucaric acid,arabinose,and formic acid up to 90.3%at glucose conversion of 69.6%,outperforming most of previously reported catalytic systems.The small amount(0.72 wt%)of single-atom Co could not only elevate the optical absorption and the efficiency of photo-generated carriers separation but also induce the efficient generation of Co(IV)O with reduced ROS to enable efficient and selective oxidation.These findings prove the great promise of high-valent metal-oxo species in biomass conversions.展开更多
Oxide dispersion strengthened(ODS)alloys are extensively used owing to high thermostability and creep strength contributed from uniformly dispersed fine oxides particles.However,the existence of these strengthening pa...Oxide dispersion strengthened(ODS)alloys are extensively used owing to high thermostability and creep strength contributed from uniformly dispersed fine oxides particles.However,the existence of these strengthening particles also deteriorates the processability and it is of great importance to establish accurate processing maps to guide the thermomechanical processes to enhance the formability.In this study,we performed particle swarm optimization-based back propagation artificial neural network model to predict the high temperature flow behavior of 0.25wt%Al2O3 particle-reinforced Cu alloys,and compared the accuracy with that of derived by Arrhenius-type constitutive model and back propagation artificial neural network model.To train these models,we obtained the raw data by fabricating ODS Cu alloys using the internal oxidation and reduction method,and conducting systematic hot compression tests between 400 and800℃with strain rates of 10^(-2)-10 S^(-1).At last,processing maps for ODS Cu alloys were proposed by combining processing parameters,mechanical behavior,microstructure characterization,and the modeling results achieved a coefficient of determination higher than>99%.展开更多
Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerg...Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals(HO˙),leading to excessive consumption of H_(2)O_(2).Through interfacial engineering of Fe-Zr bimetallic catalysts(FeZrO_(x)),this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80%reduction in H_(2)O_(2)dosage compared to traditional Fe_(2)O_(3)systems.The chemical states of Fe and Zr at the(104)/(111)heterojunction interface in FeZrO_(x)exhibit marked modifications relative to their monometallic Fe_(2)O_(3)and ZrO_(2)counterparts.The elevated charge density at interfacial Fe sites in FeZrO_(x)promotes HO˙generation,while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization.This Fe-Zr synergy at the(104)/(111)heterojunction concurrently suppresses HO˙diffusion losses and directs phenolic pollutant(e.g.,phenol and bisphenol A)polymerization within the reactive interface,thereby reducing H_(2)O_(2)consumption compared to monometallic systems.展开更多
Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the el...Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.展开更多
In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrol...In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrolyte composed of ionic liquids(ILs),NaCl,and H_(2)SO_(4),integrating extraction and electrochemical oxidation to effectively remove different aromatic sulfur compounds with sulfur removals of 100%.Additionally,H_(2)is co-produced at the cathode,supporting refinery processes and reducing H_(2)storage and transportation costs,thereby improving economic viability.Detailed mechanism analysis shows that IL selectively extracts and concentrates sulfur compounds,while NaCl and H2SO4 facilitate ClO^(-)generation,serving as the in-situ oxidant.The EC-EODS system operates without external catalysts,relying on graphite electrodes that generate superoxide radicals from ClO^(-).Moreover,a strategy for the separation of desulfurization products as well as the electrolyte is proposed as well.The EC-EODS system offers a sustainable,high-efficiency strategy for desulfurization,with economic benefits through sulfur oxidation and H_(2)co-generation.展开更多
Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mec...Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.展开更多
Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that ...Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that are readily available,cost-effective,and exhibit minimal ecological toxicity.These LVSOs have the ability to generate or promote the generation of strong oxidants or reductants,which makes them widely used in advanced oxidation processes(AOPs)and advanced reduction processes(ARPs).This article provides a comprehensive review of the recent advancements in AOPs and ARPs involving LVSOs,alongside an examination of the fundamental principles governing the generation of active species within these processes.LVSOs fulfill three primary functions in AOPs:Serving as sources of reactive oxygen species(ROS),auxiliary agents,and activators.Particular attention is devoted to elucidating the reaction mechanisms through which LVSOs,in conjunction with metal ions,metal oxides,ultraviolet light(UV),and ozone,produce potent oxidizing agents in both homogeneous and heterogeneous systems.Regarding ARPs,this review delineates the mechanisms by which LVSOs generate strong reducing agents,including hydrated electrons,hydrogen radicals,and sulfite radicals,under UV irradiation,while also exploring the interactions between these reductants and pollutants.The review identifies existing gaps within the current framework and proposes future research avenues to address these challenges.展开更多
Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials...Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials(EFMs),particularly high-end oxidation systems using eco-friendly nanomaterials,show promise for absorbing and degrading ECs.This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological,physical,and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification.Through meticulous comparison,we unequivocally advocate for the imperative integration of environmentally benign nanomaterials,notably titanium-based variants,in forthcoming methodologies.Our in-depth exploration scrutinizes the catalytic efficacy,underlying mechanisms,and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts.Additionally,strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.展开更多
The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,...The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,UV/H_(2)O_(2),UV/Fenton,UV/persulfate,UV/chlorine,UV/ozone,and UV/peracetic acid.In this review,we collated recent advances in application of UV-AOPs for the abatement of fiuoroquinolones(FQs)as widely used class of antibiotics.Representative FQs of ciprofioxacin,norfioxacin,ofioxacin,and enrofioxacin were most extensively studied in the state-of-art studies.The evolvement of gas-state and solid-state UV light sources was presented and batch and continuous fiow UV reactors were compared towards practical applications in UV-AOPs.Generally,degradation of FQs followed the pseudo-first order kinetics in UV-AOPs and strongly affected by the operating factors and components of water matrix.Participation of reactive species and transformation mechanisms of FQs were compared among different UV-AOPs.Challenges and future prospects were pointed out for providing insights into the practical application of UV-AOPs for antibiotic remediation in wastewater.展开更多
Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radica...Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.展开更多
The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity ...The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity improvement and better mechanistic understanding of the state-of-the-art Ni(OH)_(2) catalyst.Herein,by utilizing low-temperature argon(Ar)plasma processing,tooth-wheel Ni(OH)_(2) nanosheets self-supported on Ni foam(Ni(OH)_(2)-Ar)are demonstrated to have improved UOR activity compared to conventional Ni(OH)_(2).The theoretical assessment confirms that the edge has a smaller cation vacancy formation energy than the basal plane,consequently explaining the structural formation.Operando and quasi-operando methods are employed to investigate the dynamic evolution of the Ni(OH)_(2) film in UOR.The crucial dehydrogenation products of Ni(OH)_(5)O^(-)intermediates are identified to be stable on the etched edge and explain the enhanced UOR in the low potential region.In addition,the dynamic active sites are monitored to elucidate the reaction mechanism in different potential ranges.展开更多
Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is i...Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is in a range of 200-500 nm with many porous.The B-α-Ni(OH)2nanoflowers were developed as electrocatalysts for urea electro-oxidation in alkaline media with more than 10 times enhancement in current density compared to bulk nickel hydroxide powders.Results demonstrated that the obtained B-α-Ni(OH)2electrode exhibited high activity and good stability.The positive correlation between the scan rates and the anodic currents implied a single diffusion-controlled kinetic process.The enhanced electro-catalytic oxidation of urea using B-α-Ni(OH)2 nanoflowers has promising applications in urea-rich wastewater remediation,hydrogen production,and fuel cells.展开更多
Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatmen...Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatment of such wastewater. Moreover, since such wastewater is also not suitable for the growth of microorganisms, the way of wastewater treatment by microorganisms is also greatly limited. For this kind of industrial waste water, apart from the degradation of organic matters, the separation of inorganic salts and waste water is also required to meet the sewage discharge standard. Based on this, the article focuses on the coal chemical high salt wastewater electro-catalytic oxidation pilot study.展开更多
The influence of the certain specific vacuum pre-oxidation process on the phase transformation of thermally-grown oxides（TGO） was studied.The CoCrAlY high temperature corrosion resistance coatings were produced onto...The influence of the certain specific vacuum pre-oxidation process on the phase transformation of thermally-grown oxides（TGO） was studied.The CoCrAlY high temperature corrosion resistance coatings were produced onto the nickel-based superalloy substrate by high velocity oxygen fuel（HVOF）.It suggests that the TGO usually consists of a great number of chromium oxides,cobalt oxides and spinel oxides besides alumina during the initial period of the high temperature oxidation if the specimens are not subjected to the appropriate vacuum pre-oxidation process.Furthermore,the amount of alumina is strongly dependent on the partial pressure of oxygen;while the CoCr2O4 spinel oxides are usually formed under the conditions of higher partial pressure of oxygen during the initial period and the lower partial pressure of oxygen during the subsequent period of the isothermal oxidation.After the appropriate vacuum pre-oxidation process,the TGO is mainly composed of alumina that contains lower Y element,while alumina that contains higher Y element sporadically distributes,and the spinel oxides cannot be found.After a longer period of the isothermal oxidation,a small amount of porous CoCr2O4 and the chrome oxide sporadically distribute near the continuous alumina.Additionally,after the appropriate vacuum pre-oxidation process,the TGO growth rate is relatively slow.展开更多
In the range of 620？710 °C, air was blown into A356 aluminum alloy melt to produce aluminum foams. In order to study the influence of temperature on the thickness of oxide film on bubble surface, Auger electron ...In the range of 620？710 °C, air was blown into A356 aluminum alloy melt to produce aluminum foams. In order to study the influence of temperature on the thickness of oxide film on bubble surface, Auger electron spectroscopy （AES） was used. Based on the knowledge of corrosion science and hydrodynamics, two oxidation kinetics models of oxide film on bubble surface were established. The thicknesses of oxide films produced at different temperatures were predicted through those two models. Furthermore, the theoretical values were compared with the experimental values. The results indicate that in the range of 620？710 °C, the theoretical values of the thickness of oxide film predicted by the model including the rising process are higher than the experimental values. While, the theoretical values predicted by the model without the rising process are in good agreement with the experimental values, which shows this model objectively describes the oxidation process of oxide film on bubble surface. This work suggests that the oxidation kinetics of oxide film on bubble surface of aluminum foams produced by gas injection foaming process follows the Arrhenius equation.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
The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different o...The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.展开更多
The short-and long-term effects of chlortetracycline（CTC） on the nitritation-anaerobic ammonium oxidation（anammox） process were evaluated. The half maximal inhibitory concentration of CTC in the batch tests of the...The short-and long-term effects of chlortetracycline（CTC） on the nitritation-anaerobic ammonium oxidation（anammox） process were evaluated. The half maximal inhibitory concentration of CTC in the batch tests of the nitritation-anammox process was 278.91 mg/L at an exposure time of 12 hr. The long-term effects of CTC on the process were examined in a continuous-flow nitritation-anammox reactor. Within 14 days, the nitrogen removal rate significantly decreased from 0.61 to 0.25 kg N/m^3/day with 60 mg/L CTC in the influent.The performance suppressed by CTC barely recovered, even after CTC was removed from the influent. Furthermore, the inhibition of CTC also reduced the relative abundance of ammonium oxidizing bacteria（AOB） and anaerobic ammonium oxidizing bacteria（An AOB）in the reactor, resulting in both a decreased amount of and an imbalance between AOB and An AOB. When fresh anammox sludge was reseeded into the nitritation-anammox reactor,the nitrogen removal rate recovered to 0.09 ± 0.03 kg N/m3/day.展开更多
In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond...In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond(BDD) film electrodes using Ta as substrates were employed for AO of SA.In the case of FP and UV/H_2O_2,most favorable experimental conditions were determined for each process and these were used for comparing with AO process.The study showed that the FP was the most effective process under aci...展开更多
In recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of was...In recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater,such as wastewater containing antibiotics,pharmaceuticals and personal care products,dyes,endocrine-disrupting chemicals,chlorinated organic pollutants,and phenolics,for the degradation of refractory organic contaminants.This paper summarizes the production of sulfate radicals,which can be generated by the activation of persulfate via conventional and emerging approaches.The existing problems of persulfate-based advanced oxidation processes were analyzed in detail,including residual sulfates,coexisting factors(coexisting inorganic anions and natural organic matter),and energy consumption.This paper proposes corresponding possible solutions to the problems mentioned above,and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.展开更多
基金supported by the National Natural Science Foundation of China(22478202,22208169,U23A20125,22478203)China Postdoctoral Science Foundation(2022M721703).
文摘Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short lifetime of reactive oxygen species(ROS)and uncontrollable oxidation pathways.Herein,we show that single-atom Co supported on carbon nitride enables the high-valent-oxo cobalt species(Co(IV)O)mediated oxidation of glucose into value-added products in acetonitrile.This photocatalytic Fenton-like system achieved an overall selectivity of gluconic acid,glucaric acid,arabinose,and formic acid up to 90.3%at glucose conversion of 69.6%,outperforming most of previously reported catalytic systems.The small amount(0.72 wt%)of single-atom Co could not only elevate the optical absorption and the efficiency of photo-generated carriers separation but also induce the efficient generation of Co(IV)O with reduced ROS to enable efficient and selective oxidation.These findings prove the great promise of high-valent metal-oxo species in biomass conversions.
基金financial support of the National Natural Science Foundation of China(No.52371103)the Fundamental Research Funds for the Central Universities,China(No.2242023K40028)+1 种基金the Open Research Fund of Jiangsu Key Laboratory for Advanced Metallic Materials,China(No.AMM2023B01).financial support of the Research Fund of Shihezi Key Laboratory of AluminumBased Advanced Materials,China(No.2023PT02)financial support of Guangdong Province Science and Technology Major Project,China(No.2021B0301030005)。
文摘Oxide dispersion strengthened(ODS)alloys are extensively used owing to high thermostability and creep strength contributed from uniformly dispersed fine oxides particles.However,the existence of these strengthening particles also deteriorates the processability and it is of great importance to establish accurate processing maps to guide the thermomechanical processes to enhance the formability.In this study,we performed particle swarm optimization-based back propagation artificial neural network model to predict the high temperature flow behavior of 0.25wt%Al2O3 particle-reinforced Cu alloys,and compared the accuracy with that of derived by Arrhenius-type constitutive model and back propagation artificial neural network model.To train these models,we obtained the raw data by fabricating ODS Cu alloys using the internal oxidation and reduction method,and conducting systematic hot compression tests between 400 and800℃with strain rates of 10^(-2)-10 S^(-1).At last,processing maps for ODS Cu alloys were proposed by combining processing parameters,mechanical behavior,microstructure characterization,and the modeling results achieved a coefficient of determination higher than>99%.
基金supported by the National Natural Science Foundation of China(Grant Nos.22476187 and 22206173)the Natural Science Foundation of Henan Province(Grant No.252300421179)+1 种基金the Foundation of Henan Educational Committee(Grant No.25A610001)the Science and Technology Innovation Leading Talent Support Program of Henan Province(Grant No.254000510035).
文摘Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals(HO˙),leading to excessive consumption of H_(2)O_(2).Through interfacial engineering of Fe-Zr bimetallic catalysts(FeZrO_(x)),this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80%reduction in H_(2)O_(2)dosage compared to traditional Fe_(2)O_(3)systems.The chemical states of Fe and Zr at the(104)/(111)heterojunction interface in FeZrO_(x)exhibit marked modifications relative to their monometallic Fe_(2)O_(3)and ZrO_(2)counterparts.The elevated charge density at interfacial Fe sites in FeZrO_(x)promotes HO˙generation,while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization.This Fe-Zr synergy at the(104)/(111)heterojunction concurrently suppresses HO˙diffusion losses and directs phenolic pollutant(e.g.,phenol and bisphenol A)polymerization within the reactive interface,thereby reducing H_(2)O_(2)consumption compared to monometallic systems.
基金supported by the National Key Research and Development Program of China(2022YFC3205300)the National Natural Science Foundation of China(22176124).
文摘Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.
基金financial support from the National Key R&D Program of China(No.2022YFA1504404,2022YFA1504403)National Science Foundation for Distinguished Young Scholars(No.22425808)+2 种基金National Natural Science Foundation of China(No.22178154)China Postdoctoral Science Foundation(No.2024M753617)Natural Science Foundation of Jiangsu Province(No.BK20230068).
文摘In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrolyte composed of ionic liquids(ILs),NaCl,and H_(2)SO_(4),integrating extraction and electrochemical oxidation to effectively remove different aromatic sulfur compounds with sulfur removals of 100%.Additionally,H_(2)is co-produced at the cathode,supporting refinery processes and reducing H_(2)storage and transportation costs,thereby improving economic viability.Detailed mechanism analysis shows that IL selectively extracts and concentrates sulfur compounds,while NaCl and H2SO4 facilitate ClO^(-)generation,serving as the in-situ oxidant.The EC-EODS system operates without external catalysts,relying on graphite electrodes that generate superoxide radicals from ClO^(-).Moreover,a strategy for the separation of desulfurization products as well as the electrolyte is proposed as well.The EC-EODS system offers a sustainable,high-efficiency strategy for desulfurization,with economic benefits through sulfur oxidation and H_(2)co-generation.
基金Project(52274348)supported by the National Natural Science Foundation of ChinaProject(2022JH1/10400024)supported by the Major Projects for the“Revealed Top”Science and Technology of Liaoning Province,China。
文摘Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.
基金supported by Natural Science Foundation of China(Nos.52070133,42107073,42477075)Natural Science Foundation of Sichuan Province(No.2024NSFSC0130)+2 种基金the Sichuan Science and Technology Program(No.2024NSFTD0014)Key Laboratory of Jiangxi Province for Persistent Pollutants Prevention Control and Resource Reuse(No.2023SSY02061)Key R&D Program of Heilongjiang Province(No.2023ZX02C01)。
文摘Low-valent sulfur oxy-acid salts(LVSOs)represent a category of oxygen-containing salts characterized by their potent reducing capabilities.Notably,sulfite,dithionite,and thiosulfate are prevalent reducing agents that are readily available,cost-effective,and exhibit minimal ecological toxicity.These LVSOs have the ability to generate or promote the generation of strong oxidants or reductants,which makes them widely used in advanced oxidation processes(AOPs)and advanced reduction processes(ARPs).This article provides a comprehensive review of the recent advancements in AOPs and ARPs involving LVSOs,alongside an examination of the fundamental principles governing the generation of active species within these processes.LVSOs fulfill three primary functions in AOPs:Serving as sources of reactive oxygen species(ROS),auxiliary agents,and activators.Particular attention is devoted to elucidating the reaction mechanisms through which LVSOs,in conjunction with metal ions,metal oxides,ultraviolet light(UV),and ozone,produce potent oxidizing agents in both homogeneous and heterogeneous systems.Regarding ARPs,this review delineates the mechanisms by which LVSOs generate strong reducing agents,including hydrated electrons,hydrogen radicals,and sulfite radicals,under UV irradiation,while also exploring the interactions between these reductants and pollutants.The review identifies existing gaps within the current framework and proposes future research avenues to address these challenges.
基金supported by the Research Platform Open Fund Project of Zhejiang Industry and Trade Vocation College(No.Kf202203)the Scientific Research Project of CCCC First Harbor Engineering Company Ltd.(No.2022-7-2)+3 种基金the National Natural Science Foundation of China(No.22406142)the Fellowship of China National Postdoctoral Program for Innovative Talents(No.BX20230262)the Fellowship of China Postdoctoral Science Foundation(No.2023M732636)the Shanghai Post-doctoral Excellence Program(No.2023755).
文摘Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants(ECs)from water,surpassing the limitations of traditional methods.Environmental functional materials(EFMs),particularly high-end oxidation systems using eco-friendly nanomaterials,show promise for absorbing and degrading ECs.This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological,physical,and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification.Through meticulous comparison,we unequivocally advocate for the imperative integration of environmentally benign nanomaterials,notably titanium-based variants,in forthcoming methodologies.Our in-depth exploration scrutinizes the catalytic efficacy,underlying mechanisms,and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts.Additionally,strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.
基金the financial support from National Natural Science Foundation of China(Nos.52100204 and 52330005)Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910004016)。
文摘The widespread occurrence of antibiotics in wastewater aroused serious attention.UV-based advanced oxidation processes(UV-AOPs)are powerful technologies in removing antibiotics in wastewater,which include UV/catalyst,UV/H_(2)O_(2),UV/Fenton,UV/persulfate,UV/chlorine,UV/ozone,and UV/peracetic acid.In this review,we collated recent advances in application of UV-AOPs for the abatement of fiuoroquinolones(FQs)as widely used class of antibiotics.Representative FQs of ciprofioxacin,norfioxacin,ofioxacin,and enrofioxacin were most extensively studied in the state-of-art studies.The evolvement of gas-state and solid-state UV light sources was presented and batch and continuous fiow UV reactors were compared towards practical applications in UV-AOPs.Generally,degradation of FQs followed the pseudo-first order kinetics in UV-AOPs and strongly affected by the operating factors and components of water matrix.Participation of reactive species and transformation mechanisms of FQs were compared among different UV-AOPs.Challenges and future prospects were pointed out for providing insights into the practical application of UV-AOPs for antibiotic remediation in wastewater.
基金supported by the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2024LHMS05048).
文摘Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.
基金the financial support from City University of Hong Kong Strategic Research Grant(SRG)(7005505)the National Natural Science Foundation of China(51601136 and 51604202)。
文摘The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity improvement and better mechanistic understanding of the state-of-the-art Ni(OH)_(2) catalyst.Herein,by utilizing low-temperature argon(Ar)plasma processing,tooth-wheel Ni(OH)_(2) nanosheets self-supported on Ni foam(Ni(OH)_(2)-Ar)are demonstrated to have improved UOR activity compared to conventional Ni(OH)_(2).The theoretical assessment confirms that the edge has a smaller cation vacancy formation energy than the basal plane,consequently explaining the structural formation.Operando and quasi-operando methods are employed to investigate the dynamic evolution of the Ni(OH)_(2) film in UOR.The crucial dehydrogenation products of Ni(OH)_(5)O^(-)intermediates are identified to be stable on the etched edge and explain the enhanced UOR in the low potential region.In addition,the dynamic active sites are monitored to elucidate the reaction mechanism in different potential ranges.
基金Supported by the National Natural Science Foundation of China(21403053,U1404503)
文摘Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is in a range of 200-500 nm with many porous.The B-α-Ni(OH)2nanoflowers were developed as electrocatalysts for urea electro-oxidation in alkaline media with more than 10 times enhancement in current density compared to bulk nickel hydroxide powders.Results demonstrated that the obtained B-α-Ni(OH)2electrode exhibited high activity and good stability.The positive correlation between the scan rates and the anodic currents implied a single diffusion-controlled kinetic process.The enhanced electro-catalytic oxidation of urea using B-α-Ni(OH)2 nanoflowers has promising applications in urea-rich wastewater remediation,hydrogen production,and fuel cells.
文摘Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatment of such wastewater. Moreover, since such wastewater is also not suitable for the growth of microorganisms, the way of wastewater treatment by microorganisms is also greatly limited. For this kind of industrial waste water, apart from the degradation of organic matters, the separation of inorganic salts and waste water is also required to meet the sewage discharge standard. Based on this, the article focuses on the coal chemical high salt wastewater electro-catalytic oxidation pilot study.
基金Project supported the by State Key Laboratory of Internal Combustion Engines of Tianjin University,ChinaProject(51507077)supported by the National Natural Science Foundation of China+1 种基金Project(15KJB470005)supported by the Natural Science Research of Higher Education Institutions of Jiangsu Province,ChinaProjects(YKJ201308,QKJB201401)supported by Nanjing Institute of Technology,China
文摘The influence of the certain specific vacuum pre-oxidation process on the phase transformation of thermally-grown oxides（TGO） was studied.The CoCrAlY high temperature corrosion resistance coatings were produced onto the nickel-based superalloy substrate by high velocity oxygen fuel（HVOF）.It suggests that the TGO usually consists of a great number of chromium oxides,cobalt oxides and spinel oxides besides alumina during the initial period of the high temperature oxidation if the specimens are not subjected to the appropriate vacuum pre-oxidation process.Furthermore,the amount of alumina is strongly dependent on the partial pressure of oxygen;while the CoCr2O4 spinel oxides are usually formed under the conditions of higher partial pressure of oxygen during the initial period and the lower partial pressure of oxygen during the subsequent period of the isothermal oxidation.After the appropriate vacuum pre-oxidation process,the TGO is mainly composed of alumina that contains lower Y element,while alumina that contains higher Y element sporadically distributes,and the spinel oxides cannot be found.After a longer period of the isothermal oxidation,a small amount of porous CoCr2O4 and the chrome oxide sporadically distribute near the continuous alumina.Additionally,after the appropriate vacuum pre-oxidation process,the TGO growth rate is relatively slow.
基金Project(51371104)supported by the National Nature Science Foundation of China
文摘In the range of 620？710 °C, air was blown into A356 aluminum alloy melt to produce aluminum foams. In order to study the influence of temperature on the thickness of oxide film on bubble surface, Auger electron spectroscopy （AES） was used. Based on the knowledge of corrosion science and hydrodynamics, two oxidation kinetics models of oxide film on bubble surface were established. The thicknesses of oxide films produced at different temperatures were predicted through those two models. Furthermore, the theoretical values were compared with the experimental values. The results indicate that in the range of 620？710 °C, the theoretical values of the thickness of oxide film predicted by the model including the rising process are higher than the experimental values. While, the theoretical values predicted by the model without the rising process are in good agreement with the experimental values, which shows this model objectively describes the oxidation process of oxide film on bubble surface. This work suggests that the oxidation kinetics of oxide film on bubble surface of aluminum foams produced by gas injection foaming process follows the Arrhenius equation.
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.
基金the financial support from the National Natural Science Foundation of China(No. 51878423)Graduate Student’s Research and Innovation Fund of Sichuan University(No.2018YJSY075)
文摘The electrochemical advanced oxidation processes(EAOPs) have been extensively applied in the treatment of organic pollutants degradation.Herein,the mini review provides the coupling systems about EAOPs and different oxidants(e.g.,persulfate(PS),peroxymonosulfate(PMS),and ozone(O3)),including EAOPs-PS systems,EAOPs-PMS systems,EAOPs-peroxone systems,and photoelectro-oxidants systems,for the organic compounds degradation.The coupling system of EAOPs with oxidants is an effective way to improve the generated free radicals(e.g.,HO^·and SO4^·-) concentration and to accelerate pollutant degradation.In this review,we make a summary of the homogeneous and heterogeneous EAOPs-oxidant processes.The reaction mechanisms of EAOPs combined with different oxidants are elucidated in detail,as well as the synergistic effect for improving the degradation and mineralization efficiency.
基金supported by the National Natural Science Foundation of China (No. 51578043)the Basic research funds (No. C16JB00480)
文摘The short-and long-term effects of chlortetracycline（CTC） on the nitritation-anaerobic ammonium oxidation（anammox） process were evaluated. The half maximal inhibitory concentration of CTC in the batch tests of the nitritation-anammox process was 278.91 mg/L at an exposure time of 12 hr. The long-term effects of CTC on the process were examined in a continuous-flow nitritation-anammox reactor. Within 14 days, the nitrogen removal rate significantly decreased from 0.61 to 0.25 kg N/m^3/day with 60 mg/L CTC in the influent.The performance suppressed by CTC barely recovered, even after CTC was removed from the influent. Furthermore, the inhibition of CTC also reduced the relative abundance of ammonium oxidizing bacteria（AOB） and anaerobic ammonium oxidizing bacteria（An AOB）in the reactor, resulting in both a decreased amount of and an imbalance between AOB and An AOB. When fresh anammox sludge was reseeded into the nitritation-anammox reactor,the nitrogen removal rate recovered to 0.09 ± 0.03 kg N/m3/day.
文摘In this study,advanced oxidation processes(AOPs) such as anodic oxidation(AO),UV/H_2O_2 and Fenton processes(FP) were investigated for the degradation of salicylic acid(SA) in lab-scale experiments.Boron-doped diamond(BDD) film electrodes using Ta as substrates were employed for AO of SA.In the case of FP and UV/H_2O_2,most favorable experimental conditions were determined for each process and these were used for comparing with AO process.The study showed that the FP was the most effective process under aci...
基金the National Natural Science Foundation of China(No.51678185)Talents of High Level Scientific Research Foundation of Qingdao Agricultural University(No.6651120004).
文摘In recent years,with the emergence of new pollutants,the effective treatment of wastewater has become very important.Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater,such as wastewater containing antibiotics,pharmaceuticals and personal care products,dyes,endocrine-disrupting chemicals,chlorinated organic pollutants,and phenolics,for the degradation of refractory organic contaminants.This paper summarizes the production of sulfate radicals,which can be generated by the activation of persulfate via conventional and emerging approaches.The existing problems of persulfate-based advanced oxidation processes were analyzed in detail,including residual sulfates,coexisting factors(coexisting inorganic anions and natural organic matter),and energy consumption.This paper proposes corresponding possible solutions to the problems mentioned above,and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.
