The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,a...The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,and the well matching band structure successfully constitutes a new Type-II heterojunction.As expected,the photocatalytic hydrogen production experiment showed that the quantity of hydrogen produced on 5% SnS_(2)/C_(3)N_(5)was 922.5μmol/(g.h),which is 3.6 times higher than that of pure g-C_(3)N_(5).Meanwhile,in photocatalytic degradation of methylene blue,5%SnS2/C,Ns composite material can degrade 95% of contaminants within 40 min,showing good photocatalytic degradation performance.The mechanism study indicates that SnS_(2)/C_(3)N_(5)heterojunction improves the photogenerated charge migration rate and reduces the electron-hole recombination rate,and effectively improves the photocatalytic performance of g-C_(3)N_(5).This work provides a new idea for designing C,Ns-based heterojunctions with efficient hydrogen production and degradation performance.展开更多
Photocatalysis is an important process in energy conversion and environmental usage because of its feasible,profitable,and environmentally safe benefits.Coordination chemistry of the CeO_(2)is gaining significant inte...Photocatalysis is an important process in energy conversion and environmental usage because of its feasible,profitable,and environmentally safe benefits.Coordination chemistry of the CeO_(2)is gaining significant interest because its nanocomposites show unique characteristics namely optically active,wide bandgap(Eg),reversible valence states(Ce^(3+/4+)),rich defect architectures,high O_(2)storage capability,ionic conductivity,and exceptional chemical resistance.Systematically summarized the importance of synthesis methods,particle morphology,and crystal structure aiming at how to heighten the efficacy of CeO_(2)-derived hybrid heterojunction(HHJ)photocatalyst.Selection of an appropriate synthesis method and morphology of the composite materials are beneficial in inhibiting the rapid electron-hole(e^(−)-h^(+))recombination,improvement in visible light adsorption,and large generation of e^(−)-h^(+)pairs to accelerate the photocatalysts activities.Various modification approaches include elemental doping(metal/non-metal doping),heterojunction construction(lower/wide Eg semiconductors(SCD),carbon,conducting polymeric materials),imperfection engineering,and multicomponent hybrid composites.These methods assist as a valuable resource for the rational design of effective CeO_(2)-based composite photocatalysts for sustainable development owing to the enhancement of oxygen species mobility,rapid charge transfer,maximum visible light captivation and slow down the charge recombination rate with increase photogeneration of e−-h+pairs.Also examines the advancements made in CeO_(2)conjugated hybrid composites in photo-oxidation of wastewater effluents(antibiotic/organic dyes/chemical/pharmaceutical),heavy metal removal,H2 production,CO_(2)reduction,and H2O splitting applications.Subsequently,the difficulties and fundamental ideas behind several heterojunction photocatalysts encountered by CeO_(2)-based composites are examined,and future directions for their development are suggested.展开更多
Developing environmental-friendly non-metal photocatalysts for the efficient removal of antibiotics from environment is a significant challenge.The construction of heterojunction is regarded as a powerful strategy to ...Developing environmental-friendly non-metal photocatalysts for the efficient removal of antibiotics from environment is a significant challenge.The construction of heterojunction is regarded as a powerful strategy to enhance the photodegradation efficiency of photocatalysts for pollutants,being due that this strategy can effectively suppress the recombination of the photo-induced electron and hole.In this research,a novel double Z-scheme BN/C_(60)/g-C_(3)N_(4) heterojunction was successfully synthesized via one-step synthetic approach.Based on a series of experimental characterization,BN/C_(60)/g-C_(3)N_(4) is most likely formed via the interaction between N element of BN and g-C_(3)N_(4) with C_(60) under UV-light irradiation.The band structures of BN,C_(60),g-C_(3)N_(4) and the internal electric field among them suggest that BN/C_(60)/g-C_(3)N_(4) may has a direct double z-type band arrangement,which facilitates efficient charge transfer.The photodegradation rate of BN/C_(60)/g-C_(3)N_(4) for tetracycline reached 90.1%,which is 2.9 times higher than that observed with BN and 2.3 times higher than that of g-C_(3)N_(4).BN/C_(60)/g-C_(3)N_(4) exhibits remarkable photocatalytic performance across a wide pH range and in the influence of different anions.This study offers significant insights about how to design double z-scheme metal-free photocatalyst with high photodegradation efficiency for antibiotic.展开更多
It has been challenging for Fe(Ⅲ)regeneration in Fe-based photocatalysts for continuous peroxydisulfate(PDS)activation due to the lower ability to reduce Fe(Ⅲ).In this work,Fe-doped ultrathin VO_(2)(Fe-VO_(2))nanobe...It has been challenging for Fe(Ⅲ)regeneration in Fe-based photocatalysts for continuous peroxydisulfate(PDS)activation due to the lower ability to reduce Fe(Ⅲ).In this work,Fe-doped ultrathin VO_(2)(Fe-VO_(2))nanobelts were synthesized for purifying metronidazole(MNZ)via PDS activation.As an efficient Fentonlike catalyst for PDS activation,2 wt%Fe-doped VO_(2)can remove 98%of MNZ within 40 min and exhibits impressive recyclability.The synergistic effect of Fe-VO_(2)and Fe(Ⅲ)activated PDS boosted the photocatalytic performance.Moreover,SO_(4)•^(−),h+,O_(2)•^(−),^(1)O_(2),and•OH were the main reactive radicals.The effects of initial MNZ concentration,Fe-VO_(2),PDS dosage,and various anions/cations on MNZ removal by the Fe-VO_(2)/PDS/Vis system were studied.The intermediates of MNZ degradation and possible pathways were determined by density function theory(DFT)calculations and HPLC-MS.This study provided a sustainable technology using Fe-doped ultrathin VO_(2)nanobelts for photocatalytic PDS activation and decontamination of pharmaceutical wastewater.展开更多
Photodegradation is considered as a universal contributing factor to litter decomposition and carbon(C)cycling within the Earth’s biomes.Identifying how solar radiation modifies the molecular structure of litter is e...Photodegradation is considered as a universal contributing factor to litter decomposition and carbon(C)cycling within the Earth’s biomes.Identifying how solar radiation modifies the molecular structure of litter is essen-tial to understand the mechanism controlling its decom-position and reaction to shifts in climatic conditions and land-use.In this study,we performed a spectral-attenuation experiment following litter decomposition in an understory and gap of a temperate deciduous forest.We found that short-wavelength visible light,especially blue light,was the main factor driving variation in litter molecular struc-ture of Fagus crenata Blume,Quercus crispula Blume,Acer carpinifolium Siebold&Zuccarini and Betula platyphylla Sukaczev,explaining respectively 56.5%,19.4%,66.3%,and 16.7%of variation in its chemical composition.However,the variation also depended on canopy openness:Only in the forest gap was lignin aromatic C negatively associated with C-oxygen(C–O)bonding in polysaccharides receiv-ing treatments containing blue light of the full spectrum of solar radiation.Regardless of species,the decomposition index of litter that explained changes in mass and lignin loss was driven by the relative content of C–O stretching in poly-saccharides and lignin aromatic C.The results suggest that the availability of readily degradable polysaccharides pro-duced by the reduction in lignin aromatic C most plausibly explains the rate of litter photodegradation.Photo-products of photodegradation might augment the C pool destabilized by the input of readily degradable organic compounds(i.e.,polysaccharides).展开更多
Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composit...Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composite was evaluated using the degradation of rhodamine B(RhB)and tetracycline hydrochloride(TCH)under visible light.The results demonstrated that Ti_(3)C_(2)/BOC composite had higher photocatalytic activity than pure BOC.The optimum incorporation amount of Ti_(3)C_(2) was 2 wt%.The photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC at 10 min to 20 mg/L RhB was 97.6%,which was much higher than that of BOC(75.3%).Similarly,the photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC to 10 mg/L TCH at 30 min was 80.4%,which was higher than BOC(68.1%).In addition,the prepared 2 wt%-Ti_(3)C_(2)/BOC composite also maintained good stability even after four cycles.Electrochemical impedance spectroscopy(EIS),transient photocurrent response(IT)and ultraviolet-visible diffuse reflectance spectroscopy(UV-vis)confirmed that the photoelectrochemical properties of 2 wt%-Ti_(3)C_(2)/BOC composite were significantly improved.On the basis of analyzing the action mechanism of photocatalyst,it was pointed out that·O_(2)^(-)and h~+were the main active substances in the photodegradation of RhB and TCH by 2 wt%-Ti_(3)C_(2)/BOC.展开更多
Lead-free halide perovskite material has drawn fast-growing interest due to its superiorsolar-conversion efficiency and nontoxic nature. In this work, we have successfully fabricatedcesium silver bismuth bromide (Cs2A...Lead-free halide perovskite material has drawn fast-growing interest due to its superiorsolar-conversion efficiency and nontoxic nature. In this work, we have successfully fabricatedcesium silver bismuth bromide (Cs2AgBiBr6) quantum dots utilizing the hot injectionmethod. The as-synthesized quantum dots were characterized by combined techniques,which showed remarkable visible-light photocatalytic activity for organic dyes and antibioticdegradation in ethanol. Specifically, about 97% of rhodamine B and methyl orange maybe removed within 10 min and 30 min, respectively. Additionally, 60% of antibiotic residueof tetracycline hydrochloride is degraded in 30min which is 7 times more than that on commercialtitania (P25). The reactive species for the photodegradation are determined throughcapture experiments, and a reaction mechanism is proposed accordingly. This work providesa novel photocatalyst for the selective removal of diverse organic contaminants inethanol and an alternative for the potential application of lead-free halide perovskites.展开更多
The widespread application of phenolic substances in the field of food,medicine and industry,is harmful to the environment and human health.Therefore,it is very important to develop a con-venient and effective method ...The widespread application of phenolic substances in the field of food,medicine and industry,is harmful to the environment and human health.Therefore,it is very important to develop a con-venient and effective method to detect and degrade phenolic compounds.Herein,we report a new keggin-type polyoxometallate-based metal-organic complex self-assembled under solvothermal condition,{[Cu(dap)(3-PA)]4(SiW_(12)O_(40))(H_(2)O)_(2)}·2H_(2)O(1,dap=1,2-diaminopropane,3-HPA=3-pyridineacrylic acid).1 shows an interesting 1D ladder-like structure.As a bifunctional catalyst,1 can be employed as a colori-metric sensor toward phenol with the relatively low detection limit(LOD)of 0.36μmol/L(S/N=3)in the wide range(0.001-0.1 mmol/L).The title colorimetric sensor is applied to determine phenol in various water environment with good recoveries ranging from 95%-105%.In addition,1 also exhibits excellent photocatalytic degradation toward phenol under visible light with the highest removal efficiency at 96%for 100 min and wide pH universality.The selectivity,stability and reliability of the detection of 1 towards phenol,as well as the detection for 4-chlorophenol,o-cresol,4-nitrophenol and phloroglucinol were stud-ied.Furthermore,the photocatalytic reaction kinetics and the mechanisms of photodegradation of phenol were also investigated in detail.展开更多
The edge-graphitized carbon nitride(C_(3)N_(4)-C g)was prepared by secondary pyrolysis to construct ZnO/C_(3)N_(4)-C g(ZCN)type-Ⅱheterojunction photocatalyst via a facile sonication dispersion method,which achieved∼...The edge-graphitized carbon nitride(C_(3)N_(4)-C g)was prepared by secondary pyrolysis to construct ZnO/C_(3)N_(4)-C g(ZCN)type-Ⅱheterojunction photocatalyst via a facile sonication dispersion method,which achieved∼7.04-fold and∼18.3-fold enhanced visible-light-driven photocatalytic performance for refrac-tory micropollutant removal and simultaneous hydrogen(H_(2))evolution respectively compared to con-ventional ZnO/g-C_(3)N_(4)Step-scheme heterojunction.The apparent quantum efficiency of the ZCN_(0.4)het-erojunction reaches 0.92%(λ=420 nm).Such excellent performance stems from that the edge-graphene moieties stitched onto the interface of heterojunction extend light absorption to the full visible spec-trum,meanwhile,the built-in electric field generated during Fermi level alignment accompanying fa-vorable band-bending structure provides an effective pathway for the rapid migration of photoinduced electrons via the edge graphene channel to improve interfacial charge separation efficiency.Interestingly,the midgap states introduced in ZCN heterojunction could temporarily retain photoexcited electrons to effectively inhibit the in situ carrier recombination for improved photocatalytic H_(2)evolution.Moreover,ZCN/peroxymonosulfate system exhibited excellent anti-interference performance against complex water bodies under visible illumination due to the synergistic effect between the co-existing anions and organic matter.Meanwhile,the eco-friendly nature of the ZCN/peroxymonosulfate system showed no biotoxicity of reaction filtrate on cell proliferation after treatment,which avoided secondary contamination.Consid-ering the outstanding performance in photocatalysis,the ZCN system exhibits broad potential for practical applications in water pollution control and green energy production.展开更多
Inactivation of cyanobacterial cells and simultaneous control of secondary metabolites is of significant necessity for the treatment of cyanobacteria-laden water.Acetylacetone(AcAc)has been reported a specific algicid...Inactivation of cyanobacterial cells and simultaneous control of secondary metabolites is of significant necessity for the treatment of cyanobacteria-laden water.Acetylacetone(AcAc)has been reported a specific algicide to inactivate Microcystis aeruginosa(M.aeruginosa)and an effective light activator to degrade pollutants.This study systematically investigated the photodegradation ability of AcAc under xenon(Xe)irradiation on the secondary metabolites of M.aeruginosa,mainly algal organic matter(AOM),especially toxic microcystin-LR(MC-LR).Results showed that AcAc outperformed H_(2)O_(2)in destructing the protein-like substances,humic acid-like matters,aromatic proteins and fulvic-like substances of AOM.For MC-LR(250μg/L),0.05 mmol/L AcAc attained the same degradation efficiency(87.0%)as 0.1mmol/L H_(2)O_(2).The degradation mechanism of Xe/AcAc might involve photo-induced energy/electron transfer and formation of carbon center radicals.Alkaline conditions(pH>9.0)were detrimental to the photoactivity of AcAc,corresponding to the observed degradation rate constant(k_(1)value)of MC-LR drastically decreasing to 0.0013 min^(-1)as solution pH exceeded 9.0.The PO_(4)^(3-)and HCO_(3)^(-)ions had obvious inhibition effects,whereas NO_(3)^(-)slightly improved k_(1)value from 0.0277 min^(-1)to 0.0321 min^(-1).The presence of AOM did not significantly inhibit MC-LR degradation in Xe/AcAc system.In addition,the biological toxicity of MC-LR was greatly reduced after photoreaction.These results demonstrated that AcAc was an alternative algicidal agent to effectively inactivate algal cells and simultaneously control the secondary metabolites after cell lysis.Nevertheless,the concentration and irradiation conditions should be further optimized in practical application.展开更多
La,Ce co-doped ZnO nanorods(ZnLC)were synthesized through a one-step solvothermal route.The photocatalysts were characterized by X-ray diffraction,Raman spectroscopy,field-emission scanning electron microscopy,energy ...La,Ce co-doped ZnO nanorods(ZnLC)were synthesized through a one-step solvothermal route.The photocatalysts were characterized by X-ray diffraction,Raman spectroscopy,field-emission scanning electron microscopy,energy dispersive X-ray,transmission electron microscopy,UV-vis diffuse reflectance spectroscopy and photo luminescence spectroscopy.The La and Ce doping enhanced the visible light absorption ability of ZnLC and a red shift was detected for ZnLC.Under simulated solar light irradiation,the ZnO doped with 3 at%La and 1 at%Ce(ZnLC1)degrades methylene blue(MB)more effectively than those of pure ZnO,La-doped ZnO(ZnL)and commercially available ZnO.The improved photocatalytic performance of ZnLC1 can be attributed to the high charge separation efficiency as demonstrated by the photoluminescence spectra.Additionally,the photocatalytic experiments reveal that several parameters have their own impact on the MB degradation.Using a variety of radical scavengers,it is discovered that superoxide anion radical plays a crucial role in the degradation of MB.The ZnLC1 is also reused several times without noticeable decrease of photoactivity,indicating that it has a substantial potential for environmental remediation applications.展开更多
Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health ...Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.展开更多
Developing high-efficiency photocatalysts for tetracycline hydrochloride(TCH)degradation is of great sig-nificance to ecosystems and human beings.In this work,a two-step process of exfoliation and re-stacking was perf...Developing high-efficiency photocatalysts for tetracycline hydrochloride(TCH)degradation is of great sig-nificance to ecosystems and human beings.In this work,a two-step process of exfoliation and re-stacking was performed to prepare re-stacked HTiNbO_(5) nanosheets(R-HTNS)and then coupled with Ti_(3)C_(2) MXene to construct Ti_(3)C_(2) MXene/R-HTNS(MX/RTS)with a 2D/2D Schottky heterojunction.These 2D/2D het-erostructures between Ti_(3)C_(2) MXene and R-HTNS can produce an internal electric field and provide max-imum interface area for efficient charge transfer across the intimate interface.The photocatalytic perfor-mance of samples was evaluated by TCH degradation under simulated sunlight.The MX/RTS composites,with an optimal sample of 3-MX/RTS,show enhanced photocatalytic activity for TCH degradation com-pared with R-HTNS.The characterization results reveal that the introduction of Ti_(3)C_(2) MXene can signif-icantly increase specific surface area for providing more reactive sites and broaden the light absorption region.Besides,the incident light energy is absorbed by the Ti_(3)C_(2) MXene component in MX/RTS compos-ites to generate photothermal energy(heat),which facilitates the charge carrier separation and surface reaction kinetics.Thus,the enhanced TCH photodegradation activity for MX/RTS composites is due to the introduction of Ti_(3)C_(2) MXene,which possesses the synergistic effect of the increased specific surface area,improved light-harvesting capacity,2D/2D Schottky heterojunction,and photothermal energy effect.Additionally,the TCH photodegradation behavior is deliberated with a detailed discussion on various co-existing ions.During TCH photodegradation,the active radical species are determined for 3-MX/RTS.Ac-cording to the characterization results,the possible TCH photodegradation pathway and mechanism over 3-MX/RTS are explored.This work may offer a novel insight for constructing MXene-based heterostruc-tured photocatalysts with high efficiency.展开更多
Environmental pollution,such as water contamination,is a critical issue that must be absolutely addressed.Here,three different morphologies of tungsten-based photocatalysts(WO_(3)nanorods,WO_(3)/WS_(2)nanobricks,WO_(3...Environmental pollution,such as water contamination,is a critical issue that must be absolutely addressed.Here,three different morphologies of tungsten-based photocatalysts(WO_(3)nanorods,WO_(3)/WS_(2)nanobricks,WO_(3)/WS_(2)nanorods)are made using a simple hydrothermal method by changing the solvents(H_(2)O,DMF,aqueous HCl solution).The as-prepared nanocatalysts have excellent thermal stability,large porosity,and high hydrophilicity.The results show all materials have good photocatalytic activity in aqueous media,with WO_(3)/WS_(2)nanorods(NRs)having the best activity in the photodegradation of bisphenol A(BPA)under visible-light irradiation.This may originate from increased migration of charge carriers and effective prevention of electron–hole recombination in WO_(3)/WS_(2)NRs,whereby this photocatalyst is able to generate more reactive·OH and·O_(2)^(–)species,leading to greater photocatalytic activity.About 99.6% of BPA is photodegraded within 60 min when using 1.5 g/L WO_(3)/WS_(2)NRs and 5.0 mg/L BPA at pH 7.0.Additionally,the optimal conditions(pH,catalyst dosage,initial BPA concentration)for WO_(3)/WS_(2)NRs are also elaborately investigated.These rod-like heterostructures are expressed as potential catalysts with excellent photostability,efficient reusability,and highly active effectivity in different types of water.In particular,the removal efficiency of BPA by WO_(3)/WS_(2)NRs reduces by only 1.5% after five recycling runs and even reaches 89.1%in contaminated lake water.This study provides promising insights for the nearly complete removal of BPA from wastewater or different water resources,which is advantageous to various applications in environmental remediation.展开更多
In dye-photocatalysis, widening the wavelengths absorption range of catalysts as well as aborting the recombination of the photoexcited charge carriers(electrons-holes pairs) are of paramount significance.In the curre...In dye-photocatalysis, widening the wavelengths absorption range of catalysts as well as aborting the recombination of the photoexcited charge carriers(electrons-holes pairs) are of paramount significance.In the current study, we report the photocatalytic characteristics of four compositions composed of TiO_(2),Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders for two harmful dyes(Congo red and methylene blue). The X-ray diffraction technique verified the configuration of mixed anatase and rutile phases in pure TiO_(2)and Ti_(0.97)Cu_(0.03)O_(2)powders while Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders possess anatase phase only. The changes of the band gap structure and dimensions of the unit cell volume of TiO_(2)confirm the substitution of Ti^(4+)sites by Cu^(2+)and La^(3+)ions. Remarkable widening of wavelengths absorption with formation of long absorption tails were found in TiO_(2)(3.13 e V) through insertion of La^(3+)plus Cu^(2+)ions. Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)samples exhibit a visible light band gap of 2.3 and 2.7 e V, respectively. Based on SEM images, incorporation of Cu^(2+)and La^(3+)ions influences the surface morphology of TiO_(2). The resulting Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders present enhanced photocatalytic activity towards Congo red dye degradation compared to pure one under natural solar spectrum. The best Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst exhibits superior photocatalytic activity of 96% for 10 ppm CR dye in 20 min as well as above average photocatalytic efficiency of 63% for 30 ppm CR dye in 120 min. As well, it showed acceptable photodegradation activity of 52% for 30 ppm MB solution in 140 min of sunlight irradiation. The heightened photodegradation efficiency of Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst can be clarified in terms of higher charge carriers' separation(Cu^(2+)+ e-→ Cu^(+), La^(3+)+ e-→ La^(2+)), oxygen vacancies, full anatase phase structure as well as the wide range of visible light absorption.展开更多
Semiconductor heterojunction engineering and three-dimensional(3D)architecture con-struction have been considered highly desirable strategies to enhance photocatalytic perfor-mance.Herein,a BiOI/ZnO composite photocat...Semiconductor heterojunction engineering and three-dimensional(3D)architecture con-struction have been considered highly desirable strategies to enhance photocatalytic perfor-mance.Herein,a BiOI/ZnO composite photocatalyst with a 3D flower-like architecture was successfully prepared,whichwas stably immobilized on three-dimensional porous lignocel-lulosic biomass Juncus effusus(JE)fiber.The outstanding photocatalytic performance of the BiOI/ZnO-JE fiber was confirmed by the degradation of tetracycline hydrochloride(TC,90%),ciprofloxacin(CIP,79%),and norfloxacin(NOR,81%).The enhanced photocatalytic activities were mainly attributed to the synergistic absorption performance of the lignocellulosic JE and the effective transfer and separation of charges.Moreover,the hydroxyl(·OH)and super-oxide radicals(·O_(2)^(−))are themain reactive species in the photocatalytic process according to the analysis.This work may provide a novel perspective for constructing high-performance lignocellulosic-based photocatalytic materials.展开更多
We investigated the influence mechanism of N-doping for dissolved black carbon(DBC)photodegradation of organic pollutants.The degradation performance of N-doped dissolved black carbon(NDBC)for tetracycline(TC)(71%)is ...We investigated the influence mechanism of N-doping for dissolved black carbon(DBC)photodegradation of organic pollutants.The degradation performance of N-doped dissolved black carbon(NDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under irradiation.These levels are both better than DBC degradation performances for TC(68%)and MB(18%)under irradiation.Reactive species quenching experiments suggest that h and-O,are the main reactive species for NDBC photodegraded TC,while-OH and h*are the main reactive species for NDBC photodegraded MB.-OH is not observed during DBC photodegradation of MB.This is likely because N-doping increases valence-band(VB)energy from 1.55 eV in DBC to 2.04 eV in NDBC;the latter is strong enough to oxidize water to form-OH.Additionally,N-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC,resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in DBC.AIl these factors give NDBC stronger photodegradation performance for TC and MB than DBC.High-performance liquid chromatography-mass spectrometry(HPLC-MS)characterization and toxicity evaluation with the quantitative structure-activity relationship(QSAR)method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by DBC.We adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species produced.Our results add to the understanding of the photochemical behavior of NDBC.展开更多
It is important to investigate whether combining two modification strategies has a synergistic effect on the activity of photocatalysts.In this manuscript,Fe-doped BiOBr/Bi_(2)WO_(6) heterojunctions were synthesized b...It is important to investigate whether combining two modification strategies has a synergistic effect on the activity of photocatalysts.In this manuscript,Fe-doped BiOBr/Bi_(2)WO_(6) heterojunctions were synthesized by a one-pot solvothermal method,and excellent photocatalytic performance was obtained for the degradation of tetracycline hydrochloride(TCH)in water without the addition of surfactant.Combining experiments and characterization,the synergistic effect between Fe ion doping and the BiOBr/Bi_(2)WO_(6) heterojunction was elucidated.The Fe/BiOBr/Bi_(2)WO_(6) composite photocatalyst had a beneficial void structure,enhanced visible light response,and could inhibit the recombination of photogenerated support well,which improved the photocatalytic activity.The presented experiments demonstrate that Fe/BiOBr/Bi_(2)WO_(6) removes 97% of TCH from aqueous solution,while pure BiOBr and Bi_(2)WO_(6) only remove 56% and 65% of TCH,respectively.Finally,the separation and transfer mechanisms of photoexcited carriers were determined in conjunction with the experimental results.This study provides a new direction for the design of efficient photocatalysts through the use of a dual co-modification strategy.展开更多
The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by ...The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.展开更多
Constructing new photocatalysts for the photocatalytic reduction of CO_(2)and efficient degradation of Lev-ofloxacin is of great importance to renewable energy.Here,S-scheme Bi_(2)MoO_(6-x)/MoS_(2)heterojunction nanos...Constructing new photocatalysts for the photocatalytic reduction of CO_(2)and efficient degradation of Lev-ofloxacin is of great importance to renewable energy.Here,S-scheme Bi_(2)MoO_(6-x)/MoS_(2)heterojunction nanospheres containing abundant surface defects(oxygen vacancies)were designed and successfully syn-thesized to enhance CO_(2)photoreduction activity in the absence of other sacrificial agents,co-catalysts or photosensitisers.At the same time,it can efficiently degrade organic pollutants(Levofloxacin).This heterogeneous structure with surface defects provides an abundance of reactive sites,accelerates charge separation and improves oxidation capacity.The improved Bi_(2)MoO_(6-x)/MoS_(2)heterogeneous nanospheres show excellent performance under simulated solar light,with the selectivity and yield of 92.45%and 29.01μmol h^(−1),respectively,for the generation of CO.Under visible light,the degradation efficiency of levofloxacin hydrochloride(LVX)reached 96.3%within 25 min and remained as high as 95%after three cycles.This work provides a new idea for the design of new S-scheme photocatalysts and an important reference for the preparation of photocatalysts for the efficient photocatalytic reduction of CO_(2)and the efficient degradation of organic pollutants at the same time.展开更多
基金This project was supported by the Fundamental Research Program of Shanxi Province(202303021221058)。
文摘The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,and the well matching band structure successfully constitutes a new Type-II heterojunction.As expected,the photocatalytic hydrogen production experiment showed that the quantity of hydrogen produced on 5% SnS_(2)/C_(3)N_(5)was 922.5μmol/(g.h),which is 3.6 times higher than that of pure g-C_(3)N_(5).Meanwhile,in photocatalytic degradation of methylene blue,5%SnS2/C,Ns composite material can degrade 95% of contaminants within 40 min,showing good photocatalytic degradation performance.The mechanism study indicates that SnS_(2)/C_(3)N_(5)heterojunction improves the photogenerated charge migration rate and reduces the electron-hole recombination rate,and effectively improves the photocatalytic performance of g-C_(3)N_(5).This work provides a new idea for designing C,Ns-based heterojunctions with efficient hydrogen production and degradation performance.
文摘Photocatalysis is an important process in energy conversion and environmental usage because of its feasible,profitable,and environmentally safe benefits.Coordination chemistry of the CeO_(2)is gaining significant interest because its nanocomposites show unique characteristics namely optically active,wide bandgap(Eg),reversible valence states(Ce^(3+/4+)),rich defect architectures,high O_(2)storage capability,ionic conductivity,and exceptional chemical resistance.Systematically summarized the importance of synthesis methods,particle morphology,and crystal structure aiming at how to heighten the efficacy of CeO_(2)-derived hybrid heterojunction(HHJ)photocatalyst.Selection of an appropriate synthesis method and morphology of the composite materials are beneficial in inhibiting the rapid electron-hole(e^(−)-h^(+))recombination,improvement in visible light adsorption,and large generation of e^(−)-h^(+)pairs to accelerate the photocatalysts activities.Various modification approaches include elemental doping(metal/non-metal doping),heterojunction construction(lower/wide Eg semiconductors(SCD),carbon,conducting polymeric materials),imperfection engineering,and multicomponent hybrid composites.These methods assist as a valuable resource for the rational design of effective CeO_(2)-based composite photocatalysts for sustainable development owing to the enhancement of oxygen species mobility,rapid charge transfer,maximum visible light captivation and slow down the charge recombination rate with increase photogeneration of e−-h+pairs.Also examines the advancements made in CeO_(2)conjugated hybrid composites in photo-oxidation of wastewater effluents(antibiotic/organic dyes/chemical/pharmaceutical),heavy metal removal,H2 production,CO_(2)reduction,and H2O splitting applications.Subsequently,the difficulties and fundamental ideas behind several heterojunction photocatalysts encountered by CeO_(2)-based composites are examined,and future directions for their development are suggested.
基金supported by the Project of State Key Laboratory of Treatments and Recycling for Organic Effluents by the Adsorption in Petroleum and Chemical Industry,Soochow University(No.SDHY2207)the Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes,Ministry of Education,College of Environment,Hohai University(No.B230203006)A Project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Developing environmental-friendly non-metal photocatalysts for the efficient removal of antibiotics from environment is a significant challenge.The construction of heterojunction is regarded as a powerful strategy to enhance the photodegradation efficiency of photocatalysts for pollutants,being due that this strategy can effectively suppress the recombination of the photo-induced electron and hole.In this research,a novel double Z-scheme BN/C_(60)/g-C_(3)N_(4) heterojunction was successfully synthesized via one-step synthetic approach.Based on a series of experimental characterization,BN/C_(60)/g-C_(3)N_(4) is most likely formed via the interaction between N element of BN and g-C_(3)N_(4) with C_(60) under UV-light irradiation.The band structures of BN,C_(60),g-C_(3)N_(4) and the internal electric field among them suggest that BN/C_(60)/g-C_(3)N_(4) may has a direct double z-type band arrangement,which facilitates efficient charge transfer.The photodegradation rate of BN/C_(60)/g-C_(3)N_(4) for tetracycline reached 90.1%,which is 2.9 times higher than that observed with BN and 2.3 times higher than that of g-C_(3)N_(4).BN/C_(60)/g-C_(3)N_(4) exhibits remarkable photocatalytic performance across a wide pH range and in the influence of different anions.This study offers significant insights about how to design double z-scheme metal-free photocatalyst with high photodegradation efficiency for antibiotic.
基金the financial supports from the National Key Research and Development Program of China(Nos.2021YFB3500600,2021YFB3500605,2022YFB3504100)Key R&D Program of Jiangsu Province(No.BE2022142)+6 种基金Ministry of Education Chunhui plan international cooperation project(No.202200554)National Natural Science Foundation of China(No.grant 22208170)Natural Science Foundation of Inner Mongolia(No.2021BS02016)Jiangsu International Cooperation Project(No.BZ2021018)Nanjing Science and Technology Top Experts Gathering Plan,and Open Foundation of State Environmental Protection Key Laboratory of Soil Environmental Management and Pollution Control(No.SEMPC2023004)Cooperation Foundation for the Chunhui Plan Program of Ministry of Education of China(No.202200554)Open Project Program of Key Laboratory of Opticelectric Sensing and Analytical Chemistry for Life Science(No.M2024-7),MOE。
文摘It has been challenging for Fe(Ⅲ)regeneration in Fe-based photocatalysts for continuous peroxydisulfate(PDS)activation due to the lower ability to reduce Fe(Ⅲ).In this work,Fe-doped ultrathin VO_(2)(Fe-VO_(2))nanobelts were synthesized for purifying metronidazole(MNZ)via PDS activation.As an efficient Fentonlike catalyst for PDS activation,2 wt%Fe-doped VO_(2)can remove 98%of MNZ within 40 min and exhibits impressive recyclability.The synergistic effect of Fe-VO_(2)and Fe(Ⅲ)activated PDS boosted the photocatalytic performance.Moreover,SO_(4)•^(−),h+,O_(2)•^(−),^(1)O_(2),and•OH were the main reactive radicals.The effects of initial MNZ concentration,Fe-VO_(2),PDS dosage,and various anions/cations on MNZ removal by the Fe-VO_(2)/PDS/Vis system were studied.The intermediates of MNZ degradation and possible pathways were determined by density function theory(DFT)calculations and HPLC-MS.This study provided a sustainable technology using Fe-doped ultrathin VO_(2)nanobelts for photocatalytic PDS activation and decontamination of pharmaceutical wastewater.
基金supported by the National Natural Science Foundation of China (32122059)the National Key R&D Program of China(2021YFD2200402)+5 种基金the Chinese Academy of Sciences Young Talents Programthe LiaoNing Revitalization Talents Program (XLYC2007016) to QWW2024 Joint Fund Project Funding Program (2023-MSBA-137) to JJDChinese Academy of Sciences President's International Fellowship Initiative (2022VCA0010)the Japan Society for the Promotion of Science (KAKENHI,17F17403) to QWW and HKAcademy of Finland Project(324555) to TMR
文摘Photodegradation is considered as a universal contributing factor to litter decomposition and carbon(C)cycling within the Earth’s biomes.Identifying how solar radiation modifies the molecular structure of litter is essen-tial to understand the mechanism controlling its decom-position and reaction to shifts in climatic conditions and land-use.In this study,we performed a spectral-attenuation experiment following litter decomposition in an understory and gap of a temperate deciduous forest.We found that short-wavelength visible light,especially blue light,was the main factor driving variation in litter molecular struc-ture of Fagus crenata Blume,Quercus crispula Blume,Acer carpinifolium Siebold&Zuccarini and Betula platyphylla Sukaczev,explaining respectively 56.5%,19.4%,66.3%,and 16.7%of variation in its chemical composition.However,the variation also depended on canopy openness:Only in the forest gap was lignin aromatic C negatively associated with C-oxygen(C–O)bonding in polysaccharides receiv-ing treatments containing blue light of the full spectrum of solar radiation.Regardless of species,the decomposition index of litter that explained changes in mass and lignin loss was driven by the relative content of C–O stretching in poly-saccharides and lignin aromatic C.The results suggest that the availability of readily degradable polysaccharides pro-duced by the reduction in lignin aromatic C most plausibly explains the rate of litter photodegradation.Photo-products of photodegradation might augment the C pool destabilized by the input of readily degradable organic compounds(i.e.,polysaccharides).
基金Funded by the National Natural Science Foundation of China(Nos.52102110 and 42272355)the China Postdoctoral Science Foundation(No.2023M732724)。
文摘Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composite was evaluated using the degradation of rhodamine B(RhB)and tetracycline hydrochloride(TCH)under visible light.The results demonstrated that Ti_(3)C_(2)/BOC composite had higher photocatalytic activity than pure BOC.The optimum incorporation amount of Ti_(3)C_(2) was 2 wt%.The photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC at 10 min to 20 mg/L RhB was 97.6%,which was much higher than that of BOC(75.3%).Similarly,the photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC to 10 mg/L TCH at 30 min was 80.4%,which was higher than BOC(68.1%).In addition,the prepared 2 wt%-Ti_(3)C_(2)/BOC composite also maintained good stability even after four cycles.Electrochemical impedance spectroscopy(EIS),transient photocurrent response(IT)and ultraviolet-visible diffuse reflectance spectroscopy(UV-vis)confirmed that the photoelectrochemical properties of 2 wt%-Ti_(3)C_(2)/BOC composite were significantly improved.On the basis of analyzing the action mechanism of photocatalyst,it was pointed out that·O_(2)^(-)and h~+were the main active substances in the photodegradation of RhB and TCH by 2 wt%-Ti_(3)C_(2)/BOC.
基金supported by the National Key Research and Development Program of China(No.2023YFF0612601)the Key Research and Development Program of Zhejiang Province(No.2023C02038)+3 种基金the Key Research and Development Program of Ningbo(No.2022Z178)China Construction Technology Research and Development Project(No.CSCEC-2021-Z-5)Zhejiang Provincial Natural Science Foundation of China(No.LQ23B010003)the Open Research Fund Program of Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang Province(No.SISPM-2022-03).
文摘Lead-free halide perovskite material has drawn fast-growing interest due to its superiorsolar-conversion efficiency and nontoxic nature. In this work, we have successfully fabricatedcesium silver bismuth bromide (Cs2AgBiBr6) quantum dots utilizing the hot injectionmethod. The as-synthesized quantum dots were characterized by combined techniques,which showed remarkable visible-light photocatalytic activity for organic dyes and antibioticdegradation in ethanol. Specifically, about 97% of rhodamine B and methyl orange maybe removed within 10 min and 30 min, respectively. Additionally, 60% of antibiotic residueof tetracycline hydrochloride is degraded in 30min which is 7 times more than that on commercialtitania (P25). The reactive species for the photodegradation are determined throughcapture experiments, and a reaction mechanism is proposed accordingly. This work providesa novel photocatalyst for the selective removal of diverse organic contaminants inethanol and an alternative for the potential application of lead-free halide perovskites.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.21901018,21971024,22271021)the Natural Science Foundation and Education Department of Liaoning province(Nos.2022-MS-373,2021-MS-312,LJ2020008).
文摘The widespread application of phenolic substances in the field of food,medicine and industry,is harmful to the environment and human health.Therefore,it is very important to develop a con-venient and effective method to detect and degrade phenolic compounds.Herein,we report a new keggin-type polyoxometallate-based metal-organic complex self-assembled under solvothermal condition,{[Cu(dap)(3-PA)]4(SiW_(12)O_(40))(H_(2)O)_(2)}·2H_(2)O(1,dap=1,2-diaminopropane,3-HPA=3-pyridineacrylic acid).1 shows an interesting 1D ladder-like structure.As a bifunctional catalyst,1 can be employed as a colori-metric sensor toward phenol with the relatively low detection limit(LOD)of 0.36μmol/L(S/N=3)in the wide range(0.001-0.1 mmol/L).The title colorimetric sensor is applied to determine phenol in various water environment with good recoveries ranging from 95%-105%.In addition,1 also exhibits excellent photocatalytic degradation toward phenol under visible light with the highest removal efficiency at 96%for 100 min and wide pH universality.The selectivity,stability and reliability of the detection of 1 towards phenol,as well as the detection for 4-chlorophenol,o-cresol,4-nitrophenol and phloroglucinol were stud-ied.Furthermore,the photocatalytic reaction kinetics and the mechanisms of photodegradation of phenol were also investigated in detail.
基金supported by the Natural Science Foundation of Shenzhen(No.GXWD20201230155427003-20200802110025006)the National Natural Science Foundation of China(Nos.52170157 and 52111530188)+3 种基金the Major Program of Jiangxi Provincial Depart-ment of Science and Technology(No.2022KSG01004)the Natural Science Foundation of Shenzhen(No.JCYJ20220531095408020)the Start-up Grant Harbin Institute of Technology(Shenzhen)(No.IA45001007)the Start-up Talent Grant at Harbin Institute of Technology(Shenzhen)(No.HA11409066).
文摘The edge-graphitized carbon nitride(C_(3)N_(4)-C g)was prepared by secondary pyrolysis to construct ZnO/C_(3)N_(4)-C g(ZCN)type-Ⅱheterojunction photocatalyst via a facile sonication dispersion method,which achieved∼7.04-fold and∼18.3-fold enhanced visible-light-driven photocatalytic performance for refrac-tory micropollutant removal and simultaneous hydrogen(H_(2))evolution respectively compared to con-ventional ZnO/g-C_(3)N_(4)Step-scheme heterojunction.The apparent quantum efficiency of the ZCN_(0.4)het-erojunction reaches 0.92%(λ=420 nm).Such excellent performance stems from that the edge-graphene moieties stitched onto the interface of heterojunction extend light absorption to the full visible spec-trum,meanwhile,the built-in electric field generated during Fermi level alignment accompanying fa-vorable band-bending structure provides an effective pathway for the rapid migration of photoinduced electrons via the edge graphene channel to improve interfacial charge separation efficiency.Interestingly,the midgap states introduced in ZCN heterojunction could temporarily retain photoexcited electrons to effectively inhibit the in situ carrier recombination for improved photocatalytic H_(2)evolution.Moreover,ZCN/peroxymonosulfate system exhibited excellent anti-interference performance against complex water bodies under visible illumination due to the synergistic effect between the co-existing anions and organic matter.Meanwhile,the eco-friendly nature of the ZCN/peroxymonosulfate system showed no biotoxicity of reaction filtrate on cell proliferation after treatment,which avoided secondary contamination.Consid-ering the outstanding performance in photocatalysis,the ZCN system exhibits broad potential for practical applications in water pollution control and green energy production.
基金supported by the National Natural Science Foundation of China (No.21906085)the Natural Science Foundation of Jiangsu Province of China (No.BK20190547)the State Key Laboratory of Pollution Control and Resource Reuse Foundation (No.PCRRF21046)。
文摘Inactivation of cyanobacterial cells and simultaneous control of secondary metabolites is of significant necessity for the treatment of cyanobacteria-laden water.Acetylacetone(AcAc)has been reported a specific algicide to inactivate Microcystis aeruginosa(M.aeruginosa)and an effective light activator to degrade pollutants.This study systematically investigated the photodegradation ability of AcAc under xenon(Xe)irradiation on the secondary metabolites of M.aeruginosa,mainly algal organic matter(AOM),especially toxic microcystin-LR(MC-LR).Results showed that AcAc outperformed H_(2)O_(2)in destructing the protein-like substances,humic acid-like matters,aromatic proteins and fulvic-like substances of AOM.For MC-LR(250μg/L),0.05 mmol/L AcAc attained the same degradation efficiency(87.0%)as 0.1mmol/L H_(2)O_(2).The degradation mechanism of Xe/AcAc might involve photo-induced energy/electron transfer and formation of carbon center radicals.Alkaline conditions(pH>9.0)were detrimental to the photoactivity of AcAc,corresponding to the observed degradation rate constant(k_(1)value)of MC-LR drastically decreasing to 0.0013 min^(-1)as solution pH exceeded 9.0.The PO_(4)^(3-)and HCO_(3)^(-)ions had obvious inhibition effects,whereas NO_(3)^(-)slightly improved k_(1)value from 0.0277 min^(-1)to 0.0321 min^(-1).The presence of AOM did not significantly inhibit MC-LR degradation in Xe/AcAc system.In addition,the biological toxicity of MC-LR was greatly reduced after photoreaction.These results demonstrated that AcAc was an alternative algicidal agent to effectively inactivate algal cells and simultaneously control the secondary metabolites after cell lysis.Nevertheless,the concentration and irradiation conditions should be further optimized in practical application.
文摘La,Ce co-doped ZnO nanorods(ZnLC)were synthesized through a one-step solvothermal route.The photocatalysts were characterized by X-ray diffraction,Raman spectroscopy,field-emission scanning electron microscopy,energy dispersive X-ray,transmission electron microscopy,UV-vis diffuse reflectance spectroscopy and photo luminescence spectroscopy.The La and Ce doping enhanced the visible light absorption ability of ZnLC and a red shift was detected for ZnLC.Under simulated solar light irradiation,the ZnO doped with 3 at%La and 1 at%Ce(ZnLC1)degrades methylene blue(MB)more effectively than those of pure ZnO,La-doped ZnO(ZnL)and commercially available ZnO.The improved photocatalytic performance of ZnLC1 can be attributed to the high charge separation efficiency as demonstrated by the photoluminescence spectra.Additionally,the photocatalytic experiments reveal that several parameters have their own impact on the MB degradation.Using a variety of radical scavengers,it is discovered that superoxide anion radical plays a crucial role in the degradation of MB.The ZnLC1 is also reused several times without noticeable decrease of photoactivity,indicating that it has a substantial potential for environmental remediation applications.
基金supported by the National Natural Science Foundation of China (Nos.42177354 and 21777032)the National Key R&D Program of China (No.2019YFC0214402)the Guangdong Basic and Applied Basic Research oundation (No.2019B151502064)。
文摘Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.
基金National Natural Science Foundation of China(Nos.51902282 and 12274361)Qinglan Project of Jiangsu of China,the Natural Science Foundation of Jiangsu Province(No.BK20211361)College Natural Science Research Project of Jiangsu Province(No.20KJA430004).
文摘Developing high-efficiency photocatalysts for tetracycline hydrochloride(TCH)degradation is of great sig-nificance to ecosystems and human beings.In this work,a two-step process of exfoliation and re-stacking was performed to prepare re-stacked HTiNbO_(5) nanosheets(R-HTNS)and then coupled with Ti_(3)C_(2) MXene to construct Ti_(3)C_(2) MXene/R-HTNS(MX/RTS)with a 2D/2D Schottky heterojunction.These 2D/2D het-erostructures between Ti_(3)C_(2) MXene and R-HTNS can produce an internal electric field and provide max-imum interface area for efficient charge transfer across the intimate interface.The photocatalytic perfor-mance of samples was evaluated by TCH degradation under simulated sunlight.The MX/RTS composites,with an optimal sample of 3-MX/RTS,show enhanced photocatalytic activity for TCH degradation com-pared with R-HTNS.The characterization results reveal that the introduction of Ti_(3)C_(2) MXene can signif-icantly increase specific surface area for providing more reactive sites and broaden the light absorption region.Besides,the incident light energy is absorbed by the Ti_(3)C_(2) MXene component in MX/RTS compos-ites to generate photothermal energy(heat),which facilitates the charge carrier separation and surface reaction kinetics.Thus,the enhanced TCH photodegradation activity for MX/RTS composites is due to the introduction of Ti_(3)C_(2) MXene,which possesses the synergistic effect of the increased specific surface area,improved light-harvesting capacity,2D/2D Schottky heterojunction,and photothermal energy effect.Additionally,the TCH photodegradation behavior is deliberated with a detailed discussion on various co-existing ions.During TCH photodegradation,the active radical species are determined for 3-MX/RTS.Ac-cording to the characterization results,the possible TCH photodegradation pathway and mechanism over 3-MX/RTS are explored.This work may offer a novel insight for constructing MXene-based heterostruc-tured photocatalysts with high efficiency.
基金The Vietnam National Foundation for Science and Technology Development(NAFOSTED)and the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(Grant No.NRF-2022R1A2C1012996)。
文摘Environmental pollution,such as water contamination,is a critical issue that must be absolutely addressed.Here,three different morphologies of tungsten-based photocatalysts(WO_(3)nanorods,WO_(3)/WS_(2)nanobricks,WO_(3)/WS_(2)nanorods)are made using a simple hydrothermal method by changing the solvents(H_(2)O,DMF,aqueous HCl solution).The as-prepared nanocatalysts have excellent thermal stability,large porosity,and high hydrophilicity.The results show all materials have good photocatalytic activity in aqueous media,with WO_(3)/WS_(2)nanorods(NRs)having the best activity in the photodegradation of bisphenol A(BPA)under visible-light irradiation.This may originate from increased migration of charge carriers and effective prevention of electron–hole recombination in WO_(3)/WS_(2)NRs,whereby this photocatalyst is able to generate more reactive·OH and·O_(2)^(–)species,leading to greater photocatalytic activity.About 99.6% of BPA is photodegraded within 60 min when using 1.5 g/L WO_(3)/WS_(2)NRs and 5.0 mg/L BPA at pH 7.0.Additionally,the optimal conditions(pH,catalyst dosage,initial BPA concentration)for WO_(3)/WS_(2)NRs are also elaborately investigated.These rod-like heterostructures are expressed as potential catalysts with excellent photostability,efficient reusability,and highly active effectivity in different types of water.In particular,the removal efficiency of BPA by WO_(3)/WS_(2)NRs reduces by only 1.5% after five recycling runs and even reaches 89.1%in contaminated lake water.This study provides promising insights for the nearly complete removal of BPA from wastewater or different water resources,which is advantageous to various applications in environmental remediation.
文摘In dye-photocatalysis, widening the wavelengths absorption range of catalysts as well as aborting the recombination of the photoexcited charge carriers(electrons-holes pairs) are of paramount significance.In the current study, we report the photocatalytic characteristics of four compositions composed of TiO_(2),Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders for two harmful dyes(Congo red and methylene blue). The X-ray diffraction technique verified the configuration of mixed anatase and rutile phases in pure TiO_(2)and Ti_(0.97)Cu_(0.03)O_(2)powders while Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders possess anatase phase only. The changes of the band gap structure and dimensions of the unit cell volume of TiO_(2)confirm the substitution of Ti^(4+)sites by Cu^(2+)and La^(3+)ions. Remarkable widening of wavelengths absorption with formation of long absorption tails were found in TiO_(2)(3.13 e V) through insertion of La^(3+)plus Cu^(2+)ions. Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)samples exhibit a visible light band gap of 2.3 and 2.7 e V, respectively. Based on SEM images, incorporation of Cu^(2+)and La^(3+)ions influences the surface morphology of TiO_(2). The resulting Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders present enhanced photocatalytic activity towards Congo red dye degradation compared to pure one under natural solar spectrum. The best Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst exhibits superior photocatalytic activity of 96% for 10 ppm CR dye in 20 min as well as above average photocatalytic efficiency of 63% for 30 ppm CR dye in 120 min. As well, it showed acceptable photodegradation activity of 52% for 30 ppm MB solution in 140 min of sunlight irradiation. The heightened photodegradation efficiency of Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst can be clarified in terms of higher charge carriers' separation(Cu^(2+)+ e-→ Cu^(+), La^(3+)+ e-→ La^(2+)), oxygen vacancies, full anatase phase structure as well as the wide range of visible light absorption.
基金supported by the Foundation of Science Re-search Program from the Hubei Provincial Department of Ed-ucation(No.Q20221711)the Program ofWuhan Research Center of Ecodyeing&Finishing and Functional Textile(No.EDFT2021002).
文摘Semiconductor heterojunction engineering and three-dimensional(3D)architecture con-struction have been considered highly desirable strategies to enhance photocatalytic perfor-mance.Herein,a BiOI/ZnO composite photocatalyst with a 3D flower-like architecture was successfully prepared,whichwas stably immobilized on three-dimensional porous lignocel-lulosic biomass Juncus effusus(JE)fiber.The outstanding photocatalytic performance of the BiOI/ZnO-JE fiber was confirmed by the degradation of tetracycline hydrochloride(TC,90%),ciprofloxacin(CIP,79%),and norfloxacin(NOR,81%).The enhanced photocatalytic activities were mainly attributed to the synergistic absorption performance of the lignocellulosic JE and the effective transfer and separation of charges.Moreover,the hydroxyl(·OH)and super-oxide radicals(·O_(2)^(−))are themain reactive species in the photocatalytic process according to the analysis.This work may provide a novel perspective for constructing high-performance lignocellulosic-based photocatalytic materials.
基金supported by the Project of the State Key Laboratory of Pollution Control and Resource Reuse Foundation,Nanjing University(No.PCRRF21012)。
文摘We investigated the influence mechanism of N-doping for dissolved black carbon(DBC)photodegradation of organic pollutants.The degradation performance of N-doped dissolved black carbon(NDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under irradiation.These levels are both better than DBC degradation performances for TC(68%)and MB(18%)under irradiation.Reactive species quenching experiments suggest that h and-O,are the main reactive species for NDBC photodegraded TC,while-OH and h*are the main reactive species for NDBC photodegraded MB.-OH is not observed during DBC photodegradation of MB.This is likely because N-doping increases valence-band(VB)energy from 1.55 eV in DBC to 2.04 eV in NDBC;the latter is strong enough to oxidize water to form-OH.Additionally,N-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC,resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in DBC.AIl these factors give NDBC stronger photodegradation performance for TC and MB than DBC.High-performance liquid chromatography-mass spectrometry(HPLC-MS)characterization and toxicity evaluation with the quantitative structure-activity relationship(QSAR)method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by DBC.We adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species produced.Our results add to the understanding of the photochemical behavior of NDBC.
基金supported by the Hunan Provincial Natural Science Foundation of China(No.2021JJ30728 and 2019JJ50672)the Scientific Research Projects of Ecology and Environment Department of Hunan(No.HBKT-2021012)the Water Conservancy Science and Technology Project of Hunan Province(Nos.XSKJ2022068-03 and XSKJ2019081-46)are highly appreciated。
文摘It is important to investigate whether combining two modification strategies has a synergistic effect on the activity of photocatalysts.In this manuscript,Fe-doped BiOBr/Bi_(2)WO_(6) heterojunctions were synthesized by a one-pot solvothermal method,and excellent photocatalytic performance was obtained for the degradation of tetracycline hydrochloride(TCH)in water without the addition of surfactant.Combining experiments and characterization,the synergistic effect between Fe ion doping and the BiOBr/Bi_(2)WO_(6) heterojunction was elucidated.The Fe/BiOBr/Bi_(2)WO_(6) composite photocatalyst had a beneficial void structure,enhanced visible light response,and could inhibit the recombination of photogenerated support well,which improved the photocatalytic activity.The presented experiments demonstrate that Fe/BiOBr/Bi_(2)WO_(6) removes 97% of TCH from aqueous solution,while pure BiOBr and Bi_(2)WO_(6) only remove 56% and 65% of TCH,respectively.Finally,the separation and transfer mechanisms of photoexcited carriers were determined in conjunction with the experimental results.This study provides a new direction for the design of efficient photocatalysts through the use of a dual co-modification strategy.
基金supported by the National Natural Science Foundation of China(Nos.22176145,82172612)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2001)the Fundamental Research Funds for the Central Universities(22120210137).
文摘The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
基金supported by the Anhui Provincial Natural Science Foundation of China(No.1508085SME219).
文摘Constructing new photocatalysts for the photocatalytic reduction of CO_(2)and efficient degradation of Lev-ofloxacin is of great importance to renewable energy.Here,S-scheme Bi_(2)MoO_(6-x)/MoS_(2)heterojunction nanospheres containing abundant surface defects(oxygen vacancies)were designed and successfully syn-thesized to enhance CO_(2)photoreduction activity in the absence of other sacrificial agents,co-catalysts or photosensitisers.At the same time,it can efficiently degrade organic pollutants(Levofloxacin).This heterogeneous structure with surface defects provides an abundance of reactive sites,accelerates charge separation and improves oxidation capacity.The improved Bi_(2)MoO_(6-x)/MoS_(2)heterogeneous nanospheres show excellent performance under simulated solar light,with the selectivity and yield of 92.45%and 29.01μmol h^(−1),respectively,for the generation of CO.Under visible light,the degradation efficiency of levofloxacin hydrochloride(LVX)reached 96.3%within 25 min and remained as high as 95%after three cycles.This work provides a new idea for the design of new S-scheme photocatalysts and an important reference for the preparation of photocatalysts for the efficient photocatalytic reduction of CO_(2)and the efficient degradation of organic pollutants at the same time.
