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
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
A series of spinel fe rrites magnetic nanopa rticles NiFe2 O4 we re synthesized as the heterogeneous Fentonlike catalyst by hydrothermal method and then NiFe2 O4@SiO2 catalysts were obtained by the modification of NiF...A series of spinel fe rrites magnetic nanopa rticles NiFe2 O4 we re synthesized as the heterogeneous Fentonlike catalyst by hydrothermal method and then NiFe2 O4@SiO2 catalysts were obtained by the modification of NiFe2 O4 via micro emulsion method.XRD,VSM,FTIR,SEM,TEM,BET and XPS were carried to analyze the difference between the above two catalysts.NiFe2 O4@SiO2 catalyst exhibited the higher catalytic activity than NiFe2 O4 for the degradation of Rhodamine B owe to the outer Si02 layers surface,the more important is both of them showed the better catalytic performance when at neutral pH environment.展开更多
Background Artificial insemination(AI)is a routine breeding technology in animal reproduction.Nevertheless,the temperature-sensitive nature and short fertile lifespan of ram sperm samples hamper its use in AI.In this ...Background Artificial insemination(AI)is a routine breeding technology in animal reproduction.Nevertheless,the temperature-sensitive nature and short fertile lifespan of ram sperm samples hamper its use in AI.In this sense,nanotechnology is an interesting tool to improve sperm protection due to the development of nanomaterials for AI,which could be used as delivery vehicles.In this work,we explored the feasibility of vitamin E nanoemulsion(NE)for improving sperm quality during transport.Results With the aim of evaluating this proposal,ejaculates of 7 mature rams of Manchega breed were collected by artificial vagina and extended to 60×10^(6)spz/mL in AndromedR.Samples containing control and NE(12 mmol/L)with and without exogenous oxidative stress(100μmol/L Fe2+/ascorbate)were stored at 22 and 15℃and motility(CASA),viability(YO-PRO/PI),acrosomal integrity(PNA-FITC/PI),mitochondrial membrane potential(Mitotracker Deep Red 633),lipoperoxidation(C11 BODIPY 581/591),intracellular reactive oxygen species(ROS)production and DNA status(SCSAR)monitored during 96 h.Our results show that NE could be used to maintain ram spermatozoa during transport at 15 and 22℃for up to 96 h,with no appreciable loss of kinematic and physiological characteristics of freshly collected samples.Conclusions The storage of ram spermatozoa in liquid form for 2-5 d with vitamin E nanoemulsions may lead more flexibility to breeders in AI programs.In view of the potential and high versatility of these nanodevices,further studies are being carried out to assess the proposed sperm preservation medium on fertility after artificial insemination.展开更多
Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stab...Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites,thus meeting fundamental requirements for practical application.The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts(SACs)prepared based on silicon-based materials(mesoporous silica,silicon-based minerals,and organosilicon materials)has unique advantages such as structural stability(especially important under strong oxidation conditions)and environmental protection.In this paper,the preparation strategies for the silicon-based SACs were assessed first,and the structural characteristics of various silicon-based SACs are systematically discussed,their application process and mechanism in Fenton-like process to achieve water purification are investigated,and the progress of Fenton-like process in density functional theory(DFT)of siliconbased derived single atom catalysts is summarized.In this paper,the preparation strategies and applications of silicon-based derived SACs are analyzed in depth,and their oxidation activities and pathways to different pollutants in water are reviewed.In addition,this paper also summarizes the device design and application of silicon-based derived SACs,and prospects the future development of silicon-based SACs in Fenton-like applications.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
Precise manipulation of the catalytic spin configuration and delineation of the relationship between spin related properties and oxidation pathways remain significant challenges in Fenton-like processes.Herein,encapsu...Precise manipulation of the catalytic spin configuration and delineation of the relationship between spin related properties and oxidation pathways remain significant challenges in Fenton-like processes.Herein,encapsulated cobalt nanoparticles and cobalt-nitrogen-doped carbon moieties,endowed with confinement effects and variations in shell curvature were constructed via straightforward pyrolysis strategies,inducing alterations in magnetic anisotropy,electronic energy levels and spin polarization.The enhanced spin polarization at cobalt sites leads to a reduction in crystal field splitting energy and an increase in electronic spin density.This phenomenon facilitated electron transfer from cobalt orbitals to pz orbitals of oxygen species within peroxymonosulfate molecules,thereby promoting the formation of high-valent cobalt species.The encapsulation effectively stabilized cobalt nanoparticles,mitigating their dissolution or deactivation during reactions,which in turn enhances stability and durability in continuous flow processes.The high-valent cobalt species within the shell exhibit increased exposure and generate localized high concentrations,thereby intensifying interactions with migrating pollutants and enabling efficient and selective oxidation of emerging compounds with elevated redox potentials.This work underscores the profound impact of confined encapsulation curvature and spin polarization characteristics of metal sites on catalytic oxidation pathways and performance,opening novel avenues for spin engineering in practical environmental catalysis.展开更多
The photocatalytic degradation on the bismuth containing complex oxide was revised in detail including the synthesis and classification of photocatalyts, and then the photocatalytic reaction, scavenger, and the mechan...The photocatalytic degradation on the bismuth containing complex oxide was revised in detail including the synthesis and classification of photocatalyts, and then the photocatalytic reaction, scavenger, and the mechanism of reaction. In particular, the perspectives of photocatalytic degradation on the bismuth containing oxide were analyzed in detail.展开更多
[ Objective] This study aimed to investigate enzymatic hydrolysis technology of glutinous rice and the oxidation resistance activity of the enzymatic hydrolysis solution. [ Method ] White glutinous rice was hydrolyzed...[ Objective] This study aimed to investigate enzymatic hydrolysis technology of glutinous rice and the oxidation resistance activity of the enzymatic hydrolysis solution. [ Method ] White glutinous rice was hydrolyzed using four kinds of proteases including neutral protease, alkaline protease, papain and trypsin. Using the scavenging rate of hydroxyl radical （ ·OH） as an indicator and appropriate protease as hydrolytic enzyme, the effects of protein substrate concentration, enzyme dosage, enzymatic hydrolysis temperature and initial pH on the abilities of proteases to scavenge hydroxyl radical from enzymatic hydrolysis solution of glutinous rice were investigated. Based on single-factor test, L9 （34） orthogonal experimental design was adopted, to determine the optimal enzymatic hydrolysis condi- tions leading to the highest oxidation resistance activity of enzymatic hydrolysis solution. [ Result] The optimized process parameters for enzymatic hydrolysis of glu- tinous rice protein with neutral protease were： protein substrate concentration of 2%, enzyme dosage of 24 000 U/g protein （protein meter）, enzymatic hydrolysis temperature of 55 ℃, initial pH of 8.0, and enzymatic hydrolysis duration of 0.5 h; under these conditions, the hydroxyl radical scavenging rate could reach 56. 05% ; protein substrate concentration, enzyme dosage, enzymatic hydrolysis temperature and initial pH had extremely significant effects on the hydroxyl radical scavenging rate. In addition, the activities of antioxidant peptides in glutinous rice hydrolysates were well maintained within a temperature range of 60 - 100℃. [Condusion] The study produced theoretical feasibility reference for the production of functional base powder by spray drying.展开更多
A three-terminal silicon-based light emitting device is proposed and fabricated in standard 0.35 μm complementary metal-oxide-semiconductor technology. This device is capable of versatile working modes： it can emit ...A three-terminal silicon-based light emitting device is proposed and fabricated in standard 0.35 μm complementary metal-oxide-semiconductor technology. This device is capable of versatile working modes： it can emit visible to near infra-red （NIR） light （the spectrum ranges from 500 nm to 1000 nm） in reverse bias avalanche breakdown mode with working voltage between 8.35 V-12 V and emit NIR light （the spectrum ranges from 900 nm to 1300 nm） in the forward injection mode with working voltage below 2 V. An apparent modulation effect on the light intensity from the polysilicon gate is observed in the forward injection mode. Furthermore, when the gate oxide is broken down, NIR light is emitted from the polysilicon/oxide/silicon structure. Optoelectronic characteristics of the device working in different modes are measured and compared. The mechanisms behind these different emissions are explored.展开更多
This article, for the first time, provides a novel advanced oxidation process based on sulfate radical （SO^4·-） to degrade organic pollutants in wastewater： microwave （MW）-activated persulfate oxidation （AP...This article, for the first time, provides a novel advanced oxidation process based on sulfate radical （SO^4·-） to degrade organic pollutants in wastewater： microwave （MW）-activated persulfate oxidation （APO） with or without active carbon （AC）. Azo dye acid Orange 7 （AO7） is used as a model compound to investigate the high reactivity of MW-APO. It is found that AO7 （up to 1000 mg/L） is completely decolorized within 5-7 min under an 800 W MW furnace assisted-APO. In the presence of chloride ion （up to 0.50 mol/L）, the decolorization is still 100% completed, though delayed for about 1-2 min. Experiments are made to examine the enhancement by AC. It is exciting to find that the 100% decolorization of AO7 （500 mg/L） is achieved within 3 min by MW-APO using 1.0 g/L AC as catalyst, while the degradation efficiency maintains at 50% by MW energy without persulfate after about 5 min. Besides the destruction of visible light chromophore band of AO7 （484 nm）, during MW-APO, two bands in the ultraviolet region （228 nm and 310 nm） are rapidly broken down. The removal of COD is about 83%-95% for 500 mg/L AO7. SO^4·- is identified with quenching studies using specific alcohols. Both SO^4·- and ·OH could degrade AO7, but SO^4·- plays the dominant role. In a word, MW-APO AC is a new catalytic combustion technology for destruction of organic contamination even for high concentration.展开更多
Many studies have successfully built iron-mediatedmaterials to activate or catalyze Fentonlike reactions,with applications in water and wastewater treatment being investigated.However,the developed materials are rarel...Many studies have successfully built iron-mediatedmaterials to activate or catalyze Fentonlike reactions,with applications in water and wastewater treatment being investigated.However,the developed materials are rarely compared with each other regarding their performance of organic contaminant removal.In this review,the recent advances of Fentonlike processes in homogeneous and heterogeneous ways are summarized,especially the performance and mechanism of activators including ferrous iron,zero valent iron,iron oxides,iron-loaded carbon,zeolite,and metal organic framework materials.Also,this work mainly compares three O-O bond containing oxidants including hydrogen dioxide,persulfate,and percarbonate,which are environmental-friendly oxidants and feasible for in-situ chemical oxidation.The influence of reaction conditions,catalyst properties and benefits are analyzed and compared.In addition,the challenges and strategies of these oxidants in applications and the major mechanisms of the oxidation process have been discussed.This work can help understand the mechanistic insights of variable Fenton-like reactions,the role of emerging iron-based materials,and provide guidance for choosing appropriate technologies when facing real-world water and wastewater applications.展开更多
Between the two major arsenic-containing salts in natural water, arsenite(As(Ⅲ)) is far more harmful to human and the environment than arsenate(As(V)) due to its high toxicity and transportability. Therefore, preoxid...Between the two major arsenic-containing salts in natural water, arsenite(As(Ⅲ)) is far more harmful to human and the environment than arsenate(As(V)) due to its high toxicity and transportability. Therefore, preoxidation of As(Ⅲ) to As(V) is considered to be an effective means to reduce the toxicity of arsenic and to promote the removal efficiency of arsenic. Due to their high catalytic activity and arsenic affinity, iron-based functional materials can quickly oxidize As(Ⅲ) to As(V) in heterogeneous Fenton-like systems, and then remove As(V) from water through adsorption and surface coprecipitation. In this review, the effects of different iron-based functional materials such as zero-valent iron and iron(hydroxy) oxides on arsenic removal are compared, and the catalytic oxidation mechanism of As(Ⅲ) in heterogeneous Fenton process is further clarified. Finally, the main challenges and opportunities faced by iron-based As(Ⅲ) oxidation functional materials are prospected.展开更多
Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)proce...Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)process,which combines coal gasification and high-temperature fuel cells,was proposed in 2017 to improve the efficiency of coal-based power generation and reduce CO_(2)emissions.Supported by the National Key R&D Program of China,the IGFC for nearzero CO_(2)emissions program was enacted with the goal of achieving near-zero CO_(2)emissions based on(1)catalytic combustion of the flue gas from solid oxide fuel cell(SOFC)stacks and(2)CO_(2)conversion using solid oxide electrolysis cells(SOECs).In this work,we investigated a kW-level catalytic combustion burner and SOEC stack,evaluated the electrochemical performance of the SOEC stack in H2O electrolysis and H2O/CO_(2)co-electrolysis,and established a multiscale and multi-physical coupling simulation model of SOFCs and SOECs.The process developed in this work paves the way for the demonstration and deployment of IGFC technology in the future.展开更多
The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared wi...The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared with electrochemical oxidation technology,ozonation technology,and traditional peroxone technology.Due to the high kinetics of pollutant degradation,the electro-peroxone process can reduce the reaction time and energy consumption of pollutant treatment in wastewater.The electroperoxone technology can promote pollutant degradation and mineralization,which shows obvious synergistic effects of electrochemical oxidation and ozonation for wastewater treatment.Most importantly,the research mechanism of the electro-peroxone technology is systematically introduced from two aspects of cathode reaction and bulk reaction.The influence of experimental parameters on the wastewater treatment effect is also discussed.Finally,the potential applications and future research directions of the electro-peroxone technology in the wastewater field are proposed.The electro-peroxone process can offer a highly efficient and energy saving water treatment method to improve the performance of existing ozonation and electrochemical systems and has therefore become a promising electrochemical advanced oxidation process for wastewater treatment.展开更多
The elimination of neonicotinoids(NEOs)from water has been a research priority due to their threats to human health and ecosystems.In this study,we established the heterogeneous peroxymonosulfate(PMS)activation system...The elimination of neonicotinoids(NEOs)from water has been a research priority due to their threats to human health and ecosystems.In this study,we established the heterogeneous peroxymonosulfate(PMS)activation system using manganese catalyst(Mn NC)and cobalt catalyst(Co NC)to trigger the nonradical oxidation and synergistic oxidation pathway,respectively to remove NEOs.The results showed that the nonradical oxidation system exhibited superior NEOs degradation capability.The composition of organic pollutants in wastewater significantly impacted subsequent degradation processes.The charge distribution and reaction sites of various NEOs were analyzed using density functional theory(DFT)calculations,and it demonstrated the electron distribution and activity of NEOs were significantly influenced by the type and number of substituents.Nitro group(–NO_(2))and cyanide group(–C≡N)were identified as strong electron-withdrawing groups and prone to be attacked by negatively charged radicals.The transformation of NEOs was analyzed,and result showed that the C and N sites adjacent to the nitro group and cyanide group were more susceptible to oxidation attacks.S and N atoms,which possess strong electronegativity and high electron cloud density,were identified as key active sites in the degradation pathway.The outcomes of this study provide valuable guidance for the oriented regulation of oxidation pathways towards efficient removal of NEOs in water.展开更多
Pervoskite-type oxides LaFe_ 1-yCu_yO_3 was prepared by citrate method. Using a fluorescent Hg lamp as irradiator, the degradation experiments of acid red 3B were carried out in the suspension system of LaFe_ 1-yCu_yO...Pervoskite-type oxides LaFe_ 1-yCu_yO_3 was prepared by citrate method. Using a fluorescent Hg lamp as irradiator, the degradation experiments of acid red 3B were carried out in the suspension system of LaFe_ 1-yCu_yO_3. The results show that the doped oxides LaFe_ 1-yCu_yO_3 have good photocatalytic oxidation property. With the study of positron annihilation, its photocatalytic activity is mainly related with defect structures resulted by doping.展开更多
The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese oxides.Our work elab...The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese oxides.Our work elaborates,at the atomic level,through in-situ experimental and theoretical methods,the synergistic effects of two types of structural defect sites of Vo-e(edge-sharing oxygen)and Vo-c(corner-sharing oxygen)and MnO6 structural motifs of manganese oxides.Multi-dimensional manganese oxides,namely those with corner-connected MnOs structural motifs and Vo-c structural oxygen defect sites,significantly improved the activation of vinyl acetate.Enhancement of enol structure formation,acetate and formate intermediate species,and tautomerism between enol structure and acetaldehyde were detected when oxygen vacancies of manganese oxides were present in combination with corner/edge-connected MnO6.Moreover,the activation of chemical bonds and deep catalytic oxidation of vinyl acetate depend on the presence of a redox couple,surface oxygen species,and weakened Mn-O bonds.It provides a valuable notion for investigating and designing catalytic systems and reaction processes for the purpose of emission reduction and the management of environmental contaminants.展开更多
Nano-TiO2 photocatalytic oxidation was used to perform the advanced treatment of biologically treated chemical comprehensive wastewater. The effects of reaction time,nano-TiO2 dosage and initial p H of the wastewater ...Nano-TiO2 photocatalytic oxidation was used to perform the advanced treatment of biologically treated chemical comprehensive wastewater. The effects of reaction time,nano-TiO2 dosage and initial p H of the wastewater on the removal rate of COD were tested. The GC/MS and EEM techniques were used to qualitatively analyze organic compounds in the wastewater before and after treatment. The result showed that after the biologically treated chemical comprehensive wastewater was treated by nano-TiO2 photocatalytic oxidation under the conditions of reaction time 3 h,nano-TiO2 dosage 8 g/L,and pH 8. 0,the effluent COD was 61. 9 mg/L and its removal rate was 63. 8%. Additionally,the species of organic pollutants reduced from 12 to 6. Meanwhile,the content of humic-like and fulvic-like substances dropped dramatically.展开更多
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 Fundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn202211012)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.
基金the financial support from the Fundamental Research Funds for the Central Universities(No. xjj2016045)
文摘A series of spinel fe rrites magnetic nanopa rticles NiFe2 O4 we re synthesized as the heterogeneous Fentonlike catalyst by hydrothermal method and then NiFe2 O4@SiO2 catalysts were obtained by the modification of NiFe2 O4 via micro emulsion method.XRD,VSM,FTIR,SEM,TEM,BET and XPS were carried to analyze the difference between the above two catalysts.NiFe2 O4@SiO2 catalyst exhibited the higher catalytic activity than NiFe2 O4 for the degradation of Rhodamine B owe to the outer Si02 layers surface,the more important is both of them showed the better catalytic performance when at neutral pH environment.
基金the financial support,grants AGL2017-85603-P,PID2020-120281RB-100 and PID2020-117788RB-100 funded by MCIN/AEI/10,13039/501100011033grants SBPLY/21/180501/000111 and SBPLY/21/180501/000050 funded by JCCM by EU through Fondo Europeo de Desarrollo Regional+1 种基金supported by a UCLM scholarshipsupported by a JCCM scholarship
文摘Background Artificial insemination(AI)is a routine breeding technology in animal reproduction.Nevertheless,the temperature-sensitive nature and short fertile lifespan of ram sperm samples hamper its use in AI.In this sense,nanotechnology is an interesting tool to improve sperm protection due to the development of nanomaterials for AI,which could be used as delivery vehicles.In this work,we explored the feasibility of vitamin E nanoemulsion(NE)for improving sperm quality during transport.Results With the aim of evaluating this proposal,ejaculates of 7 mature rams of Manchega breed were collected by artificial vagina and extended to 60×10^(6)spz/mL in AndromedR.Samples containing control and NE(12 mmol/L)with and without exogenous oxidative stress(100μmol/L Fe2+/ascorbate)were stored at 22 and 15℃and motility(CASA),viability(YO-PRO/PI),acrosomal integrity(PNA-FITC/PI),mitochondrial membrane potential(Mitotracker Deep Red 633),lipoperoxidation(C11 BODIPY 581/591),intracellular reactive oxygen species(ROS)production and DNA status(SCSAR)monitored during 96 h.Our results show that NE could be used to maintain ram spermatozoa during transport at 15 and 22℃for up to 96 h,with no appreciable loss of kinematic and physiological characteristics of freshly collected samples.Conclusions The storage of ram spermatozoa in liquid form for 2-5 d with vitamin E nanoemulsions may lead more flexibility to breeders in AI programs.In view of the potential and high versatility of these nanodevices,further studies are being carried out to assess the proposed sperm preservation medium on fertility after artificial insemination.
基金supported by National Natural Science Foundation of China(No.52170086)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Natural science Foundation of Shaanxi province(No.2024JC-YBQN-0252)Special Scientific Research Project of Hanzhong City-Shaanxi University of Technology Co-construction State Key Laboratory(No.SXJ2106)。
文摘Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites,thus meeting fundamental requirements for practical application.The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts(SACs)prepared based on silicon-based materials(mesoporous silica,silicon-based minerals,and organosilicon materials)has unique advantages such as structural stability(especially important under strong oxidation conditions)and environmental protection.In this paper,the preparation strategies for the silicon-based SACs were assessed first,and the structural characteristics of various silicon-based SACs are systematically discussed,their application process and mechanism in Fenton-like process to achieve water purification are investigated,and the progress of Fenton-like process in density functional theory(DFT)of siliconbased derived single atom catalysts is summarized.In this paper,the preparation strategies and applications of silicon-based derived SACs are analyzed in depth,and their oxidation activities and pathways to different pollutants in water are reviewed.In addition,this paper also summarizes the device design and application of silicon-based derived SACs,and prospects the future development of silicon-based SACs in Fenton-like applications.
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.
文摘Precise manipulation of the catalytic spin configuration and delineation of the relationship between spin related properties and oxidation pathways remain significant challenges in Fenton-like processes.Herein,encapsulated cobalt nanoparticles and cobalt-nitrogen-doped carbon moieties,endowed with confinement effects and variations in shell curvature were constructed via straightforward pyrolysis strategies,inducing alterations in magnetic anisotropy,electronic energy levels and spin polarization.The enhanced spin polarization at cobalt sites leads to a reduction in crystal field splitting energy and an increase in electronic spin density.This phenomenon facilitated electron transfer from cobalt orbitals to pz orbitals of oxygen species within peroxymonosulfate molecules,thereby promoting the formation of high-valent cobalt species.The encapsulation effectively stabilized cobalt nanoparticles,mitigating their dissolution or deactivation during reactions,which in turn enhances stability and durability in continuous flow processes.The high-valent cobalt species within the shell exhibit increased exposure and generate localized high concentrations,thereby intensifying interactions with migrating pollutants and enabling efficient and selective oxidation of emerging compounds with elevated redox potentials.This work underscores the profound impact of confined encapsulation curvature and spin polarization characteristics of metal sites on catalytic oxidation pathways and performance,opening novel avenues for spin engineering in practical environmental catalysis.
基金Supported by the Self-raised Project for the Basic Research for Application of Yunnan Province(2013FZ109)the Follow-up Project of Qujing Normal University for the National Natural Science Foundation(2106512005)+1 种基金the Innovation and Entrepreneurship Project for College Students of Qujing Normal Universitythe Project for Innovation Team of the Applied Chemical Material Preparation of Qujing Normal University(2106531001)
文摘The photocatalytic degradation on the bismuth containing complex oxide was revised in detail including the synthesis and classification of photocatalyts, and then the photocatalytic reaction, scavenger, and the mechanism of reaction. In particular, the perspectives of photocatalytic degradation on the bismuth containing oxide were analyzed in detail.
基金Supported by Education Reform Project of Jiangxi Province(No.JXJG-20084-27)
文摘[ Objective] This study aimed to investigate enzymatic hydrolysis technology of glutinous rice and the oxidation resistance activity of the enzymatic hydrolysis solution. [ Method ] White glutinous rice was hydrolyzed using four kinds of proteases including neutral protease, alkaline protease, papain and trypsin. Using the scavenging rate of hydroxyl radical （ ·OH） as an indicator and appropriate protease as hydrolytic enzyme, the effects of protein substrate concentration, enzyme dosage, enzymatic hydrolysis temperature and initial pH on the abilities of proteases to scavenge hydroxyl radical from enzymatic hydrolysis solution of glutinous rice were investigated. Based on single-factor test, L9 （34） orthogonal experimental design was adopted, to determine the optimal enzymatic hydrolysis condi- tions leading to the highest oxidation resistance activity of enzymatic hydrolysis solution. [ Result] The optimized process parameters for enzymatic hydrolysis of glu- tinous rice protein with neutral protease were： protein substrate concentration of 2%, enzyme dosage of 24 000 U/g protein （protein meter）, enzymatic hydrolysis temperature of 55 ℃, initial pH of 8.0, and enzymatic hydrolysis duration of 0.5 h; under these conditions, the hydroxyl radical scavenging rate could reach 56. 05% ; protein substrate concentration, enzyme dosage, enzymatic hydrolysis temperature and initial pH had extremely significant effects on the hydroxyl radical scavenging rate. In addition, the activities of antioxidant peptides in glutinous rice hydrolysates were well maintained within a temperature range of 60 - 100℃. [Condusion] The study produced theoretical feasibility reference for the production of functional base powder by spray drying.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.60536030,61036002,60776024,60877035 and 61036009)National High Technology Research and Development Program of China(Grant Nos.2007AA04Z329 and 2007AA04Z254)
文摘A three-terminal silicon-based light emitting device is proposed and fabricated in standard 0.35 μm complementary metal-oxide-semiconductor technology. This device is capable of versatile working modes： it can emit visible to near infra-red （NIR） light （the spectrum ranges from 500 nm to 1000 nm） in reverse bias avalanche breakdown mode with working voltage between 8.35 V-12 V and emit NIR light （the spectrum ranges from 900 nm to 1300 nm） in the forward injection mode with working voltage below 2 V. An apparent modulation effect on the light intensity from the polysilicon gate is observed in the forward injection mode. Furthermore, when the gate oxide is broken down, NIR light is emitted from the polysilicon/oxide/silicon structure. Optoelectronic characteristics of the device working in different modes are measured and compared. The mechanisms behind these different emissions are explored.
文摘This article, for the first time, provides a novel advanced oxidation process based on sulfate radical （SO^4·-） to degrade organic pollutants in wastewater： microwave （MW）-activated persulfate oxidation （APO） with or without active carbon （AC）. Azo dye acid Orange 7 （AO7） is used as a model compound to investigate the high reactivity of MW-APO. It is found that AO7 （up to 1000 mg/L） is completely decolorized within 5-7 min under an 800 W MW furnace assisted-APO. In the presence of chloride ion （up to 0.50 mol/L）, the decolorization is still 100% completed, though delayed for about 1-2 min. Experiments are made to examine the enhancement by AC. It is exciting to find that the 100% decolorization of AO7 （500 mg/L） is achieved within 3 min by MW-APO using 1.0 g/L AC as catalyst, while the degradation efficiency maintains at 50% by MW energy without persulfate after about 5 min. Besides the destruction of visible light chromophore band of AO7 （484 nm）, during MW-APO, two bands in the ultraviolet region （228 nm and 310 nm） are rapidly broken down. The removal of COD is about 83%-95% for 500 mg/L AO7. SO^4·- is identified with quenching studies using specific alcohols. Both SO^4·- and ·OH could degrade AO7, but SO^4·- plays the dominant role. In a word, MW-APO AC is a new catalytic combustion technology for destruction of organic contamination even for high concentration.
基金This work was supported by the Natural Science Foundation of China(No.52100196)China Key Technologies R&D program(No.2021YFC3200700).
文摘Many studies have successfully built iron-mediatedmaterials to activate or catalyze Fentonlike reactions,with applications in water and wastewater treatment being investigated.However,the developed materials are rarely compared with each other regarding their performance of organic contaminant removal.In this review,the recent advances of Fentonlike processes in homogeneous and heterogeneous ways are summarized,especially the performance and mechanism of activators including ferrous iron,zero valent iron,iron oxides,iron-loaded carbon,zeolite,and metal organic framework materials.Also,this work mainly compares three O-O bond containing oxidants including hydrogen dioxide,persulfate,and percarbonate,which are environmental-friendly oxidants and feasible for in-situ chemical oxidation.The influence of reaction conditions,catalyst properties and benefits are analyzed and compared.In addition,the challenges and strategies of these oxidants in applications and the major mechanisms of the oxidation process have been discussed.This work can help understand the mechanistic insights of variable Fenton-like reactions,the role of emerging iron-based materials,and provide guidance for choosing appropriate technologies when facing real-world water and wastewater applications.
基金financially supported by the National Science Fund for Excellent Young Scholars of China (No. 52022111)the Distinguished Young Scholars of China (No. 51825403)the National Natural Science Foundation of China (Nos. 51634010, 51974379)。
文摘Between the two major arsenic-containing salts in natural water, arsenite(As(Ⅲ)) is far more harmful to human and the environment than arsenate(As(V)) due to its high toxicity and transportability. Therefore, preoxidation of As(Ⅲ) to As(V) is considered to be an effective means to reduce the toxicity of arsenic and to promote the removal efficiency of arsenic. Due to their high catalytic activity and arsenic affinity, iron-based functional materials can quickly oxidize As(Ⅲ) to As(V) in heterogeneous Fenton-like systems, and then remove As(V) from water through adsorption and surface coprecipitation. In this review, the effects of different iron-based functional materials such as zero-valent iron and iron(hydroxy) oxides on arsenic removal are compared, and the catalytic oxidation mechanism of As(Ⅲ) in heterogeneous Fenton process is further clarified. Finally, the main challenges and opportunities faced by iron-based As(Ⅲ) oxidation functional materials are prospected.
基金This work was financially supported by the National Key R&D Program of China(2017YFB0601904).
文摘Changes are needed to improve the efficiency and lower the CO_(2)emissions of traditional coal-fired power generation,which is the main source of global CO_(2)emissions.The integrated gasification fuel cell(IGFC)process,which combines coal gasification and high-temperature fuel cells,was proposed in 2017 to improve the efficiency of coal-based power generation and reduce CO_(2)emissions.Supported by the National Key R&D Program of China,the IGFC for nearzero CO_(2)emissions program was enacted with the goal of achieving near-zero CO_(2)emissions based on(1)catalytic combustion of the flue gas from solid oxide fuel cell(SOFC)stacks and(2)CO_(2)conversion using solid oxide electrolysis cells(SOECs).In this work,we investigated a kW-level catalytic combustion burner and SOEC stack,evaluated the electrochemical performance of the SOEC stack in H2O electrolysis and H2O/CO_(2)co-electrolysis,and established a multiscale and multi-physical coupling simulation model of SOFCs and SOECs.The process developed in this work paves the way for the demonstration and deployment of IGFC technology in the future.
基金the financial support provided by the National Natural Science Foundation of China(No.21306175)the Zhejiang Provincial Natural Science Foundation of China(No.LGJ18E080001)+1 种基金the Project of Science and Technology Department of Jiashan(Nos.2020D02 and 2022A23)Zhejiang Province(No.2015C03017)。
文摘The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared with electrochemical oxidation technology,ozonation technology,and traditional peroxone technology.Due to the high kinetics of pollutant degradation,the electro-peroxone process can reduce the reaction time and energy consumption of pollutant treatment in wastewater.The electroperoxone technology can promote pollutant degradation and mineralization,which shows obvious synergistic effects of electrochemical oxidation and ozonation for wastewater treatment.Most importantly,the research mechanism of the electro-peroxone technology is systematically introduced from two aspects of cathode reaction and bulk reaction.The influence of experimental parameters on the wastewater treatment effect is also discussed.Finally,the potential applications and future research directions of the electro-peroxone technology in the wastewater field are proposed.The electro-peroxone process can offer a highly efficient and energy saving water treatment method to improve the performance of existing ozonation and electrochemical systems and has therefore become a promising electrochemical advanced oxidation process for wastewater treatment.
基金funded by National Natural Science Foundation of China(No.42177382)。
文摘The elimination of neonicotinoids(NEOs)from water has been a research priority due to their threats to human health and ecosystems.In this study,we established the heterogeneous peroxymonosulfate(PMS)activation system using manganese catalyst(Mn NC)and cobalt catalyst(Co NC)to trigger the nonradical oxidation and synergistic oxidation pathway,respectively to remove NEOs.The results showed that the nonradical oxidation system exhibited superior NEOs degradation capability.The composition of organic pollutants in wastewater significantly impacted subsequent degradation processes.The charge distribution and reaction sites of various NEOs were analyzed using density functional theory(DFT)calculations,and it demonstrated the electron distribution and activity of NEOs were significantly influenced by the type and number of substituents.Nitro group(–NO_(2))and cyanide group(–C≡N)were identified as strong electron-withdrawing groups and prone to be attacked by negatively charged radicals.The transformation of NEOs was analyzed,and result showed that the C and N sites adjacent to the nitro group and cyanide group were more susceptible to oxidation attacks.S and N atoms,which possess strong electronegativity and high electron cloud density,were identified as key active sites in the degradation pathway.The outcomes of this study provide valuable guidance for the oriented regulation of oxidation pathways towards efficient removal of NEOs in water.
文摘Pervoskite-type oxides LaFe_ 1-yCu_yO_3 was prepared by citrate method. Using a fluorescent Hg lamp as irradiator, the degradation experiments of acid red 3B were carried out in the suspension system of LaFe_ 1-yCu_yO_3. The results show that the doped oxides LaFe_ 1-yCu_yO_3 have good photocatalytic oxidation property. With the study of positron annihilation, its photocatalytic activity is mainly related with defect structures resulted by doping.
基金financially supported by the National Natural Science Foundation of China(No.22006079)the R&D Program of Beijing Municipal Education Commission(No.KjzD20191443001)+2 种基金the National Key Research and Development Program of China(No.2016YFC0204203)the Project of Ningxia Key Research and Development Plan(No.2020BEB04009)National First-rate Discipline Construction Project of Ningxia(No.NXYLXK2017A04).
文摘The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese oxides.Our work elaborates,at the atomic level,through in-situ experimental and theoretical methods,the synergistic effects of two types of structural defect sites of Vo-e(edge-sharing oxygen)and Vo-c(corner-sharing oxygen)and MnO6 structural motifs of manganese oxides.Multi-dimensional manganese oxides,namely those with corner-connected MnOs structural motifs and Vo-c structural oxygen defect sites,significantly improved the activation of vinyl acetate.Enhancement of enol structure formation,acetate and formate intermediate species,and tautomerism between enol structure and acetaldehyde were detected when oxygen vacancies of manganese oxides were present in combination with corner/edge-connected MnO6.Moreover,the activation of chemical bonds and deep catalytic oxidation of vinyl acetate depend on the presence of a redox couple,surface oxygen species,and weakened Mn-O bonds.It provides a valuable notion for investigating and designing catalytic systems and reaction processes for the purpose of emission reduction and the management of environmental contaminants.
文摘Nano-TiO2 photocatalytic oxidation was used to perform the advanced treatment of biologically treated chemical comprehensive wastewater. The effects of reaction time,nano-TiO2 dosage and initial p H of the wastewater on the removal rate of COD were tested. The GC/MS and EEM techniques were used to qualitatively analyze organic compounds in the wastewater before and after treatment. The result showed that after the biologically treated chemical comprehensive wastewater was treated by nano-TiO2 photocatalytic oxidation under the conditions of reaction time 3 h,nano-TiO2 dosage 8 g/L,and pH 8. 0,the effluent COD was 61. 9 mg/L and its removal rate was 63. 8%. Additionally,the species of organic pollutants reduced from 12 to 6. Meanwhile,the content of humic-like and fulvic-like substances dropped dramatically.
