Antibiotic-contaminated wastewater poses a global threat to aquatic ecosystems.Fenton-like oxidative processes effectively decompose recalcitrant pollutants.While these oxidative processes effectively break down targe...Antibiotic-contaminated wastewater poses a global threat to aquatic ecosystems.Fenton-like oxidative processes effectively decompose recalcitrant pollutants.While these oxidative processes effectively break down target contaminants,they may also produce uncontrolled intermediates,potentially resulting in unexpected combined toxicities.This review explores the chemical mechanisms behind Fenton-like reactions,particularly in antibiotic removal,and evaluates the formation of byproducts and their potential toxicological effects.Furthermore,recommendations for optimizing catalyst design and treatment conditions are provided to enhance degradation performance while minimizing ecological risks.This study highlights critical concerns regarding the toxicity of degradation byproducts and their impact on ecosystems by integrating chemical and biological risk assessments.By integrating chemical and biological risk assessments with computational toxicology,particularly quantitative structure-activity relationship(QSAR)modeling,this study proposes a comprehensive approach to evaluate degradation and toxicity.This work highlights the importance of a comprehensive framework for evaluating degradation efficiency and toxicity,contributing to safer and more effective antibiotic wastewater treatment strategies.The findings underscore the importance of balancing degradation efficiency with environmental safety in wastewater treatment processes involving advanced oxidative technologies.展开更多
In this study, Fe3O4nanoparticles（Fe3O4NPs） were successfully prepared via oxidation–precipitation method and characterized by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and Fourier transform inf...In this study, Fe3O4nanoparticles（Fe3O4NPs） were successfully prepared via oxidation–precipitation method and characterized by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and Fourier transform infrared spectroscopy（FT-IR）. The characterization results indicated that Fe3O4 NPs with regular crystal structure and a narrow of diameters had been synthesized successfully and had high purity. A series of experiments were carried out to investigate the degradation of Orange II by the obtained heterogeneous Fe3O4 catalysts in the presence of H2O2. The response surface methodology（RSM） based on Box–Behnken design（BBD） was employed to design and optimize individual and interactive effects of the four main independent parameters（catalyst loading, initial p H, reaction temperature and H2O2concentration） on decolorization efficiency of Orange II. A significant quadratic model（p-value 〈0.0001, R2= 0.9369） was derived using analysis of variance（ANOVA）. Optimum conditions were catalyst loading of 1.5 g/L, initial p H of 2.7, reaction temperature of 42 8C and H2O2 concentration of 22 mmol/L, respectively. The predicted decolorization rate under the optimum conditions as determined by the proposed model was 99.55%. Confirmatory tests were carried out and the decolorization rate of 99.49% was observed under the optimum conditions, which agreed well with the model prediction.展开更多
Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesiz...Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD).The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions,accompanied by low H_(2)O_(2)consumption.The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species,which play a significant role in the high-performance Fenton-like reaction.The pollutants that served as electron donors were decomposed in the electron-poor carbon centers,whereas H_(2)O_(2)and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds,thereby producing more active species.This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface,which provides an effective strategy to improve Fenton-like reactivity and reduce H_(2)O_(2)consumption.展开更多
Amorphous alloys are being newly applied in wastewater treatment because of their unique atomic packing structure.They possess excellent degradation efficiency,stability and reusability.In this work,Fe_(80)Si_(10)B_(1...Amorphous alloys are being newly applied in wastewater treatment because of their unique atomic packing structure.They possess excellent degradation efficiency,stability and reusability.In this work,Fe_(80)Si_(10)B_(10) and Fe_(83)Si_(5)B_(8)P_(4) amorphous ribbons exhibited ad-vanced catalytic performance for the degradation of Methyl Blue(MB)and Rhodamine B(RhB)dyes,and the color removal reach nearly 100%within 11 min for both the dyes.Com-pared with the Fe_(80)Si_(10)B_(10) amorphous ribbon,the Fe_(83)Si_(5)B_(8)P_(4) ribbon showed higher degra-dation efficiency due to its lower reaction activation energy,higher electron transfer ability and higher Fe content,and the formation of the galvanic cell between the strong Fe-P bonds and the weak Fe-B bonds.It also exhibited high stability and reusability.The degradation ef-ficiency was improved when the appropriate concentration of H_(2)O_(2) is added.As regards the pH,high degradation efficiency was observed in acidic MB solution,but it decreased as the pH increased up to pH 7.The application of the electro-Fenton-like process is discussed,which can effectively improve the degradation performance in a nearly natural solution.This study presents a high efficiency low-cost catalyst for synthetic dye degradation and expands the functional applications of Fe-based amorphous alloys.展开更多
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization w...Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.展开更多
Peracetic acid(PAA)has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions;however,the main generation and contribution of organic radicals(R-O·)with unsatisfactory oxid...Peracetic acid(PAA)has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions;however,the main generation and contribution of organic radicals(R-O·)with unsatisfactory oxidation potential compromises wastewater decontamination efficiency.In this study,we demonstrate the rational design and synthesis of ultrafine FeO_(x)nanocluster-anchored carbonaceous nanosheets(UFe-CN)for altering the PAA activation pathway from R-O·to·OH dominant process via in situ framework collapse carbonization of MIL-53(Fe).The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant(e.g.,p-nitrophenol(4-NP))decomposition by the enhanced·OH formation(up to 65.24µmol L^(-1))under a wide pH range(3.0-9.0),outperforming the benchmark iron-based catalyst counterparts by 4.2-10.8 times.This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation,ca.49 times higher than that of its MIL-53(Fe)counterpart,for interface catalysis reactions triggered by iron species cycling.Furthermore,to facilitate adaptive engineering,the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors,including the initial pH,PAA concentration,and UFe-CN dosage.More importantly,the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix,catalyst regeneration capability,and wastewater treatment efficiency.Overall,this study provides a significant understanding of·OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.展开更多
Effective removal of emerging contaminants(ECs)to minimize their impacts on human health and the natural environment is a global priority.For the removal of ECs in water,we fabricated a seaweed spherical microsphere c...Effective removal of emerging contaminants(ECs)to minimize their impacts on human health and the natural environment is a global priority.For the removal of ECs in water,we fabricated a seaweed spherical microsphere catalyst with Cu cation-πstructures by in situ doping of Cu species and ascorbic acid in mesoporous silica(Cu-C-MSNs)via a hydrothermal method.The results indicate that bisphenol A(BPA)is substantially degraded within 5 min under natural conditions,with its biological toxicity considerably weakened.Moreover,industrial wastewater could also be effectively purified by Cu-C-MSNs/H_(2)O_(2) system.The presence of metal sites and the complexation of ECs via cation-πinteraction andπ-πstacking on the catalyst surface were directly responsible for the polarization distribution of electrons,thus activating H_(2)O_(2) and dissolved oxygen(DO).The removal of contaminants could be attributed primarily to 1)the activation of H_(2)O_(2) into ^(·)OH to attack the contaminants and 2)self-cleavage because of the transfer of electrons from the contaminants to the catalysts.This study provides an innovative solution for the effective treatment of ECs and has positive implications for easing global environmental crises.展开更多
Regulating the photo-response region of iron metal-organic frameworks(Fe-MOFs)is a viable strategy for enhancing their practical application in the visible-light driven photo-Fenton-like process.This study developed a...Regulating the photo-response region of iron metal-organic frameworks(Fe-MOFs)is a viable strategy for enhancing their practical application in the visible-light driven photo-Fenton-like process.This study developed a novel pyrazine-based Fe-MOFs(MIL-101(Fe)-Pz)by substituting the 1,4-dicarboxybenzene acid ligands in typical MIL-101(Fe)with 2,5-pyrazinedicarboxylic acid(PzDC),in which sodium acetate was used as coordinative modulator to control the crystal size(2–3μm).The incorporation of Fe-pyridine N coordination structures originated from PzDC ligands gave MIL-101(Fe)-Pz narrowed band gap(1.45 eV)than MIL-101(Fe)(2.54 eV)resulting in improved visible-light adsorption capacity(λ>420 nm),and also increased the proportion of Fe(Ⅱ)in the Fe-clusters.Thus MIL-101(Fe)-Pz exhibited a synergistic enhanced photo-Fenton-like catalytic performance under visible-light irradiation.The MIL-101(Fe)-Pz/H_(2)O_(2)/Vis system could degrade 99%of sulfamethoxazolewithin 30min,whichwas 10-fold faster than that of the pristine MIL-101(Fe),it also effectively removed other organic micropollutants with high durability and stability.Mechanistic analysis revealed that the PzDC ligands substitution decreased the band gap of MIL-101(Fe),giving MIL-101(Fe)-Pz appropriate band structure(-0.40∼1.05 V vs.NHE)which can cover several light-driven process for the generation of reactive oxygen species,including Fe(Ⅲ)reduction and H_(2)O_(2) activation for accelerating•OH generation,as well as oxygen reduction reaction for generating H_(2)O_(2),O_(2)^(•−) and ^(1)O_(2).This study highlights the role of pyridine-N containing ligands in regulating the band structure of Fe-MOFs,providing valuable guidance for the design of Fe-MOFs photocatalysts.展开更多
一、作为哲学的AI for Process(一)郭为的哲学思想1.郭为是谁郭为是谁?他是一位哲学家。顺便说,他同时还领导着神州数码。为什么说郭为是哲学家呢?因为他在著作中谈到高深的哲学,如“数据如水,奔流不息,无界融合”。他引述古希腊哲学家...一、作为哲学的AI for Process(一)郭为的哲学思想1.郭为是谁郭为是谁?他是一位哲学家。顺便说,他同时还领导着神州数码。为什么说郭为是哲学家呢?因为他在著作中谈到高深的哲学,如“数据如水,奔流不息,无界融合”。他引述古希腊哲学家赫拉克利特所说的“万物流转”,又说“你不能两次踏进同一条河流,因为新的水不断地流过你的身旁”,他所表达的意思是“世界上唯一不变的就是变化”。展开更多
The aim of this study was to synthesize a novel lanthanum(La)doped catalyst and to investigate antipyrine removal in wastewater using the Fenton-like process with the catalyst.The La-doped Co-Cu-Fe catalyst was synthe...The aim of this study was to synthesize a novel lanthanum(La)doped catalyst and to investigate antipyrine removal in wastewater using the Fenton-like process with the catalyst.The La-doped Co-Cu-Fe catalyst was synthesized using the modified hydrothermal method.Results showed that the Ladoped catalyst had higher specific surface area and lower particle size than the catalyst without La doping(i.e.,the control)(267 vs.163 m2/g and 14 vs.32 nm,respectively).Under the conditions of catalyst dosage 0.5 g/L,H2O2 concentration 1.70 g/L,and NaHCO3 0.1g/L,the antipyrine removal within 60 min using the Fenton-like process with the La-doped catalyst was much higher than that with the control(95%vs.54%).The hydroxyl radical concentration with the La-doped catalyst within 60 min was two times higher than that with the control(49.2 vs.22.1 gg/L).The high catalytic activity of La-doped catalyst was mainly attributed to its high specific surface area based on the X-ray photoelectron spectroscopy result.Our La-doped catalyst should have great potential to remove antipyrine in wastewater using the heterogeneous Fenton-like process.展开更多
Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue(MB) using refined iron-containing lowgrade attapulgite(ATP) clay, and the removal mechanism was investigated. The MB was i...Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue(MB) using refined iron-containing lowgrade attapulgite(ATP) clay, and the removal mechanism was investigated. The MB was initially adsorbed on the porous ATPs, and then the enriched MB was removed by the H2O2-assisted Fenton-like oxidation with the iron-containing ATP catalyst. Under optimal conditions, the ATP powder exhibits the maximum removal efficiency of 100% with negligible iron leaching(1.5 mg L^(-1)) and no sludge formation. Furthermore,polysulfone/ATP(PSF/ATP) pellets were fabricated through a water-induced phase separation process to construct a fixed-bed reactor(FBR) for continuous contaminant removal. For the first cycle, the maximum adsorption capacity was 15.5 L with an outlet MB concentration of1.973 mg L-1(< 2 mg L^(-1), GB4287-2012) using the PSF/ATP pellets containing 50.0 g of ATP powders, and the maximum Fenton-like oxidation capacity was 35.5 L with the outlet concentration of 0.831 mg L^(-1). After five cycles, the total treated volume of the MB solution was ca. 255 L, and the efficiency remained above 99%. After 10 h of continuous treatment towards practical resin industrial wastewater, the chemical oxygen demand(COD) removal efficiency was still measured at 83.05%, costing 0.398 $ m^(-3). These results demonstrate the practical applicability of iron-containing low-grade ATP clay for textile water treatment.展开更多
In this study,different types of small molecular carbon sources such as melamine,dicyandiamine,pyrocatechol,and o-phenylenediamine were used to regulate the surface structures of iron/nitrogen/carbonbased composites(F...In this study,different types of small molecular carbon sources such as melamine,dicyandiamine,pyrocatechol,and o-phenylenediamine were used to regulate the surface structures of iron/nitrogen/carbonbased composites(Fe-N/C),which were used to activate peroxymonosulfate(PMS).The relationship between different small molecular carbon sources and the electronic structure was investigated.The characteristics of metal-carrier interaction in the Fe-N/C were clarified.As a result,there were significant differences in the degradation efficiency of catalysts prepared with different small molecular carbon sources,which was related to the types of active sites.Density functional theory(DFT)and experiments results showed that the catalyst rich in C-O-C and FeN_(x)exhibited better catalytic activity,which may be attributed to the higher adsorption energy for PMS.The main active species for catalytic degradation of ofloxacin were identified as sulfate radical(SO_(4)^(·-))and hydroxyl radical(^(·)OH)by electron paramagnetic resonance(EPR)spectra.The introduction of different small molecular carbon sources can significantly affect the distribution and electronic structure of active sites on the catalyst surface,thereby regulating the generation and migration of radicals.展开更多
Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnere...Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnered considerable attention due to their well-defined structures,extensive pipeline networks,superior mechanical strength,and adaptability for device customization.However,there remains a paucity of research that systematically summarizes Fenton-like systems based on wood-derived catalysts.In this review,we first summarize the structural designs of wood-derived catalysts based on nano-metal sites and single-atom sites,while also outlining their advantages and limitations applied in Fenton-like systems.Furthermore,we evaluate catalytic modules of wood-derived catalysts for scale-up and continuous Fenton-like systems.Additionally,wood-inspired catalytic materials utilizing commercial textures and their applications in Fenton-like processes are also discussed.This paper aims to comprehensively explore the fundamental mechanisms(e.g.,characteristics of catalytic sites,catalytic performance,and mechanisms)of wood-based catalysts in Fenton-like chemistry,as well as their equipment designs and application scenarios,as well as providing the insights into future developments.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
The Fenton-like reaction between Cu^(2+)and H_(2)O_(2)was employed in chemical mechanical polishing to achieve efficient and high-quality processing of tungsten.The microstructure evolution and material removal rate o...The Fenton-like reaction between Cu^(2+)and H_(2)O_(2)was employed in chemical mechanical polishing to achieve efficient and high-quality processing of tungsten.The microstructure evolution and material removal rate of tungsten during polishing process were investigated via scanning electron microscopy,X-ray photoelectron spectroscopy,ultraviolet−visible spectrophotometry,and electrochemical experiments.The passivation behavior and material removal mechanism were discussed.Results show that the use of mixed H_(2)O_(2)+Cu(NO_(3))_(2)oxidant can achieve higher polishing efficiency and surface quality compared with the single oxidant Cu(NO_(3))_(2)or H_(2)O_(2).The increase in material removal rate is attributed to the rapid oxidation of W into WO_(3)via the chemical reaction between the substrate and hydroxyl radicals produced by the Fenton-like reaction.In addition,material removal rate and static etch rate exhibit significantly different dependencies on the concentration of Cu(NO_(3))_(2),while the superior oxidant for achieving the balance between polishing efficiency and surface quality is 0.5 wt.%H_(2)O_(2)+1.0 wt.%Cu(NO_(3))_(2).展开更多
Carbon dot(CD)is an edge-bound,nanometer-sized carbon material possessing unique optical and electronic properties,making it promising metal-free,environmentally benign.In this study,we identified a highly hydrophilic...Carbon dot(CD)is an edge-bound,nanometer-sized carbon material possessing unique optical and electronic properties,making it promising metal-free,environmentally benign.In this study,we identified a highly hydrophilic CD complexed with Fe(Ⅲ)via carboxyl groups to form CD-COOFeⅢ,which exhibited remarkably enhanced Fenton-like reaction performance boosted by visible light irradiation.CD-COOFeⅢenabled high activity in the visible region beyondλ>420 nm,and maintained stable oxidation efficiency in the presence of H_(2)O_(2)over at least ten cycles.The capacity of electrons transferred from photo-excited CD to reduce Fe(Ⅲ)was calculated to be 1.1 mmol/g of CD.Furthermore,the quantum yield(QY)of solarto-Fe(Ⅱ)conversion reached an impressive 87.7%.These findings not only suggest a viable strategy for efficient conversion of solar-to-chemical using a CD-COOFeⅢcomplex in visible light boosted Fenton-like oxidation reaction,but also provide insight for understanding the effect of nanosized artificial and/or natural carbon materials in iron recycling in a natural surface environment.展开更多
Asymmetric single-atom catalysts(ASACs)have attracted much attention owing to their excellent catalytic properties.However,the relationship between asymmetric coordination and the spin states of metal sites remains un...Asymmetric single-atom catalysts(ASACs)have attracted much attention owing to their excellent catalytic properties.However,the relationship between asymmetric coordination and the spin states of metal sites remains unclear.Additionally,the modulation of reactive oxygen species in Fenton-like reactions remains challenging.Herein,a novel strategy is reported for the rational design of highly loaded Co ASACs(CoN_(1)C_(2)/C_(2)N)immobilized on three-dimensional flower-like C_(2)N using an in situ-generated carbon defect method.In particular,the asymmetrically tricoordinated CoN_(1)C_(2)/C_(2)N exhibited excellent catalytic activity for sulfachloropyridazine degradation,with a turnover frequency of 36.8 min^(–1).Experimental results and theoretical calculations revealed that the electron spin state of the Co-active sites was transferred from the low-spin configuration(t_(2g)^(6)e_(g)^(1))to the high-spin configuration(t_(2g)^(5)e_(g)^(2))owing to asymmetric coordination.The high-spin Co 3d orbital in CoN_(1)C_(2)/C_(2)N possessed more unpaired electrons and therefore,had a strong ability to gain electrons from the O 2p orbitals of HSO_(5)^(–),boosting d-p orbital hybridization.More importantly,the spin-electron filling in theσ^(*)orbital of high-spin Co 3d−O 2p accelerated the desorption of^(*)SO_(5)•^(−),which acted as a rate-limiting step in the reaction,thus facilitating more^(1)O_(2)generation.This study provides an innovative synthetic route for practical ASACs and clarifies the critical relationship between structure and spin state,paving the way for advancements in environmental remediation and energy conversion applications.展开更多
Agricultural Products Processing and Storage(ISSN 3059-4510,Owner:Hunan Academy of Agricultural Sciences,China.Production and hosting:Springer Nature)is an international,peer-reviewed open access journal with the aim ...Agricultural Products Processing and Storage(ISSN 3059-4510,Owner:Hunan Academy of Agricultural Sciences,China.Production and hosting:Springer Nature)is an international,peer-reviewed open access journal with the aim to offer a platform for the rapid dissemination of significant,novel,and high-impact research in the fields of agricultural product processing science,technology,engineering,and nutrition.Additionally,supplemental issues are curated and published to facilitate in-depth discussions on special topics.展开更多
This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degra...This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.展开更多
The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF...The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF)argon plasma,and the temperatures were measured using a DPV-2000 monitor.A model combining the electromagnetism,thermal flow,and heat transfer characteristics of powder during in-flight heating in argon plasma was proposed.The melting processes of CeO_(2)powders of different diameters,with and without thermal resistance effect,were investigated.Results show that the heating process of CeO_(2)powder particles consists of three main stages,one of which is relevant to a dimensionless parameter known as the Biot number.When the Biot value≥0.1,thermal resistance increases significantly,especially for the larger powders.The predicted temperature of the particles at the outlet(1800–2880 K)is in good agreement with the experimental result.展开更多
基金supported by the National Natural Science Foundation of China(No.52370168)the Key Laboratory of Functional Biology and Pollution Control in red soil regions of Jiangxi Province(No.2023SSY02051)。
文摘Antibiotic-contaminated wastewater poses a global threat to aquatic ecosystems.Fenton-like oxidative processes effectively decompose recalcitrant pollutants.While these oxidative processes effectively break down target contaminants,they may also produce uncontrolled intermediates,potentially resulting in unexpected combined toxicities.This review explores the chemical mechanisms behind Fenton-like reactions,particularly in antibiotic removal,and evaluates the formation of byproducts and their potential toxicological effects.Furthermore,recommendations for optimizing catalyst design and treatment conditions are provided to enhance degradation performance while minimizing ecological risks.This study highlights critical concerns regarding the toxicity of degradation byproducts and their impact on ecosystems by integrating chemical and biological risk assessments.By integrating chemical and biological risk assessments with computational toxicology,particularly quantitative structure-activity relationship(QSAR)modeling,this study proposes a comprehensive approach to evaluate degradation and toxicity.This work highlights the importance of a comprehensive framework for evaluating degradation efficiency and toxicity,contributing to safer and more effective antibiotic wastewater treatment strategies.The findings underscore the importance of balancing degradation efficiency with environmental safety in wastewater treatment processes involving advanced oxidative technologies.
基金financially supported by the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20114219110002)Fund from Coal Conversion and New Carbon Materials Hubei Key Laboratory(Wuhan University of Science and Technology)(No.WKDM201107)Educational Commission of Hubei Province of China(No.D20131107)
文摘In this study, Fe3O4nanoparticles（Fe3O4NPs） were successfully prepared via oxidation–precipitation method and characterized by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and Fourier transform infrared spectroscopy（FT-IR）. The characterization results indicated that Fe3O4 NPs with regular crystal structure and a narrow of diameters had been synthesized successfully and had high purity. A series of experiments were carried out to investigate the degradation of Orange II by the obtained heterogeneous Fe3O4 catalysts in the presence of H2O2. The response surface methodology（RSM） based on Box–Behnken design（BBD） was employed to design and optimize individual and interactive effects of the four main independent parameters（catalyst loading, initial p H, reaction temperature and H2O2concentration） on decolorization efficiency of Orange II. A significant quadratic model（p-value 〈0.0001, R2= 0.9369） was derived using analysis of variance（ANOVA）. Optimum conditions were catalyst loading of 1.5 g/L, initial p H of 2.7, reaction temperature of 42 8C and H2O2 concentration of 22 mmol/L, respectively. The predicted decolorization rate under the optimum conditions as determined by the proposed model was 99.55%. Confirmatory tests were carried out and the decolorization rate of 99.49% was observed under the optimum conditions, which agreed well with the model prediction.
基金financially supported by the National Natural Science Foundation of China (Nos.52070046,51808140,51838005 and 21906034)the Introduced Innovative R&D Team Project under the"Pearl River Talent Recruitment Program"of Guangdong Province (No.2019ZT08L387)the BL14W1 beamline of Shanghai Synchrotron Radiation Facility (SSRF,China)。
文摘Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD).The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions,accompanied by low H_(2)O_(2)consumption.The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species,which play a significant role in the high-performance Fenton-like reaction.The pollutants that served as electron donors were decomposed in the electron-poor carbon centers,whereas H_(2)O_(2)and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds,thereby producing more active species.This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface,which provides an effective strategy to improve Fenton-like reactivity and reduce H_(2)O_(2)consumption.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea govern-ment(MSIT)(No.2018R1A4A1022260).
文摘Amorphous alloys are being newly applied in wastewater treatment because of their unique atomic packing structure.They possess excellent degradation efficiency,stability and reusability.In this work,Fe_(80)Si_(10)B_(10) and Fe_(83)Si_(5)B_(8)P_(4) amorphous ribbons exhibited ad-vanced catalytic performance for the degradation of Methyl Blue(MB)and Rhodamine B(RhB)dyes,and the color removal reach nearly 100%within 11 min for both the dyes.Com-pared with the Fe_(80)Si_(10)B_(10) amorphous ribbon,the Fe_(83)Si_(5)B_(8)P_(4) ribbon showed higher degra-dation efficiency due to its lower reaction activation energy,higher electron transfer ability and higher Fe content,and the formation of the galvanic cell between the strong Fe-P bonds and the weak Fe-B bonds.It also exhibited high stability and reusability.The degradation ef-ficiency was improved when the appropriate concentration of H_(2)O_(2) is added.As regards the pH,high degradation efficiency was observed in acidic MB solution,but it decreased as the pH increased up to pH 7.The application of the electro-Fenton-like process is discussed,which can effectively improve the degradation performance in a nearly natural solution.This study presents a high efficiency low-cost catalyst for synthetic dye degradation and expands the functional applications of Fe-based amorphous alloys.
基金supported byHainan Provincial Natural Science Foundation of China(Nos.422RC600,519QN175)National Natural Science Foundation ofChina(Nos.52160018,21801053,52400206,52500209)High-Level Talent Program of Hainan Province(Nos.XJ2400008202,XJ2400011473).
文摘Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.
基金supported by the National Natural Science Foundation of China(22106141,22176124)the Research Start-up Funding from Shanghai Jiao Tong University(WH220416002)+1 种基金China Postdoctoral Science Foundation(2022M712827)Postdoctoral Program(TYY202103)of Zhejiang Sci-Tech University Tongxiang Research Institute.
文摘Peracetic acid(PAA)has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions;however,the main generation and contribution of organic radicals(R-O·)with unsatisfactory oxidation potential compromises wastewater decontamination efficiency.In this study,we demonstrate the rational design and synthesis of ultrafine FeO_(x)nanocluster-anchored carbonaceous nanosheets(UFe-CN)for altering the PAA activation pathway from R-O·to·OH dominant process via in situ framework collapse carbonization of MIL-53(Fe).The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant(e.g.,p-nitrophenol(4-NP))decomposition by the enhanced·OH formation(up to 65.24µmol L^(-1))under a wide pH range(3.0-9.0),outperforming the benchmark iron-based catalyst counterparts by 4.2-10.8 times.This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation,ca.49 times higher than that of its MIL-53(Fe)counterpart,for interface catalysis reactions triggered by iron species cycling.Furthermore,to facilitate adaptive engineering,the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors,including the initial pH,PAA concentration,and UFe-CN dosage.More importantly,the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix,catalyst regeneration capability,and wastewater treatment efficiency.Overall,this study provides a significant understanding of·OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
基金the National Natural Science Foundation of China(Nos.52122009,52070046,and 51838005)the Introduced Innovative R&D Team Project under the“Pearl River Talent Recruitment Program”of Guangdong Province(China)(No.2019ZT08L387)the Basic and Applied Basic Research Project of Guangzhou(China)(No.202201020163).
文摘Effective removal of emerging contaminants(ECs)to minimize their impacts on human health and the natural environment is a global priority.For the removal of ECs in water,we fabricated a seaweed spherical microsphere catalyst with Cu cation-πstructures by in situ doping of Cu species and ascorbic acid in mesoporous silica(Cu-C-MSNs)via a hydrothermal method.The results indicate that bisphenol A(BPA)is substantially degraded within 5 min under natural conditions,with its biological toxicity considerably weakened.Moreover,industrial wastewater could also be effectively purified by Cu-C-MSNs/H_(2)O_(2) system.The presence of metal sites and the complexation of ECs via cation-πinteraction andπ-πstacking on the catalyst surface were directly responsible for the polarization distribution of electrons,thus activating H_(2)O_(2) and dissolved oxygen(DO).The removal of contaminants could be attributed primarily to 1)the activation of H_(2)O_(2) into ^(·)OH to attack the contaminants and 2)self-cleavage because of the transfer of electrons from the contaminants to the catalysts.This study provides an innovative solution for the effective treatment of ECs and has positive implications for easing global environmental crises.
基金supported by the National Natural Science Foundation of China(Nos.52300120 and 52070144)the Fundamental Research Funds for the Central Universities(No.22120240465).
文摘Regulating the photo-response region of iron metal-organic frameworks(Fe-MOFs)is a viable strategy for enhancing their practical application in the visible-light driven photo-Fenton-like process.This study developed a novel pyrazine-based Fe-MOFs(MIL-101(Fe)-Pz)by substituting the 1,4-dicarboxybenzene acid ligands in typical MIL-101(Fe)with 2,5-pyrazinedicarboxylic acid(PzDC),in which sodium acetate was used as coordinative modulator to control the crystal size(2–3μm).The incorporation of Fe-pyridine N coordination structures originated from PzDC ligands gave MIL-101(Fe)-Pz narrowed band gap(1.45 eV)than MIL-101(Fe)(2.54 eV)resulting in improved visible-light adsorption capacity(λ>420 nm),and also increased the proportion of Fe(Ⅱ)in the Fe-clusters.Thus MIL-101(Fe)-Pz exhibited a synergistic enhanced photo-Fenton-like catalytic performance under visible-light irradiation.The MIL-101(Fe)-Pz/H_(2)O_(2)/Vis system could degrade 99%of sulfamethoxazolewithin 30min,whichwas 10-fold faster than that of the pristine MIL-101(Fe),it also effectively removed other organic micropollutants with high durability and stability.Mechanistic analysis revealed that the PzDC ligands substitution decreased the band gap of MIL-101(Fe),giving MIL-101(Fe)-Pz appropriate band structure(-0.40∼1.05 V vs.NHE)which can cover several light-driven process for the generation of reactive oxygen species,including Fe(Ⅲ)reduction and H_(2)O_(2) activation for accelerating•OH generation,as well as oxygen reduction reaction for generating H_(2)O_(2),O_(2)^(•−) and ^(1)O_(2).This study highlights the role of pyridine-N containing ligands in regulating the band structure of Fe-MOFs,providing valuable guidance for the design of Fe-MOFs photocatalysts.
文摘一、作为哲学的AI for Process(一)郭为的哲学思想1.郭为是谁郭为是谁?他是一位哲学家。顺便说,他同时还领导着神州数码。为什么说郭为是哲学家呢?因为他在著作中谈到高深的哲学,如“数据如水,奔流不息,无界融合”。他引述古希腊哲学家赫拉克利特所说的“万物流转”,又说“你不能两次踏进同一条河流,因为新的水不断地流过你的身旁”,他所表达的意思是“世界上唯一不变的就是变化”。
基金grants from the National Key R&D Program of China(Nos.2017YFB0903700 and 2017YFB0903703)the National Natural Science Foundation of China(Grant Nos.51608547,51278500 and 51308557)the Fundamental Research Funds for the Central Universities(181gpy43).
文摘The aim of this study was to synthesize a novel lanthanum(La)doped catalyst and to investigate antipyrine removal in wastewater using the Fenton-like process with the catalyst.The La-doped Co-Cu-Fe catalyst was synthesized using the modified hydrothermal method.Results showed that the Ladoped catalyst had higher specific surface area and lower particle size than the catalyst without La doping(i.e.,the control)(267 vs.163 m2/g and 14 vs.32 nm,respectively).Under the conditions of catalyst dosage 0.5 g/L,H2O2 concentration 1.70 g/L,and NaHCO3 0.1g/L,the antipyrine removal within 60 min using the Fenton-like process with the La-doped catalyst was much higher than that with the control(95%vs.54%).The hydroxyl radical concentration with the La-doped catalyst within 60 min was two times higher than that with the control(49.2 vs.22.1 gg/L).The high catalytic activity of La-doped catalyst was mainly attributed to its high specific surface area based on the X-ray photoelectron spectroscopy result.Our La-doped catalyst should have great potential to remove antipyrine in wastewater using the heterogeneous Fenton-like process.
基金supported by Gansu Cuihua Technology Co.,Ltd.(H2020292)Science and Technology Planning of Baiyin City,Fundamental Research Funds for the Central Universities (buctrc202208)+2 种基金Engineering Research Center of Non-metallic Minerals of Zhejiang Province and the Beijing Engineering Center for Hierarchical Catalysts. Central Government Guiding Funds for Local Science and Technology Development (2022ZY015)Nanjiang Technology Project(2023AB028)Open Laboratory of State Key Laboratory of Organic and Inorganic Composites (oic-202301006)。
文摘Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue(MB) using refined iron-containing lowgrade attapulgite(ATP) clay, and the removal mechanism was investigated. The MB was initially adsorbed on the porous ATPs, and then the enriched MB was removed by the H2O2-assisted Fenton-like oxidation with the iron-containing ATP catalyst. Under optimal conditions, the ATP powder exhibits the maximum removal efficiency of 100% with negligible iron leaching(1.5 mg L^(-1)) and no sludge formation. Furthermore,polysulfone/ATP(PSF/ATP) pellets were fabricated through a water-induced phase separation process to construct a fixed-bed reactor(FBR) for continuous contaminant removal. For the first cycle, the maximum adsorption capacity was 15.5 L with an outlet MB concentration of1.973 mg L-1(< 2 mg L^(-1), GB4287-2012) using the PSF/ATP pellets containing 50.0 g of ATP powders, and the maximum Fenton-like oxidation capacity was 35.5 L with the outlet concentration of 0.831 mg L^(-1). After five cycles, the total treated volume of the MB solution was ca. 255 L, and the efficiency remained above 99%. After 10 h of continuous treatment towards practical resin industrial wastewater, the chemical oxygen demand(COD) removal efficiency was still measured at 83.05%, costing 0.398 $ m^(-3). These results demonstrate the practical applicability of iron-containing low-grade ATP clay for textile water treatment.
基金supported by National Natural Science Foundation of China(Nos.52170086,52300056)Natural Science Foundation of Shandong Province(Nos.ZR2021ME013,ZR202211280298)。
文摘In this study,different types of small molecular carbon sources such as melamine,dicyandiamine,pyrocatechol,and o-phenylenediamine were used to regulate the surface structures of iron/nitrogen/carbonbased composites(Fe-N/C),which were used to activate peroxymonosulfate(PMS).The relationship between different small molecular carbon sources and the electronic structure was investigated.The characteristics of metal-carrier interaction in the Fe-N/C were clarified.As a result,there were significant differences in the degradation efficiency of catalysts prepared with different small molecular carbon sources,which was related to the types of active sites.Density functional theory(DFT)and experiments results showed that the catalyst rich in C-O-C and FeN_(x)exhibited better catalytic activity,which may be attributed to the higher adsorption energy for PMS.The main active species for catalytic degradation of ofloxacin were identified as sulfate radical(SO_(4)^(·-))and hydroxyl radical(^(·)OH)by electron paramagnetic resonance(EPR)spectra.The introduction of different small molecular carbon sources can significantly affect the distribution and electronic structure of active sites on the catalyst surface,thereby regulating the generation and migration of radicals.
基金supported by National Natural Science Foundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+4 种基金Shandong Provincial Excellent Youth(No.ZR2022YQ47)the doctor research start Foundation of Shaanxi University of Technology(No.SLGRCQD004)Science and Technology Innovation Team Project of Shaanxi Province(No.2025RS-CXTD-040)the General Special Scientific Research Program of the Shaanxi Provincial Department of Education(No.24JK0366)supported by funding from Shandong Provincial Key Laboratory of Monocrystalline Silicon Semiconductor Materials and Technology。
文摘Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnered considerable attention due to their well-defined structures,extensive pipeline networks,superior mechanical strength,and adaptability for device customization.However,there remains a paucity of research that systematically summarizes Fenton-like systems based on wood-derived catalysts.In this review,we first summarize the structural designs of wood-derived catalysts based on nano-metal sites and single-atom sites,while also outlining their advantages and limitations applied in Fenton-like systems.Furthermore,we evaluate catalytic modules of wood-derived catalysts for scale-up and continuous Fenton-like systems.Additionally,wood-inspired catalytic materials utilizing commercial textures and their applications in Fenton-like processes are also discussed.This paper aims to comprehensively explore the fundamental mechanisms(e.g.,characteristics of catalytic sites,catalytic performance,and mechanisms)of wood-based catalysts in Fenton-like chemistry,as well as their equipment designs and application scenarios,as well as providing the insights into future developments.
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.
文摘The Fenton-like reaction between Cu^(2+)and H_(2)O_(2)was employed in chemical mechanical polishing to achieve efficient and high-quality processing of tungsten.The microstructure evolution and material removal rate of tungsten during polishing process were investigated via scanning electron microscopy,X-ray photoelectron spectroscopy,ultraviolet−visible spectrophotometry,and electrochemical experiments.The passivation behavior and material removal mechanism were discussed.Results show that the use of mixed H_(2)O_(2)+Cu(NO_(3))_(2)oxidant can achieve higher polishing efficiency and surface quality compared with the single oxidant Cu(NO_(3))_(2)or H_(2)O_(2).The increase in material removal rate is attributed to the rapid oxidation of W into WO_(3)via the chemical reaction between the substrate and hydroxyl radicals produced by the Fenton-like reaction.In addition,material removal rate and static etch rate exhibit significantly different dependencies on the concentration of Cu(NO_(3))_(2),while the superior oxidant for achieving the balance between polishing efficiency and surface quality is 0.5 wt.%H_(2)O_(2)+1.0 wt.%Cu(NO_(3))_(2).
基金the support of Natural Science Foundation of China(No.22276123)the Shanghai Engineering Research Center of Water Environment Simulation and Ecological Restoration(No.WESER-202201)the Postdoctoral Fellowship Program of CPSF(No.GZB20240456)。
文摘Carbon dot(CD)is an edge-bound,nanometer-sized carbon material possessing unique optical and electronic properties,making it promising metal-free,environmentally benign.In this study,we identified a highly hydrophilic CD complexed with Fe(Ⅲ)via carboxyl groups to form CD-COOFeⅢ,which exhibited remarkably enhanced Fenton-like reaction performance boosted by visible light irradiation.CD-COOFeⅢenabled high activity in the visible region beyondλ>420 nm,and maintained stable oxidation efficiency in the presence of H_(2)O_(2)over at least ten cycles.The capacity of electrons transferred from photo-excited CD to reduce Fe(Ⅲ)was calculated to be 1.1 mmol/g of CD.Furthermore,the quantum yield(QY)of solarto-Fe(Ⅱ)conversion reached an impressive 87.7%.These findings not only suggest a viable strategy for efficient conversion of solar-to-chemical using a CD-COOFeⅢcomplex in visible light boosted Fenton-like oxidation reaction,but also provide insight for understanding the effect of nanosized artificial and/or natural carbon materials in iron recycling in a natural surface environment.
文摘Asymmetric single-atom catalysts(ASACs)have attracted much attention owing to their excellent catalytic properties.However,the relationship between asymmetric coordination and the spin states of metal sites remains unclear.Additionally,the modulation of reactive oxygen species in Fenton-like reactions remains challenging.Herein,a novel strategy is reported for the rational design of highly loaded Co ASACs(CoN_(1)C_(2)/C_(2)N)immobilized on three-dimensional flower-like C_(2)N using an in situ-generated carbon defect method.In particular,the asymmetrically tricoordinated CoN_(1)C_(2)/C_(2)N exhibited excellent catalytic activity for sulfachloropyridazine degradation,with a turnover frequency of 36.8 min^(–1).Experimental results and theoretical calculations revealed that the electron spin state of the Co-active sites was transferred from the low-spin configuration(t_(2g)^(6)e_(g)^(1))to the high-spin configuration(t_(2g)^(5)e_(g)^(2))owing to asymmetric coordination.The high-spin Co 3d orbital in CoN_(1)C_(2)/C_(2)N possessed more unpaired electrons and therefore,had a strong ability to gain electrons from the O 2p orbitals of HSO_(5)^(–),boosting d-p orbital hybridization.More importantly,the spin-electron filling in theσ^(*)orbital of high-spin Co 3d−O 2p accelerated the desorption of^(*)SO_(5)•^(−),which acted as a rate-limiting step in the reaction,thus facilitating more^(1)O_(2)generation.This study provides an innovative synthetic route for practical ASACs and clarifies the critical relationship between structure and spin state,paving the way for advancements in environmental remediation and energy conversion applications.
文摘Agricultural Products Processing and Storage(ISSN 3059-4510,Owner:Hunan Academy of Agricultural Sciences,China.Production and hosting:Springer Nature)is an international,peer-reviewed open access journal with the aim to offer a platform for the rapid dissemination of significant,novel,and high-impact research in the fields of agricultural product processing science,technology,engineering,and nutrition.Additionally,supplemental issues are curated and published to facilitate in-depth discussions on special topics.
基金supported by the Financial Supports of the National Natural Science Foundation of China(Nos.51508056,52370030 and 42007352)the Chongqing Postgraduate Joint Training Base Project(No.JDLHPYJD2022005)the special fund of Henan Key Labora-tory of Water Pollution Control and Rehabilitation Technology(No.CJSZ2024001).
文摘This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.
基金National Natural Science Foundation of China(11875039)Shanxi Scholarship Council of China(2023-033)+2 种基金Fundamental Research Program of Shanxi Province(202303021221071)China Baowu Low Carbon Metallurgical Innovation Foundation(2022)2023 Anhui Major Industrial Innovation Plan Project。
文摘The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF)argon plasma,and the temperatures were measured using a DPV-2000 monitor.A model combining the electromagnetism,thermal flow,and heat transfer characteristics of powder during in-flight heating in argon plasma was proposed.The melting processes of CeO_(2)powders of different diameters,with and without thermal resistance effect,were investigated.Results show that the heating process of CeO_(2)powder particles consists of three main stages,one of which is relevant to a dimensionless parameter known as the Biot number.When the Biot value≥0.1,thermal resistance increases significantly,especially for the larger powders.The predicted temperature of the particles at the outlet(1800–2880 K)is in good agreement with the experimental result.
