Carbon-doped copper ferrite(C–CuFe_(2)O_(4))was synthesized by a simple two-step hydrothermal method,which showed enhanced tetracycline hydrochloride(TCH)removal efficiency as compared to the pure CuFe_(2)O_(4) in Fe...Carbon-doped copper ferrite(C–CuFe_(2)O_(4))was synthesized by a simple two-step hydrothermal method,which showed enhanced tetracycline hydrochloride(TCH)removal efficiency as compared to the pure CuFe_(2)O_(4) in Fenton-like reaction.A removal efficiency of 94%was achieved with 0.2 g L^(-1) catalyst and 20 mmol L^(-1) H_(2)O_(2) within 90 min.We demonstrated that 5%C–CuFe_(2)O_(4) catalyst in the presence of H_(2)O_(2) was significantly efficient for TCH degradation under the near-neutral pH(5–9)without buffer.Multiple techniques,including SEM,TEM,XRD,FTIR,Raman,XPS M€ossbauer and so on,were conducted to investigate the structures,morphologies and electronic properties of as-prepared samples.The introduction of carbon can effectively accelerate electron transfer by cooperating with Cu and Fe to activate H_(2)O_(2) to generate·OH and·O_(2)^(-).Particularly,theoretical calculations display that the p,p,d orbital hybridization of C,O,Cu and Fe can form C–O–Cu and C–O–Fe bonds,and the electrons on carbon can transfer to metal Cu and Fe along the C–O–Fe and C–O–Cu channels,thus forming electron-rich reactive centers around Fe and Cu.This work provides lightful reference for the modification of spinel ferrites in Fenton-like application.展开更多
To overcome the ever-growing organic pollutions in the water system,abundant efforts have been dedicated to fabricating efficient Fenton-like carbon catalysts.However,the rational design of carbon catalysts with high ...To overcome the ever-growing organic pollutions in the water system,abundant efforts have been dedicated to fabricating efficient Fenton-like carbon catalysts.However,the rational design of carbon catalysts with high intrinsic activity remains a long-term goal.Herein,we report a new N-molecule-assisted self-catalytic carbonization process in augmenting the intrinsic Fenton-like activity of metal-organic-framework-derived carbon hybrids.During carbonization,the N-molecules provide alkane/ammonia gases and the formed iron nanocrystals act as the in situ catalysts,which result in the elaborated formation of carbon nanotubes(in situ chemical vapor deposition from alkane/iron catalysts)and micro-/meso-porous structures(ammonia gas etching).The obtained catalysts exhibited with abundant Fe/Fe-Nx/pyridinic-N active species,micro-/meso-porous structures,and conductive carbon nanotubes.Consequently,the catalysts exhibit high efficiency toward the degradation of different organic pollutions,such as bisphenol A,methylene blue,and tetracycline.This study not only creates a new pathway for achieving highly active Fenton-like carbon catalysts but also takes a step toward the customized production of advanced carbon hybrids for diverse energy and environmental applications.展开更多
The sluggish kinetics of Fe(Ⅱ)recovery in Fenton/Fenton-like reactions significantly limits the oxidation efficiency.In this study,we for the first time use boron carbide(BC)as a green and stable promotor to enhance ...The sluggish kinetics of Fe(Ⅱ)recovery in Fenton/Fenton-like reactions significantly limits the oxidation efficiency.In this study,we for the first time use boron carbide(BC)as a green and stable promotor to enhance the reaction of Fe(Ⅲ)/H_(2)O_(2) for degradation of diverse organic pollutants.Electron paramagnetic resonance analysis and chemical quenching/capturing experiments demonstrate that hydroxyl radicals(·OH)are the primary reactive species in the BC/Fe(Ⅲ)/H_(2)O_(2) system.In situ electrochemical analysis indicates that BC remarkably boosts the Fe(Ⅲ)/Fe(Ⅱ)redox cycles,where the adsorbed Fe(Ⅲ)cations were transformed to more active Fe(Ⅲ)species with a higher oxidative potential to react with H_(2)O_(2) to produce Fe(Ⅱ).Thus,the recovery of Fe(Ⅱ)from Fe(Ⅲ)is facilitated over BC surface,which enhancesOH generation via Fenton reactions.Moreover,BC exhibits outstanding reusability and stability in successive cycles and avoids the secondary pollution caused by conventional organic and metalliferous promotors.Therefore,metal-free BC boosting Fe(Ⅲ)/H_(2)O_(2) oxidation of organics provides a green and advanced strategy for water decontamination.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
Fabrication of single atom catalysts(SACs)by a green and gentle method is important for their practical Fenton-like use.In this work,a high effective iron-based catalyst was prepared from the iron-rich Enteromorpha fo...Fabrication of single atom catalysts(SACs)by a green and gentle method is important for their practical Fenton-like use.In this work,a high effective iron-based catalyst was prepared from the iron-rich Enteromorpha for NPX degradation via peroxymonosulfate(PMS).Both Fe-SACs and iron-clusters was fabricated from the intrinsic iron element in Enteromorpha after the urea saturation.The Fe-SACs/clusters can achieve 100%of NPX oxidation within 20 min with the k_(obs)of 0.282 min^(-1).Quenching tests indicated that the radical pathways were not dominated in the catalytic systems,and strong electron transfer process can be induced in the Fe-SACs/clusters+PMS system by using the NPX as electron donor and FeSACs/clusters/PMS^*complexes as electron acceptor.This result was consistent with the phenomenon observed in the galvanic oxidation system.In addition,the Fe-SACs/clusters was deposited onto the ceramic membrane(CM)by the spraying-crosslinking process to form a Fe-SACs/clusters@CM,which showed an effective and continuous NPX degradation in a heterogeneous PMS system.展开更多
Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many reactions.The widely adopted wet chemi...Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many reactions.The widely adopted wet chemistry approach uses intercalating entities especially alkali metal ions to achieve the phase transition;however,these entities are normally inert for the target reaction.Here,we describe the first use of iron atoms for the intercalation of 2H-MoS_(2) layers,driving the partial transition from 2H to 1T phase.Interestingly,in the peroxymonosulfate(PMS)-based Fenton-like reactions,the interlayered confinement of Fe atoms not only activates the inert basal plane,but also adds more reactive Fe sites for the formation of metal-PMS complex as primary reactive species for pollutant removal.In the degradation of a model pollutant carbamazepine(CBZ),the Fe-intercalated MoS_(2) exhibits a first order rate constant 13.3 times higher than 2H-MoS_(2).This strategy is a new direction for manipulating the phase composition and boosting the catalytic reactivity of MoS_(2)-based catalysts in various scenarios,including environmental remediation and energy applications.展开更多
In this work,Fe_(3)O_(4) nanoparticles(NPs)loaded inside and outside halloysite nanotubes(HNTs)were prepared and developed as the heterogeneous Fenton-like catalysts for the removal of representative organic pollutant...In this work,Fe_(3)O_(4) nanoparticles(NPs)loaded inside and outside halloysite nanotubes(HNTs)were prepared and developed as the heterogeneous Fenton-like catalysts for the removal of representative organic pollutants.Characterization results indicated that the samples with Fe_(3)O_(4) NPs loaded outside the HNTs lumen(Fe_(3)O_(4)/HNTs)and inside the HNTs lumen(Fe_(3)O_(4)@HNTs)were successfully prepared.Both samples had typical magnetic hysteresis loops,while Fe_(3)O_(4)@HNTs exhibited higher magnetization intensity.The comparative experiments showed that Fe_(3)O_(4)@HNTs had better Fenton-like catalytic ability than that of Fe_(3)O_(4)/HNTs in the degradation of various organic pollutants.Taking Rhodamine B(RhB)as an example,the adsorption thermodynamics and kinetics of RhB onto Fe_(3)O_(4)/HNTs and Fe_(3)O_(4)@HNTs were also investigated.The comparative results demonstrated that the adsorption ability of Fe_(3)O_(4)/HNTs was better than that of Fe_(3)O_(4)@HNTs.Moreover,the dissolved concentration of Fe^(2+)and production amount of hydroxyl radical(·OH)in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system were significantly higher than those in the Fe_(3)O_(4)/HNTs-H_(2)O_(2) system.Based on aforementioned comparison,the nano-confinement effect in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system was verified.This work provides meaningful guidance for the cheap and convenient design of nanoreactors for Fenton-like applications.展开更多
High energy consumption has seriously hindered the development of Fenton-like reactions for the removal of refractory organic pollutants in water.To solve this problem,we designed a novel Fenton-like catalyst(Cu-PAN3)...High energy consumption has seriously hindered the development of Fenton-like reactions for the removal of refractory organic pollutants in water.To solve this problem,we designed a novel Fenton-like catalyst(Cu-PAN3)by coprecipitation and carbon thermal reduction.The catalyst exhibits excellent Fenton-like catalytic activity and stability for the degradation of various pollutants with low H_(2)O_(2)consumption.The experimental results indicate that the dual reaction centers(DRCs)are composed of Cu-N-C and Cu-O-C bridges between copper and graphene-like carbon,which form electron-poor/rich centers on the catalyst surface.H_(2)O_(2)is mainly reduced at electron-rich Cu centers to free radicals for pollutant degradation.Meanwhile,pollutants can be oxidized by donating electrons to the electron-poor C centers of the catalyst,which inhibits the ineffective decomposition of H_(2)O_(2)at the electron-poor centers.This therefore significantly reduces the consumption of H_(2)O_(2)and reduces energy consumption.展开更多
Herein,a diatomite biomorphic Si-O doped carbon-based catalyst(DB-SiOC)was prepared using natura mineral diatomite as the silicon source and porous template.The results showed that the metal-free DB SiOC catalyst exhi...Herein,a diatomite biomorphic Si-O doped carbon-based catalyst(DB-SiOC)was prepared using natura mineral diatomite as the silicon source and porous template.The results showed that the metal-free DB SiOC catalyst exhibited ultrafast oxidation towards chlorophenol(CP)via peroxymonosulfate(PMS)activa tion,which was almost one order of magnitudes than most of carbon-based catalysts.The DB-SiOC/PMS system also showed the high ability to resist the interference of environmental matrix.The radicals(^(·)OH and SO_(4)^(·–))exhibited a very small contribution to the CP oxidation while the electron transfer processe(ETP)played the major role in the DB-SiOC/PMS system.The electron shuttles from the electron-donating CP molecules to the adjacent DB-SiOC/PMS^(*)could be efficiently triggered via Si-O bonds as bridges,mak ing it possible for ultrafast oxidation of CP.In addition,the hollow-disc shaped DB-Si OC provided the biomorphic DE structures with abundant pores for enriching the PMS and pollutants,thus further ac celerating the oxidation reaction.This work provided a new routine for the fabrication of Si-O doped carbon-based catalysts with excellent Fenton-like catalytic activity,which would greatly promote thei application prospects in Fenton-like systems.展开更多
As other natural iron-bearing minerals, schorl could be taken as an effective iron source for degradation of organic pollutants by mineral-catalyzed Fenton-like system. In our present study, the schorl-catalyzed Fento...As other natural iron-bearing minerals, schorl could be taken as an effective iron source for degradation of organic pollutants by mineral-catalyzed Fenton-like system. In our present study, the schorl-catalyzed Fenton-like system has been successfully developed for discoloration of an active commercial dye, Rhodamine B (RhB), in an aqueous solution. Through a number of batch discoloration experiments under various conditions, it was found that the reactivity of the system increased by, respectively, increasing schorl dosage, temperature, hydrogen peroxide starting concentration and by decreasing the pH. Over 90% of discoloration ratio could be gained in less than 30 min, and nearly 70% of total organic carbon (TOC) could be removed in less than 200 min. And, the schorl catalyst could be repeatedly used at least ten times, still with high catalytic activity. Comparative studies indicated that the RhB discoloration ratios were much higher in presence of schorl and H2O2 than those in presence of schorl or H2O2 only, which suggested that the schorl-catalyzed Fenton-like reaction governed the RhB discoloration process. The content of Fe ion leaching in the solution was also measured using inductively coupling plasma-atomic emission spectra (ICP-AES). A mechanism proposed herein suggested that adsorption and Fenton-like reaction (heterogeneous and homogeneous) were responsible for the discoloration of RhB.展开更多
In the pursuit of heterogeneous catalysts with high reactivity,metal organic framework(MOF)nanomaterials have received tremendous attentions.However,many MOF catalysts especially Fe-based MOFs need to be utilized imme...In the pursuit of heterogeneous catalysts with high reactivity,metal organic framework(MOF)nanomaterials have received tremendous attentions.However,many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature,because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules.Here,we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel(GA),generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use.Compared to MIL-101-Fe,GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction,attributing to smaller MIL-101-Fe particle size,presence of active Fe(II)sites,and abundant defects in GA.Strikingly,the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature,by resisting the entrance of water molecules and helping to exclude water molecules.This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component,but also overcome its intrinsic drawback by taking advantage of the properties of host.We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.展开更多
As a new water treatment technology,Fenton-like reaction has great potential.In this study,we successfully prepared an excellent Fenton-like catalyst,which is composed of cobalt monoatoms and asymmetric subnanocluster...As a new water treatment technology,Fenton-like reaction has great potential.In this study,we successfully prepared an excellent Fenton-like catalyst,which is composed of cobalt monoatoms and asymmetric subnanoclusters(labeled CoSA/Clu-C_(2)N),and exhibits excellent peroxymonosulfate(PMS)activation reactivity.By directly comparing the catalytic properties of CoSA-C_(2)N and CoSA/Clu-C_(2)N,the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were investigated.The results showed that CoSA/Clu-C_(2)N had higher degradation rates of carbamazepine(CBZ),antipyrine(AT)and chlorobenzoic acid(CA)when combined with active oxidant PMS.The cyclic frequency of CBZ was 5.4 min^(-1),which was twice as high as the catalytic constant of CoSA-C_(2)N(2.4 min^(-1)).The results show that CoSA/Clu-C_(2)N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in water.In addition,electron paramagnetic resonance(EPR)technology has proved that the introduction of Co subnano clusters in CoSA/Clu-C_(2)N is conducive to the production of singlet oxygen(1O_(2)),thereby improving the efficiency of pollutant oxidation.This work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.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
Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising...Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent ^(1)O_(2) mediated Fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H_(2)O_(2), but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0×10^(-8) mol/L to 1.0×10^(-5) mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring Fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.展开更多
Identifying the active site of oxide-supported metal catalysts and revealing the intrinsic synergistic mechanism between metal and oxide support remain a large challenge.Herein,we report the identification and separat...Identifying the active site of oxide-supported metal catalysts and revealing the intrinsic synergistic mechanism between metal and oxide support remain a large challenge.Herein,we report the identification and separation of the Pt-O-Ti interface and TiO_(2) surface in Pt-TiO_(2)-based catalysts by depositing different thickness of TiO_(2) shell with∼0.4-nm micropores onto the surface of Pt/TiO_(2) catalyst through atomic layer deposition(ALD).In the oxidation of 3,3′,5,5′-tetramethylbenzidine(TMB)by hydrogen peroxide(H_(2)O_(2))process,the TiO_(2) microporous shells can prevent the contact between TMB and embedded Pt clusters,but not delay the diffusion of H_(2)O_(2).The heterolysis of H_(2)O_(2) to ·OH occurs on the Pt-O-Ti interface,and the generated•OH migrates to the TiO_(2) surface to supplement the surface lattice oxygen,which sequentially oxidizes TMB to oxTMB.And the synergistic effect between Pt-O-Ti interface active sties and TiO_(2) surface active sites can significantly improve the catalytic performance.Our study provides a guide for the understanding of the intrinsic synergistic mechanism between the metal and oxide support in the metal-oxide catalysts.展开更多
Photocatalysis and Fenton process are two primary and promising advanced oxidation processes to degrade organic pollutants.However,the practical applications of single photocatalysis and Fenton process are still limit...Photocatalysis and Fenton process are two primary and promising advanced oxidation processes to degrade organic pollutants.However,the practical applications of single photocatalysis and Fenton process are still limited.Introducing one of them into another to form a combined photocatalytic Fentonlike system has shown great potential but still faces challenges in designing a well-tailored catalyst.Herein,a confined photocatalytic Fenton-like micro-reactor catalyst with a movable Fe_(3) O_(4) core and a mesoporous TiO_(2) shell has been constructed via a successive Stober coating strategy,followed by an ultrasound assisted etching method.The resulting micro-reactor possesses well-defined yolk-shell structures with unifo rm mesopores(~4 nm),a large Brunauer-Emmett-Teller(BET) surface area(~166.7 m^(2)/g),a high pore volume(~0.56 cm^(3)/g) and a strong magnetization(~51 emu/g),as well as tunable reactor sizes(20-90 nm).When evaluated for degrading bisphenol A under solar light in the presence of peroxymo no sulfate,the micro-reactor exhibits a superior catalytic degradation perfo rmance with a high magnetic separation efficiency and an excellent recycle ability.The outstanding performance can be attributed to its unique textual structure,which leads to a great syne rgistic effect from the photocatalytic and Fenton-like process.This study gives an important insight into the design and synthesis of an advanced micro-reactor for a combined advanced oxidation processes(AOPs).展开更多
A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and cryst...A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.展开更多
Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF d...Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF degradation by the combined process of zero-valent iron nanoparticles(nZVI)and nano calcium peroxide(nCaO_(2))were performed.A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO_(2)nanoparticles and pH value on the DCF removal.In the meantime,the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO_(2)nanoparticles in the reaction system.The results show that the nZVI/nCaO_(2)can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO_(2)added,resulting in a removal rate of greater than 90%in a 2-hour reaction with an initial pH of 5.The degradation rate of DCF was positively correlated with the dosage of nCaO_(2),and negatively correlated with both nZVI dosage and the initial pH value.The order of significance of the three factors is identified as pH value>nZVI dosage>nCaO_(2)dosage.In the continuous-flow reaction system,the DCF removal rates remained above 75%within 150 minutes at the pH of 5,with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO_(2).These results provide a theoretical basis for the nZVI/nCaO_(2)application to remove DCF in groundwater.展开更多
This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brothe...This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brother" was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/"water-brother" interfaces are very different from water/oil interfaces. The "water-brother" solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多展开更多
In this study,a magnetic P zeolite was directly synthesized by utilization of industrial solid wastes of zinc slag(ZS)and circulating fluidized bed fly ash(CFBFA)via one-step hydrothermal method.The effects of differe...In this study,a magnetic P zeolite was directly synthesized by utilization of industrial solid wastes of zinc slag(ZS)and circulating fluidized bed fly ash(CFBFA)via one-step hydrothermal method.The effects of different CFBFA/ZS ratios and hydrothermal times on the as-synthesized zeolite were investigated.The X-ray diffraction(XRD)and vibrating sample magnetometer(VSM)results indicated that the magnetic P zeolite possessed well-defined crystals and superparamagnetism.The as-prepared zeolite was employed as a Fenton-like solid catalyst for degradation of direct green B dye wastewater.It was discovered that the magnetic P zeolite took the advantage of rapid separation and efficient recovery under the external magnets in a solid-liquid reaction.The effects of the solution pH,the catalyst dosage,and the H_(2)O_(2)concentration on the degradation rate of direct green B dye wastewater were studied systematically.The results showed that the highest degradation of 96.3%was obtained and the magnetic P zeolite showed excellent stability after four cycles.Therefore,the magnetic P zeolite derived from industrial solid wastes had a potential application in wastewater treatment.展开更多
基金supported by the Program for the National Natural Science Foundation of China(52070077,51879101,51779090)the National Program for Support of Top-Notch Young Professionals of China(2014)+1 种基金the Program for Changjiang Scholars and Innovative Research Team in University(IRT-13R17)Natural Science Foundation of Hunan Province(2022JJ20013,2021JJ40098).
文摘Carbon-doped copper ferrite(C–CuFe_(2)O_(4))was synthesized by a simple two-step hydrothermal method,which showed enhanced tetracycline hydrochloride(TCH)removal efficiency as compared to the pure CuFe_(2)O_(4) in Fenton-like reaction.A removal efficiency of 94%was achieved with 0.2 g L^(-1) catalyst and 20 mmol L^(-1) H_(2)O_(2) within 90 min.We demonstrated that 5%C–CuFe_(2)O_(4) catalyst in the presence of H_(2)O_(2) was significantly efficient for TCH degradation under the near-neutral pH(5–9)without buffer.Multiple techniques,including SEM,TEM,XRD,FTIR,Raman,XPS M€ossbauer and so on,were conducted to investigate the structures,morphologies and electronic properties of as-prepared samples.The introduction of carbon can effectively accelerate electron transfer by cooperating with Cu and Fe to activate H_(2)O_(2) to generate·OH and·O_(2)^(-).Particularly,theoretical calculations display that the p,p,d orbital hybridization of C,O,Cu and Fe can form C–O–Cu and C–O–Fe bonds,and the electrons on carbon can transfer to metal Cu and Fe along the C–O–Fe and C–O–Cu channels,thus forming electron-rich reactive centers around Fe and Cu.This work provides lightful reference for the modification of spinel ferrites in Fenton-like application.
基金supported by the National Key R&D Program of China(2019YFA0110600 and 2019YFA0110601)National Natural Science Foundation of China(Nos.51603134,51903178,51803134,and 51703141)+1 种基金Sichuan Province’s Science and Technology Planning Project(No.2016GZ0350)the Postgraduate Course Construction Project of Sichuan University(No.2017KCSJ036)and for their financial support.
文摘To overcome the ever-growing organic pollutions in the water system,abundant efforts have been dedicated to fabricating efficient Fenton-like carbon catalysts.However,the rational design of carbon catalysts with high intrinsic activity remains a long-term goal.Herein,we report a new N-molecule-assisted self-catalytic carbonization process in augmenting the intrinsic Fenton-like activity of metal-organic-framework-derived carbon hybrids.During carbonization,the N-molecules provide alkane/ammonia gases and the formed iron nanocrystals act as the in situ catalysts,which result in the elaborated formation of carbon nanotubes(in situ chemical vapor deposition from alkane/iron catalysts)and micro-/meso-porous structures(ammonia gas etching).The obtained catalysts exhibited with abundant Fe/Fe-Nx/pyridinic-N active species,micro-/meso-porous structures,and conductive carbon nanotubes.Consequently,the catalysts exhibit high efficiency toward the degradation of different organic pollutions,such as bisphenol A,methylene blue,and tetracycline.This study not only creates a new pathway for achieving highly active Fenton-like carbon catalysts but also takes a step toward the customized production of advanced carbon hybrids for diverse energy and environmental applications.
基金support to visit The University of Adelaide from the China Scholarship Council(No.201906240037).
文摘The sluggish kinetics of Fe(Ⅱ)recovery in Fenton/Fenton-like reactions significantly limits the oxidation efficiency.In this study,we for the first time use boron carbide(BC)as a green and stable promotor to enhance the reaction of Fe(Ⅲ)/H_(2)O_(2) for degradation of diverse organic pollutants.Electron paramagnetic resonance analysis and chemical quenching/capturing experiments demonstrate that hydroxyl radicals(·OH)are the primary reactive species in the BC/Fe(Ⅲ)/H_(2)O_(2) system.In situ electrochemical analysis indicates that BC remarkably boosts the Fe(Ⅲ)/Fe(Ⅱ)redox cycles,where the adsorbed Fe(Ⅲ)cations were transformed to more active Fe(Ⅲ)species with a higher oxidative potential to react with H_(2)O_(2) to produce Fe(Ⅱ).Thus,the recovery of Fe(Ⅱ)from Fe(Ⅲ)is facilitated over BC surface,which enhancesOH generation via Fenton reactions.Moreover,BC exhibits outstanding reusability and stability in successive cycles and avoids the secondary pollution caused by conventional organic and metalliferous promotors.Therefore,metal-free BC boosting Fe(Ⅲ)/H_(2)O_(2) oxidation of organics provides a green and advanced strategy for water decontamination.
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supported by National Natural Science Foundation of China(No.52170086)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Fabrication of single atom catalysts(SACs)by a green and gentle method is important for their practical Fenton-like use.In this work,a high effective iron-based catalyst was prepared from the iron-rich Enteromorpha for NPX degradation via peroxymonosulfate(PMS).Both Fe-SACs and iron-clusters was fabricated from the intrinsic iron element in Enteromorpha after the urea saturation.The Fe-SACs/clusters can achieve 100%of NPX oxidation within 20 min with the k_(obs)of 0.282 min^(-1).Quenching tests indicated that the radical pathways were not dominated in the catalytic systems,and strong electron transfer process can be induced in the Fe-SACs/clusters+PMS system by using the NPX as electron donor and FeSACs/clusters/PMS^*complexes as electron acceptor.This result was consistent with the phenomenon observed in the galvanic oxidation system.In addition,the Fe-SACs/clusters was deposited onto the ceramic membrane(CM)by the spraying-crosslinking process to form a Fe-SACs/clusters@CM,which showed an effective and continuous NPX degradation in a heterogeneous PMS system.
基金support from the National Natural Science Foundation of China(Nos.22276095,22106071,and 81801029)the Natural Science Foundation of Jiangsu Province(Nos.BK20211522 and BK20200504)the Project of Jiangsu Provincial Commission of Health(No.M2022060).We gratefully acknowledge HZWTECH for providing computation facilities.
文摘Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many reactions.The widely adopted wet chemistry approach uses intercalating entities especially alkali metal ions to achieve the phase transition;however,these entities are normally inert for the target reaction.Here,we describe the first use of iron atoms for the intercalation of 2H-MoS_(2) layers,driving the partial transition from 2H to 1T phase.Interestingly,in the peroxymonosulfate(PMS)-based Fenton-like reactions,the interlayered confinement of Fe atoms not only activates the inert basal plane,but also adds more reactive Fe sites for the formation of metal-PMS complex as primary reactive species for pollutant removal.In the degradation of a model pollutant carbamazepine(CBZ),the Fe-intercalated MoS_(2) exhibits a first order rate constant 13.3 times higher than 2H-MoS_(2).This strategy is a new direction for manipulating the phase composition and boosting the catalytic reactivity of MoS_(2)-based catalysts in various scenarios,including environmental remediation and energy applications.
基金supported by the Natural Science Foundation of Heilongjiang Province,China(Grant No.LH2022E083).
文摘In this work,Fe_(3)O_(4) nanoparticles(NPs)loaded inside and outside halloysite nanotubes(HNTs)were prepared and developed as the heterogeneous Fenton-like catalysts for the removal of representative organic pollutants.Characterization results indicated that the samples with Fe_(3)O_(4) NPs loaded outside the HNTs lumen(Fe_(3)O_(4)/HNTs)and inside the HNTs lumen(Fe_(3)O_(4)@HNTs)were successfully prepared.Both samples had typical magnetic hysteresis loops,while Fe_(3)O_(4)@HNTs exhibited higher magnetization intensity.The comparative experiments showed that Fe_(3)O_(4)@HNTs had better Fenton-like catalytic ability than that of Fe_(3)O_(4)/HNTs in the degradation of various organic pollutants.Taking Rhodamine B(RhB)as an example,the adsorption thermodynamics and kinetics of RhB onto Fe_(3)O_(4)/HNTs and Fe_(3)O_(4)@HNTs were also investigated.The comparative results demonstrated that the adsorption ability of Fe_(3)O_(4)/HNTs was better than that of Fe_(3)O_(4)@HNTs.Moreover,the dissolved concentration of Fe^(2+)and production amount of hydroxyl radical(·OH)in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system were significantly higher than those in the Fe_(3)O_(4)/HNTs-H_(2)O_(2) system.Based on aforementioned comparison,the nano-confinement effect in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system was verified.This work provides meaningful guidance for the cheap and convenient design of nanoreactors for Fenton-like applications.
基金supported by the National Natural Science Foundation of China(Nos.52150056,51838005,and 52100032)the Introduced Innovative R&D Team Project under the“Pearl River Talent Recruitment Program”of Guangdong Province(No.2019ZT08L387)+1 种基金the Special Basic Research Fund for Central Public Research Institutes of China(No.PMzx703-202204-152)the support from the BL14W1 beamline of Shanghai Synchrotron Radiation Facility(SSRF,China)。
文摘High energy consumption has seriously hindered the development of Fenton-like reactions for the removal of refractory organic pollutants in water.To solve this problem,we designed a novel Fenton-like catalyst(Cu-PAN3)by coprecipitation and carbon thermal reduction.The catalyst exhibits excellent Fenton-like catalytic activity and stability for the degradation of various pollutants with low H_(2)O_(2)consumption.The experimental results indicate that the dual reaction centers(DRCs)are composed of Cu-N-C and Cu-O-C bridges between copper and graphene-like carbon,which form electron-poor/rich centers on the catalyst surface.H_(2)O_(2)is mainly reduced at electron-rich Cu centers to free radicals for pollutant degradation.Meanwhile,pollutants can be oxidized by donating electrons to the electron-poor C centers of the catalyst,which inhibits the ineffective decomposition of H_(2)O_(2)at the electron-poor centers.This therefore significantly reduces the consumption of H_(2)O_(2)and reduces energy consumption.
基金supported by National Natural Science Foundation of China(No.52170086)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Herein,a diatomite biomorphic Si-O doped carbon-based catalyst(DB-SiOC)was prepared using natura mineral diatomite as the silicon source and porous template.The results showed that the metal-free DB SiOC catalyst exhibited ultrafast oxidation towards chlorophenol(CP)via peroxymonosulfate(PMS)activa tion,which was almost one order of magnitudes than most of carbon-based catalysts.The DB-SiOC/PMS system also showed the high ability to resist the interference of environmental matrix.The radicals(^(·)OH and SO_(4)^(·–))exhibited a very small contribution to the CP oxidation while the electron transfer processe(ETP)played the major role in the DB-SiOC/PMS system.The electron shuttles from the electron-donating CP molecules to the adjacent DB-SiOC/PMS^(*)could be efficiently triggered via Si-O bonds as bridges,mak ing it possible for ultrafast oxidation of CP.In addition,the hollow-disc shaped DB-Si OC provided the biomorphic DE structures with abundant pores for enriching the PMS and pollutants,thus further ac celerating the oxidation reaction.This work provided a new routine for the fabrication of Si-O doped carbon-based catalysts with excellent Fenton-like catalytic activity,which would greatly promote thei application prospects in Fenton-like systems.
基金Supported by Heilongjiang Science Fundation for Young Scholars (Grant No. QC07C02)Scientific Foundation of Heilongjiang Education Department, China (Grant No. 11531035)
文摘As other natural iron-bearing minerals, schorl could be taken as an effective iron source for degradation of organic pollutants by mineral-catalyzed Fenton-like system. In our present study, the schorl-catalyzed Fenton-like system has been successfully developed for discoloration of an active commercial dye, Rhodamine B (RhB), in an aqueous solution. Through a number of batch discoloration experiments under various conditions, it was found that the reactivity of the system increased by, respectively, increasing schorl dosage, temperature, hydrogen peroxide starting concentration and by decreasing the pH. Over 90% of discoloration ratio could be gained in less than 30 min, and nearly 70% of total organic carbon (TOC) could be removed in less than 200 min. And, the schorl catalyst could be repeatedly used at least ten times, still with high catalytic activity. Comparative studies indicated that the RhB discoloration ratios were much higher in presence of schorl and H2O2 than those in presence of schorl or H2O2 only, which suggested that the schorl-catalyzed Fenton-like reaction governed the RhB discoloration process. The content of Fe ion leaching in the solution was also measured using inductively coupling plasma-atomic emission spectra (ICP-AES). A mechanism proposed herein suggested that adsorption and Fenton-like reaction (heterogeneous and homogeneous) were responsible for the discoloration of RhB.
基金The authors thanked the financial support from the National Natural Science Foundation of China(No.21925602)Natural Science Foundation of Jiangsu Province(No.BK20201309)the Fundamental Research Funds for the Central Universities(No.30920021116).
文摘In the pursuit of heterogeneous catalysts with high reactivity,metal organic framework(MOF)nanomaterials have received tremendous attentions.However,many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature,because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules.Here,we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel(GA),generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use.Compared to MIL-101-Fe,GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction,attributing to smaller MIL-101-Fe particle size,presence of active Fe(II)sites,and abundant defects in GA.Strikingly,the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature,by resisting the entrance of water molecules and helping to exclude water molecules.This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component,but also overcome its intrinsic drawback by taking advantage of the properties of host.We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
基金supported by the National Natural Science Foundation of China(No.22375019).
文摘As a new water treatment technology,Fenton-like reaction has great potential.In this study,we successfully prepared an excellent Fenton-like catalyst,which is composed of cobalt monoatoms and asymmetric subnanoclusters(labeled CoSA/Clu-C_(2)N),and exhibits excellent peroxymonosulfate(PMS)activation reactivity.By directly comparing the catalytic properties of CoSA-C_(2)N and CoSA/Clu-C_(2)N,the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were investigated.The results showed that CoSA/Clu-C_(2)N had higher degradation rates of carbamazepine(CBZ),antipyrine(AT)and chlorobenzoic acid(CA)when combined with active oxidant PMS.The cyclic frequency of CBZ was 5.4 min^(-1),which was twice as high as the catalytic constant of CoSA-C_(2)N(2.4 min^(-1)).The results show that CoSA/Clu-C_(2)N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in water.In addition,electron paramagnetic resonance(EPR)technology has proved that the introduction of Co subnano clusters in CoSA/Clu-C_(2)N is conducive to the production of singlet oxygen(1O_(2)),thereby improving the efficiency of pollutant oxidation.This work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.
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 Natural Science Foundation of China (Nos. 21577156, 21876184)the Fundamental Research Funds for the Central University (No. 310421124)。
文摘Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent ^(1)O_(2) mediated Fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H_(2)O_(2), but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0×10^(-8) mol/L to 1.0×10^(-5) mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring Fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.
基金financially supported from the National Natural Science Foundation of China(21802094,22272127,22002118,and 22172119)the National Science Fund for Distinguished Young Scholars(21825204)+1 种基金the Fundamental Research Funds for the Central Universities(D5000210666)the Natural Science Basic Research Plan in Shaanxi Province of China(2021JM-047).
文摘Identifying the active site of oxide-supported metal catalysts and revealing the intrinsic synergistic mechanism between metal and oxide support remain a large challenge.Herein,we report the identification and separation of the Pt-O-Ti interface and TiO_(2) surface in Pt-TiO_(2)-based catalysts by depositing different thickness of TiO_(2) shell with∼0.4-nm micropores onto the surface of Pt/TiO_(2) catalyst through atomic layer deposition(ALD).In the oxidation of 3,3′,5,5′-tetramethylbenzidine(TMB)by hydrogen peroxide(H_(2)O_(2))process,the TiO_(2) microporous shells can prevent the contact between TMB and embedded Pt clusters,but not delay the diffusion of H_(2)O_(2).The heterolysis of H_(2)O_(2) to ·OH occurs on the Pt-O-Ti interface,and the generated•OH migrates to the TiO_(2) surface to supplement the surface lattice oxygen,which sequentially oxidizes TMB to oxTMB.And the synergistic effect between Pt-O-Ti interface active sties and TiO_(2) surface active sites can significantly improve the catalytic performance.Our study provides a guide for the understanding of the intrinsic synergistic mechanism between the metal and oxide support in the metal-oxide catalysts.
基金supported by the National Natural Science Foundation of China (Nos.5182220221972163 and 51772050)the Fundamental Research Funds for the Central Universities (No. 2232020D-02)+7 种基金Shanghai Sailing Program (No.20YF1400500)Shanghai Natural Science Foundation (No.20ZR1401500)Shanghai Rising-Star Program (No.18QA1400100)Youth Top-notch Talent Support Program of Shanghai,Science and Technology Commission of Shanghai Municipality (No.19520713200)Shanghai Scientific and Technological Innovation Project (No. 19JC1410400)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 20JC1415300)DHU Distinguished Young Professor ProgramFundamental Research Funds for the Central Universities。
文摘Photocatalysis and Fenton process are two primary and promising advanced oxidation processes to degrade organic pollutants.However,the practical applications of single photocatalysis and Fenton process are still limited.Introducing one of them into another to form a combined photocatalytic Fentonlike system has shown great potential but still faces challenges in designing a well-tailored catalyst.Herein,a confined photocatalytic Fenton-like micro-reactor catalyst with a movable Fe_(3) O_(4) core and a mesoporous TiO_(2) shell has been constructed via a successive Stober coating strategy,followed by an ultrasound assisted etching method.The resulting micro-reactor possesses well-defined yolk-shell structures with unifo rm mesopores(~4 nm),a large Brunauer-Emmett-Teller(BET) surface area(~166.7 m^(2)/g),a high pore volume(~0.56 cm^(3)/g) and a strong magnetization(~51 emu/g),as well as tunable reactor sizes(20-90 nm).When evaluated for degrading bisphenol A under solar light in the presence of peroxymo no sulfate,the micro-reactor exhibits a superior catalytic degradation perfo rmance with a high magnetic separation efficiency and an excellent recycle ability.The outstanding performance can be attributed to its unique textual structure,which leads to a great syne rgistic effect from the photocatalytic and Fenton-like process.This study gives an important insight into the design and synthesis of an advanced micro-reactor for a combined advanced oxidation processes(AOPs).
基金sponsored by Shanghai Pujiang Program, China (No. 16PJ1401100)the Shanghai Committee of Science and Technology, China (No.15ZR1402000)+3 种基金Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 17JC1400100)the NSF of China(No. 21673048)National Youth Top Talent Support Program of National High-Level Personnel of Special Support Program (Youth Top-notch Talent Support Program)the State Key Laboratory of Transducer Technology of China (No. SKT1503)
文摘A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.
基金the National Natural Science Foundation of China(42077176,41601514)Shanghai“Science and Technology Innovation Action Plan”Project(19230742400,19ZR1459300)+1 种基金Shanghai Peak Discipline Project(0200121005/053,2019010202)State Key Laboratory of Petroleum Pollution Control(PPC2016019)。
文摘Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF degradation by the combined process of zero-valent iron nanoparticles(nZVI)and nano calcium peroxide(nCaO_(2))were performed.A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO_(2)nanoparticles and pH value on the DCF removal.In the meantime,the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO_(2)nanoparticles in the reaction system.The results show that the nZVI/nCaO_(2)can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO_(2)added,resulting in a removal rate of greater than 90%in a 2-hour reaction with an initial pH of 5.The degradation rate of DCF was positively correlated with the dosage of nCaO_(2),and negatively correlated with both nZVI dosage and the initial pH value.The order of significance of the three factors is identified as pH value>nZVI dosage>nCaO_(2)dosage.In the continuous-flow reaction system,the DCF removal rates remained above 75%within 150 minutes at the pH of 5,with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO_(2).These results provide a theoretical basis for the nZVI/nCaO_(2)application to remove DCF in groundwater.
基金supported by the National Natural Science Foundation of China(Nos.21273059,21528501,21511130060)the HIT Environment and Ecology Innovation Special Funds(No.HSCJ201617)
文摘This paper reports a template-free method to synthesize a series of inorganic hollow spheres(IHSs)including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/"water-brother" interfaces. "Water-brother" was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/"water-brother" interfaces are very different from water/oil interfaces. The "water-brother" solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多
基金financially supported by the National Natural Science Foundation of China(No.21676209)Key Research Development Project of Shaanxi Province(No.2019GY-137)the Cultivating Fund of Excellent Doctorate Thesis of Xi’an University of Architecture and Technology(No.6040318008).
文摘In this study,a magnetic P zeolite was directly synthesized by utilization of industrial solid wastes of zinc slag(ZS)and circulating fluidized bed fly ash(CFBFA)via one-step hydrothermal method.The effects of different CFBFA/ZS ratios and hydrothermal times on the as-synthesized zeolite were investigated.The X-ray diffraction(XRD)and vibrating sample magnetometer(VSM)results indicated that the magnetic P zeolite possessed well-defined crystals and superparamagnetism.The as-prepared zeolite was employed as a Fenton-like solid catalyst for degradation of direct green B dye wastewater.It was discovered that the magnetic P zeolite took the advantage of rapid separation and efficient recovery under the external magnets in a solid-liquid reaction.The effects of the solution pH,the catalyst dosage,and the H_(2)O_(2)concentration on the degradation rate of direct green B dye wastewater were studied systematically.The results showed that the highest degradation of 96.3%was obtained and the magnetic P zeolite showed excellent stability after four cycles.Therefore,the magnetic P zeolite derived from industrial solid wastes had a potential application in wastewater treatment.