By virtue of genetic engineering technology,we developed a highly sensitive biosensor for tetracycline detection based on the interaction between the tetracycline regulator TetR and tetracycline.In the absence of tetr...By virtue of genetic engineering technology,we developed a highly sensitive biosensor for tetracycline detection based on the interaction between the tetracycline regulator TetR and tetracycline.In the absence of tetracycline,TetR binds to the tetO sequence,inhibiting the expression of the sfGFP reporter gene.When tetracycline is present,it induces TetR to release from tetO,allowing sfGFP expression.The biosensor was optimized through the selection of transcription factors and reporter genes,and the optimization of spacer lengths.Chassis cells were grown to mid-log phase in a tetracycline-supplemented medium for subsequent fluorescence intensity measurement.The biosensor exhibited a strong linear correlation between fluorescence intensity and tetracycline concentration(I=37,620.7×[C(Tc)]+4048.5,R^(2)=0.998),demonstrating high sensitivity with a detection limit of 0.0097 mg/L.The response time of the biosensor ranged from 2 to 4 h within the working concentration range,making it suitable for real-time detection.It shows potential for application in actual water sample analysis and as an early warning technology for water pollution risks.展开更多
In this study,a nickel-based MOF{(NH_(2)(CH_(3))_(2))_(2)[Ni_(3)(O)(L)3(NH(CH_(3))_(2))_(3)]}_(n)(Ni_(3)-MOF),with pore sizes of approximately 1.6 nm×1.6 nm,was synthesized by reacting 4,4′-biphenyldicarboxylic ...In this study,a nickel-based MOF{(NH_(2)(CH_(3))_(2))_(2)[Ni_(3)(O)(L)3(NH(CH_(3))_(2))_(3)]}_(n)(Ni_(3)-MOF),with pore sizes of approximately 1.6 nm×1.6 nm,was synthesized by reacting 4,4′-biphenyldicarboxylic acid(H_(2)L)with Ni(NO_(3))_(2)·6H_(2)O in an N,N-dimethylformamide(DMF)solution.The nanoscale adsorbent Ni_(3)-MOF-N with a particle diameter of approximately 200 nm was prepared using Ni_(3)-MOF.It exhibited a maximum equilibrium tetracycline(TC)adsorption capacity of 358.2 mg·g^(-1)at its isoelectric point(pH=6.50),outperforming most reported MOF-based adsorbents.This exceptional performance is likely attributed to the well-matched pore size of Ni_(3)-MOF-N(1.6 nm×1.6 nm)and the molecular dimensions of TC(0.8 nm×1.2 nm),combined with the presence of partial Ni(Ⅱ)sites on the surface of Ni_(3)-MOF-N.These features collectively facilitate effective TC adsorption through a combination of pore filling,electrostatic attraction,hydrogen bonding,surface complexation,andπ-πinteractions.Recycling experiments demonstrated that Ni_(3)-MOF-N possesses excellent structural stability and consistent adsorption performance.CCDC:2481791,Ni_(3)-MOF.展开更多
To overcome the limitations of traditional photocatalysts,such as inefficient separation of charge carriers and poor visible-light absorption,S-scheme g-C_(3)N_(4)/TiO_(2) heterojunction photocatalysts were synthesize...To overcome the limitations of traditional photocatalysts,such as inefficient separation of charge carriers and poor visible-light absorption,S-scheme g-C_(3)N_(4)/TiO_(2) heterojunction photocatalysts were synthesized via a combined method of thermal polymerization,hydrothermal synthesis,and calcination.The crystal structures,morphological features,and optical properties of the composites were systematically characterized,and their photocatalytic performance was evaluated through tetracycline(TC)degradation and hydrogen evolution experiments.Trapping experiments and electron paramagnetic resonance(EPR)measurements were conducted to elucidate the reaction mechanisms.The results demonstrate that the S-scheme heterojunction effectively extends the visible-light absorption range and facilitates the efficient separation of photogenerated electron-hole pairs.Under optimal conditions,the composite achieved a TC degradation rate of 94.5%and a hydrogen evolution rate of 329.1μmol·h^(-1)·g^(-1) after 8 h of irradiation,both values being significantly higher than those of pristine g-C_(3)N_(4) or TiO_(2).Moreover,the S-scheme g-C_(3)N_(4)/TiO_(2) heterojunction retained high photocatalytic activity over five consecutive cycles,confirming its excellent stability.Mechanistic investigations revealed that the S-scheme heterojunction maintained strong redox capacities,with superoxide radicals(·O_(2)^(-)),hydroxyl radicals(·OH),electrons(e-),and holes(h+)serving as the primary active species responsible for TC degradation and H2 production.展开更多
In this work,we constructed a three-dimensional electrochemical system(3D-ECO),which included the cathode and anode electrode plates,as well as the screening of three-dimensional particle electrodes and parameter opti...In this work,we constructed a three-dimensional electrochemical system(3D-ECO),which included the cathode and anode electrode plates,as well as the screening of three-dimensional particle electrodes and parameter opti-mization,for the degradation of landfill leachate(LL)containing elevated levels of tetracycline(TC),and explored its mechanism of action.Firstly,titanium-based ruthenium-iridium(Ti/RuO_(2)-IrO_(2)),titanium-based ruthenium-iridium-platinum(Ti/Pt-RuO_(2)-IrO_(2)),and titanium-based tin-antimony(Ti/SnO_(2)-Sb_(2)O_(3))were employed as an-odes in the electrocatalytic oxidation system,with titanium and stainless steel plates serving as cathodes,to construct the optimal two-dimensional electrocatalytic oxidation system(2D-ECO)through cross-comparison ex-periments.Subsequently,using granular activated carbon(GAC),coconut shell biochar(CBC),walnut shell carbon(WBC),and bamboo charcoal(BBC)as particle electrodes,a 3D-ECO system was developed.The influence of var-ious operational parameters on treating TC-containing LL was investigated.The optimal operating parameters obtained from the study was:pH=5,current density of 30 mA/cm^(2),particle dosage of 7 g/L,particle size ranging from 1.70 to 2.00 mm,and electrode spacing of 4 cm.Under these conditions,the COD removal rate of 3D-ECO within three hours was 90.25%,the TC removal rate was 72.41%,and the NH_(3)-N removal rate was 39.52%.The removal of TC followed a pseudo-first-order kinetic model.Additionally,degradation mechanisms were elucidated through electron paramagnetic resonance(EPR)spectrometer and Tert-Butanol(TBA)quenching experiments,indicating that the degradation primarily occurred through a non-radical(1O_(2))pathway.This re-search offers a comprehensive analysis of the simultaneous breakdown of intricate LL matrices and TC,enhancing our comprehension of the degradation processes and underlying mechanisms.展开更多
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization w...Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.展开更多
AgVO_(3)/ZIF-8 composites with enhanced photocatalytic effect were prepared by the combination of AgVO_(3)and ZIF-8.X-ray diffraction(XRD),scanning electron microscopy(SEM),high-power transmission electron microscopy(...AgVO_(3)/ZIF-8 composites with enhanced photocatalytic effect were prepared by the combination of AgVO_(3)and ZIF-8.X-ray diffraction(XRD),scanning electron microscopy(SEM),high-power transmission electron microscopy(HRTEM),X-ray photoelectron spectroscopy(XPS),ultraviolet-visible diffuse reflectance spectroscopy(UV-Vis DRS),photoluminescence(PL)spectroscopy,electron spin resonance(ESR)spectroscopy,transient photocurrent and electrochemical impedance spectroscopy(EIS)were used to characterize binary composites.Tetracycline(TC)was used as a substrate to study the performance efficiency of the degradation of photocatalysts under light conditions,and the degradation effect of TC was also evaluated under different mass concentrations and ionic contents.In addition,we further investigated the photocatalytic mechanism of the binary composite material AgVO_(3)/ZIF-8 and identified the key active components responsible for the catalytic degradation of this new photocatalyst.The experimental results show that the degradation efficiency of 10%-AZ,prepared with a molar ratio of 10%AgVO_(3)and ZIF-8 to TC,was 75.0%.This indicates that the photocatalytic activity can be maintained even under a certain ionic content,making it a suitable photocatalyst for optimal use.In addition,the photocatalytic mechanism of binary composites was further studied by the active species trapping experiment.展开更多
Metal-organic frameworks(MOFs)and their derivatives have gained significant attention in recent years for their ability to catalyze the advanced oxidation of persulfates.Cerium-doped MOFs,in particular,have shown prom...Metal-organic frameworks(MOFs)and their derivatives have gained significant attention in recent years for their ability to catalyze the advanced oxidation of persulfates.Cerium-doped MOFs,in particular,have shown promise due to their high catalytic efficiency,practical applicability,and cost-effectiveness.However,their structure,catalytic properties,and mechanisms are not yet fully understood.ZIF-8 was chosen as the raw material to prepare cerium-doped hollow carbon nano fibers(Ce-HCNFs)using the electrostatic spinning-calcination method.The objective is to investigate the structure,catalytic performance,and catalytic mechanism of Ce-HCNFs.The results show that Ce-HCNFs catalyzed the degradation of tetracycline(TC)by persulfate up to 76.9%,Quenching experiments and electron paramagnetic resonance experiments indicate the dominant role of single-linear oxygen.Furthermore,the experiments on the influence factor and cycling demonstrate the exceptional stability and recycling capability of Ce-HCNFs in real-world water environments.展开更多
A series of CeO_(2)@MnO_(2)composites was prepared by deposition-precipitation methods.These materials were used to activate sodium persulfate(PDS)for the oxidation of tetracycline.It is found that the composites,espe...A series of CeO_(2)@MnO_(2)composites was prepared by deposition-precipitation methods.These materials were used to activate sodium persulfate(PDS)for the oxidation of tetracycline.It is found that the composites,especially the CeO_(2)@MnO_(2)-1:4 composites,exhibit better tetracycline removal rates than the pure components.X-ray diffraction(XRD),Raman and scanning electron microscopy(SEM)analyses all indicate that the composite has been successfully prepared with high purity and high crystalline.The XPS analysis shows that the strong interaction between the components promotes the electron transfer.Additionally,the kinetic rate constants of CeO_(2)@MnO_(2)-1:4 after 60 min are 3.8 and 12.7 times higher than pure CeO_(2)and MnO_(2),respectively.CeO_(2)@MnO_(2-)1:4 composite also exhibits excellent catalytic activity for individual and hybrid pollutants.The effects of wastewater matrix,pH,circulation and ion stre ngth on the degradation of tetracycline were investigated.It is found that CeO_(2)@MnO_(2)-1:4 composite has good practical application prospects.CeO_(2)@MnO_(2)composites with synergistic adsorption catalysis can activate PDS and peroxymo no sulfate(PMS)for efficient organic catalytic oxidation.This paper provides the theoretical basis and data support for the practical application of the CeO_(2)@MnO_(2)composite materials.展开更多
Tetracycline(TC)is a broad-spectrum antibiotic,and its residues in the environment and food are harmful to human health.Therefore,it is essential to rapidly,sensitively,and conveniently detect TC.In this work,we devel...Tetracycline(TC)is a broad-spectrum antibiotic,and its residues in the environment and food are harmful to human health.Therefore,it is essential to rapidly,sensitively,and conveniently detect TC.In this work,we developed a portable silicon nanoparticles chelated Europium(Ⅲ)-based polyacrylonitrile(Eu-SiNPs/PAN)nanofiber membrane for rapid,sensitive,and convenient detection of TC.The Eu-SiNPs were synthesized with a facile one-pot method.The Eu-SiNPs/PAN nanofiber membrane was fabricated by electrospinning,combining Eu-SiNPs and PAN with three-dimensional porous membrane structures and UV resistance.Both the Eu-SiNPs and the Eu-SiNPs/PAN nanofiber membranes have good selectivity and anti-interference ability towards TC.The combined merits of rapid response,long storage life,easy portability,and naked-eye recognition of TC make the Eu-SiNPs/PAN nanofiber membrane a promising material for convenient TC detection applications.The practicability of these nanofiber membranes was further verified by detecting TC in real samples,such as lake water,drinking water and honey,and achieved quantitative detection.展开更多
A novel nitrogen-doped graphene(NG)supporting magnetic nanoparticles(Fe and Fe_(3)C)was synthesized from g-C_(3)N_(4)and Fe(C_(5)H_(5))_(2).When used as a photocatalyst exposed to visible light,the material was excell...A novel nitrogen-doped graphene(NG)supporting magnetic nanoparticles(Fe and Fe_(3)C)was synthesized from g-C_(3)N_(4)and Fe(C_(5)H_(5))_(2).When used as a photocatalyst exposed to visible light,the material was excellent in degrading tetracycline(TC)in aqueous solutions.Scanning electron microscopy indicated that it had a folded sheet structure,with numerous nanoparticles observed on graphene sheets.Raman spectroscopy confirmed the presence of significant defects in the material,which suppressed the recombination of photogenerated electron-hole pairs.The performance and degradation mechanism of the photocatalyst was verified using a series of optical and electrochemical experiments and theoretical calculations.The degradation efficiency of the catalyst for TC was as high as 97.1%in 120 min under visible light irradiation,which is superior to other reported catalysts.A mechanism study showed that TC is rapidly degraded into CO_(2),H_(2)O and other small inorganic molecules,with holes(h^(+))serving as the primary driving force.The catalyst had an outstanding stability and reusability,and could be easily recovered using an external magnetic field.展开更多
Herein,a luminescent europium-based metal-organic framework(Eu-MOF,[Eu_(3)(L)(HL)(NO_(3))_(2)(DMF)_(2)]·4DMF·5H_(2)O,H_(4)L=5,5′-(pyrazine-2,6-diyl)diisophthalic acid,DMF=N,N-dimethylformamide)was developed...Herein,a luminescent europium-based metal-organic framework(Eu-MOF,[Eu_(3)(L)(HL)(NO_(3))_(2)(DMF)_(2)]·4DMF·5H_(2)O,H_(4)L=5,5′-(pyrazine-2,6-diyl)diisophthalic acid,DMF=N,N-dimethylformamide)was developed for the dual-functional detection of environmental pollutants.This fluorescence-quenching-based sensor exhibited excep-tional sensitivity for both 2,4,6-trinitrophenol(TNP)and tetracycline(TC),achieving remarkably low detection lim-its of 1.96×10^(-6)and 1.71×10^(-7)mol·L^(-1),respectively.Notably,the system exhibited 99%fluorescence quenching ef-ficiency for TC,indicating ultra-efficient analyte recognition.The detection performance surpasses most reported lu-minescent MOF sensors,attributed to synergistic mechanisms of fluorescence resonance energy transfer(FRET)and photoinduced electron transfer(PET).CCDC:2446483.展开更多
The synergetic technology of hydrodynamic cavitation(HC)and peroxydisulfate(PDS)has been adopted for the treatment of organic pollutants,while the rationale behind the thermal-activation of PDS in this process remains...The synergetic technology of hydrodynamic cavitation(HC)and peroxydisulfate(PDS)has been adopted for the treatment of organic pollutants,while the rationale behind the thermal-activation of PDS in this process remains lacking.This paper presented investigation on the degradation of tetracycline under two types of operating conditions,including“internal reaction conditions”(pH value and TC/PDS molar ratio)and“external physical conditions”(hole shape,solution temperature and inlet pressure).Special emphasis was paid on the analysis of thermal effects through a robust modeling approach.The results showed that a synergy index of 6.26 and a degradation rate of 56.71%could be obtained by the HC-PDS process,respectively,when the reaction conditions were optimized.Quenching experiment revealed that·OH and·SO_(4)^(-)were the predominant free radicals and their contribution to the degradation was 75.4%and 24.6%respectively,since a part of·SO_(4)^(-)was transformed into·OH in the solution.The thermal activation of PDS mainly occurred near the hole where the fitting temperature was around 340 K,while·OH was generated in the bubble collapse region downstream the hole,where the temperature was much higher and favorable for the cleavage of water molecular.The average temperature under different external physical conditions was in good consistence with the degradation rates.This research developed a useful method to effectively evaluate the activation extent of PDS by HC and could provide reliable guidance for further development of cavitational reactors to treat organic pollutants based on this hybrid approach.展开更多
Tetracyclines (TCs) are the second most commonly used antibiotics worldwide, utilized in medical treatments and animal husbandry. Although effective against various infectious diseases, TC residues persist in the envi...Tetracyclines (TCs) are the second most commonly used antibiotics worldwide, utilized in medical treatments and animal husbandry. Although effective against various infectious diseases, TC residues persist in the environment and contribute to the emergence of antibiotic-resistant pathogens, posing significant risks to human health. This study employed the heterogeneous Fenton process to degrade TC using soybean residue-derived magnetic biochar (Fe-SoyB) as the catalyst. The Fe-SoyB sample was characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and superconducting quantum interference device (SQUID) techniques. The effects of key parameters, including pH, H2O2 concentration, catalyst dosage, and initial TC concentration, on TC degradation were investigated. The results indicated that the TC removal efficiency decreased with increasing initial TC concentration, while it was improved with higher H2O2 concentrations and greater catalyst dosages. The optimal conditions for the Fenton-like process were determined: a pH of 3, a H2O2 concentration of 245 mmol/L, an initial TC concentration of 800 mg/L, and a catalyst dosage of 0.75 g/L, achieving a removal efficiency of 90.0% after 150 min. Additionally, the TC removal efficiency of the Fe-SoyB system varied significantly across different water matrices, with 87.1% for deionized water, 78.5% for tap water, and 72.5% for river water. The catalyst demonstrated notable stability, maintaining a TC removal efficiency of 79.7% after three cycles of use. Overall, Fe-SoyB shows promise as a cost-effective catalyst for the elimination of organic pollutants in aqueous solutions.展开更多
Eliminating highly concentrated antibiotic wastewater by transition metal catalyst-assisted AOPs is challenging.Herein,by varying the metal precursor composition(Co/Fe ratios of 1/1,1.5/2/3),alloyed Co_(7)Fe_(3)nanocr...Eliminating highly concentrated antibiotic wastewater by transition metal catalyst-assisted AOPs is challenging.Herein,by varying the metal precursor composition(Co/Fe ratios of 1/1,1.5/2/3),alloyed Co_(7)Fe_(3)nanocrystals or spinel-like CoFe_(2)O_(4)can be switched and both confined within the porous N-doped graphitic carbon fibers by electrospinning and controlled graphitization.Impressively,iron precursors played a dual role in working as reactive centers and main activators for the creation of porous carbon networks affording improved accessibility to catalytic sites and easy tetracycline(TC)diffusion effect.The catalytic activity of the resulting materials was closely related to surface metal valence and composition.Notably,the CoFe_(2)O_(4)exhibited a significant improvement in peroxymonosulfate(PMS)adsorption and activation,explained by the present electron-deficient Co and Fe synergetic sites together with the interesting Jahn-Teller effect.Fe_(1)Co_(2)/CNF demonstrated the highest efficiency in degrading TC,achieving a reaction rate constant of 0.4647 min^(-1)with a low activation energy of 9.3 kJ·mol^(-1),nearly a 7.5-fold enhancement compared to Fe_(1)Co_(3)/CNF(0.062 min^(-1)).The reaction mechanism and the role of reactive oxidative species revealed a synergy of·SO_(4)^(-),·OH,·O_(2)^(-)and^(1)O_(2).Wherein,·O_(2)^(-)plays a more dominant role in the degradation of TC than other reactive species.Additionally,a reinforced electron-transfer pathway in the Fe_(1)Co_(2)/CNF system during PMS interaction was demonstrated.Furthermore,the degradation routes of TC were unraveled,and the toxicity of various intermediate by-products was assessed.Importantly,our continuous flow-type TC degradation process and light-driven photothermal strengthened reaction process demonstrated consistent performance,thereby offering a promising approach for tackling highly concentrated antibiotic wastewater.展开更多
This study introduced a microwave-assisted pyrolysis method for the rapid and efficientpreparation of boron-doped porous biochar. The resulting biochar exhibited a large specificsurface area (933.39 m^(2)/g), a rich p...This study introduced a microwave-assisted pyrolysis method for the rapid and efficientpreparation of boron-doped porous biochar. The resulting biochar exhibited a large specificsurface area (933.39 m^(2)/g), a rich porous structure (1.044 cm3/g), and abundant active sites.Consequently, the prepared boron-doped porous biochar exhibited higher efficiency in adsorbingtetracycline with a maximum adsorption capacity of 413.223 mg/g, which significantlyexceeded that of unmodified biochar andmost commercial and reported adsorbents.The correlation analysis between the adsorption capacity and adsorbent characteristics revealedthat the formation of the –BCO_(2) group enhanced π–π electron donor–acceptor interactionsbetween boron-doped porous biochar and tetracycline. This mechanism mainlycontributed to the enhanced adsorption of tetracycline by boron-doped porous biochar. Additionally,the as-prepared boron-doped porous biochar exhibited broad applications in removingantibiotics (tetracycline), phenolics (bisphenol A), and dyes (methylene blue andrhodamine B). Moreover, the boron-doped porous biochar exhibited satisfactory stability,and its adsorption capacity can be nearly completely regenerated through simple heat treatment.This study provides new insights into the effectiveness of boron-doped carbonaceousmaterials in removing antibiotic contaminants.展开更多
Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were...Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.展开更多
Mariculture tailwater typically contains a certain concentration of antibiotics;however,conventional biological treatment methods struggle to effectively remove these antibiotics.Therefore,in this study,we modified th...Mariculture tailwater typically contains a certain concentration of antibiotics;however,conventional biological treatment methods struggle to effectively remove these antibiotics.Therefore,in this study,we modified the carbon felt(CF)anode in sediment microbial fuel cells(SMFCs)to enhance tetracycline(TC)removal in mariculture systems.We fabricated a novel composite material by integrating instant freeze-drying technology with the solvothermal reaction method to combine graphene oxide(GO)and nanoscale SiO_(2).Subsequently,the composite material was incorporated into CF for anodic modification,resulting in improved performance of SMFCs in TC removal and electricity generation.The maximum power density achieved was 63.72 mW/m^(2),nearly 2.9 times higher than that of the unmodified anode.Modified SMFCs exhibited a twofold increase in the degradation rate of tetracycline compared to natural degradation alone and showed significant improvements compared to both the control group and conditions with only GO addition.Furthermore,the modified anode effectively enriched populations of Leisingera,Oceanimonas,and Halomonas,thereby significantly enhancing the electrochemical performance of the SMFCs.This study successfully demonstrates the application of a modified-anode SMFC using a composite material consisting of GO and SiO_(2)for on-site removal of TC from mariculture environments.展开更多
The arbitrary discharge of tetracycline(TC)residuals has seriously influenced the ecosystem and human health.Laccase(Lac)-based biodegradation technology is considered a more effective way to remove TC due to its high...The arbitrary discharge of tetracycline(TC)residuals has seriously influenced the ecosystem and human health.Laccase(Lac)-based biodegradation technology is considered a more effective way to remove TC due to its high catalytic efficiency and less by-product.Nevertheless,free Lac suffers from poor stability,easy inactivation and difficult recovery,restricting its application.Immobilization of Lac is considered an efficient strategy for addressing these obstacles.In this study,a magnetic metal-organic framework of Fe_(3)O_(4)@SiO_(2)@UiO-66-NH_(2)(MMOF)was prepared and used as a carrier to immobilize Lac(Lac@MMOF)for TC degradation.Benefiting from the multiple binding sites,adsorption,and protection effect of MMOF,Lac@MMOF displayed a wider pH application range(2–7)and better thermal(15–85℃),repeatability,and storage stability than free Lac.Furthermore,owing to the synergism of MOF adsorption and Lac biocatalysis,the removal rate of Lac@MMOF for TC could be up to 98%at pH=7 within 1 hr,which was 1.29 and 1.24 times that of free Lac and MMOF,respectively.More importantly,Lac@MMOF could easily be separated from aqueous solution under a magnetic field and maintained good removal performance(80%)after five cycles.The degradation products were identified by applying LC-MS/MS,and possible degradation mechanisms and pathways were proposed.Finally,the antibacterial activity of intermediate products was evaluated using Escherichia coli,which revealed that the toxicity of TC was reduced effectively by the degradation of Lac@MMOF.Overall,Lac@MMOF is a green alternative for residual antibiotic removal in water.展开更多
Developing a low-cost stable and high-performance peroxymonosulfate(PMS)catalyst to degrade refractory organic pollutants is still an urgent problem.Herein,this study reported FeVO_(4)nanorods decorated sepiolite(FeVO...Developing a low-cost stable and high-performance peroxymonosulfate(PMS)catalyst to degrade refractory organic pollutants is still an urgent problem.Herein,this study reported FeVO_(4)nanorods decorated sepiolite(FeVO_(4)/sepiolite)through simple hydrothermal method as an adsorptive-catalyst for PMS activation to degrade tetracycline(TC).Benefiting from the introduction of sepiolite support,FeVO_(4)nanorods could be uniformly immobilized onto fibrous sepiolite surface.As a result,FeVO_(4)/sepiolite composite was endowed with excellent adsorption properties,rich surface hydroxyl groups,more reaction active sites,and the stable redox cycle of Fe^(3+)/Fe^(2+)and V5^(+)/V4^(+).Therefore,higher TC degradation efficiency(91.19%within 40 min)and larger reaction rate constant(0.1649 min^(-1))were obtained in FeVO_(4)/sepiolite/PMS system than in FeVO_(4)/PMS system.Besides,the composite presented good stability and reusability,and the effects of application parameters on TC degradation were investigated in detail.Through quenching experiment and electron paramagentic resonance(EPR)test,it was found that both radical and non-radical species participates in TC degradation,and ^(1)O_(2) were the main active species.The PMS activation mechanism was proposed,and the possible degradation pathway was also analyzed according to the high performance liquid chromatography-mass spectrometry(HPLC-MS)results.Overall,this work provides meaningful insights for designing natural mineral based PMS activators to effectively remediate antibiotic wastewater.展开更多
Two-dimensional luminescent metal-organic frameworks(2D LMOFs),have garnered significant attention for their unique fluorescent properties and highly accessible active sites,yet designing these LMOFs with target-depen...Two-dimensional luminescent metal-organic frameworks(2D LMOFs),have garnered significant attention for their unique fluorescent properties and highly accessible active sites,yet designing these LMOFs with target-dependent fluorescence for sensing remains a challenging endeavor.Herein,a zinc tetra(4-carboxyphenyl)porphine(Zn-TCPP)LMOF was prepared and first applied to the fast and sensitive sensing of tetracycline hydrochloride(TCH).Upon TCH exposure,the signature red fluorescence of Zn-TCPP at 609 nm diminishes,accompanied by the emergence of a 520 nm peak,which were originated from photo-induced electron transfer(PET)of Zn-TCPP to TCH and inner filter effect(IFE)of TCH towards Zn-TCPP,and the triggers of Zn-TCPP on the instinct fluorescence of TCH,respectively.Notably,the I_(520)nm/I_(609)nm fluorescence intensity ratio showed good linearity over a wide range of TCH concentrations(0.1–25μmol/L),with a limit of detection(LOD)of 65.4 nmol/L.Additionally,the Zn-TCPP probe showed good TCH selectivity and anti-interference properties.The probe's practicability was also validated by detecting TCH in spiked tap water,milk and chicken samples.Furthermore,test papers impregnated with the Zn-TCPP probe were prepared,allowing the visual detection of TCH with a smartphone.Results suggest the developed method is suitable for practical TCH detection.展开更多
基金supported by Chinese National Key Programs for Fun-damental Research and Development(No.2023YFC3709005).
文摘By virtue of genetic engineering technology,we developed a highly sensitive biosensor for tetracycline detection based on the interaction between the tetracycline regulator TetR and tetracycline.In the absence of tetracycline,TetR binds to the tetO sequence,inhibiting the expression of the sfGFP reporter gene.When tetracycline is present,it induces TetR to release from tetO,allowing sfGFP expression.The biosensor was optimized through the selection of transcription factors and reporter genes,and the optimization of spacer lengths.Chassis cells were grown to mid-log phase in a tetracycline-supplemented medium for subsequent fluorescence intensity measurement.The biosensor exhibited a strong linear correlation between fluorescence intensity and tetracycline concentration(I=37,620.7×[C(Tc)]+4048.5,R^(2)=0.998),demonstrating high sensitivity with a detection limit of 0.0097 mg/L.The response time of the biosensor ranged from 2 to 4 h within the working concentration range,making it suitable for real-time detection.It shows potential for application in actual water sample analysis and as an early warning technology for water pollution risks.
文摘In this study,a nickel-based MOF{(NH_(2)(CH_(3))_(2))_(2)[Ni_(3)(O)(L)3(NH(CH_(3))_(2))_(3)]}_(n)(Ni_(3)-MOF),with pore sizes of approximately 1.6 nm×1.6 nm,was synthesized by reacting 4,4′-biphenyldicarboxylic acid(H_(2)L)with Ni(NO_(3))_(2)·6H_(2)O in an N,N-dimethylformamide(DMF)solution.The nanoscale adsorbent Ni_(3)-MOF-N with a particle diameter of approximately 200 nm was prepared using Ni_(3)-MOF.It exhibited a maximum equilibrium tetracycline(TC)adsorption capacity of 358.2 mg·g^(-1)at its isoelectric point(pH=6.50),outperforming most reported MOF-based adsorbents.This exceptional performance is likely attributed to the well-matched pore size of Ni_(3)-MOF-N(1.6 nm×1.6 nm)and the molecular dimensions of TC(0.8 nm×1.2 nm),combined with the presence of partial Ni(Ⅱ)sites on the surface of Ni_(3)-MOF-N.These features collectively facilitate effective TC adsorption through a combination of pore filling,electrostatic attraction,hydrogen bonding,surface complexation,andπ-πinteractions.Recycling experiments demonstrated that Ni_(3)-MOF-N possesses excellent structural stability and consistent adsorption performance.CCDC:2481791,Ni_(3)-MOF.
文摘To overcome the limitations of traditional photocatalysts,such as inefficient separation of charge carriers and poor visible-light absorption,S-scheme g-C_(3)N_(4)/TiO_(2) heterojunction photocatalysts were synthesized via a combined method of thermal polymerization,hydrothermal synthesis,and calcination.The crystal structures,morphological features,and optical properties of the composites were systematically characterized,and their photocatalytic performance was evaluated through tetracycline(TC)degradation and hydrogen evolution experiments.Trapping experiments and electron paramagnetic resonance(EPR)measurements were conducted to elucidate the reaction mechanisms.The results demonstrate that the S-scheme heterojunction effectively extends the visible-light absorption range and facilitates the efficient separation of photogenerated electron-hole pairs.Under optimal conditions,the composite achieved a TC degradation rate of 94.5%and a hydrogen evolution rate of 329.1μmol·h^(-1)·g^(-1) after 8 h of irradiation,both values being significantly higher than those of pristine g-C_(3)N_(4) or TiO_(2).Moreover,the S-scheme g-C_(3)N_(4)/TiO_(2) heterojunction retained high photocatalytic activity over five consecutive cycles,confirming its excellent stability.Mechanistic investigations revealed that the S-scheme heterojunction maintained strong redox capacities,with superoxide radicals(·O_(2)^(-)),hydroxyl radicals(·OH),electrons(e-),and holes(h+)serving as the primary active species responsible for TC degradation and H2 production.
基金supported by the National Natural Science Foundation of China(Nos.42477406 and 51878617)the Horizontal Scientific Research Project(No.KYY-HX-20220803)the Engineering Research Center of Ministry of Education for Renewable Energy Infrastructure Construction Technology.
文摘In this work,we constructed a three-dimensional electrochemical system(3D-ECO),which included the cathode and anode electrode plates,as well as the screening of three-dimensional particle electrodes and parameter opti-mization,for the degradation of landfill leachate(LL)containing elevated levels of tetracycline(TC),and explored its mechanism of action.Firstly,titanium-based ruthenium-iridium(Ti/RuO_(2)-IrO_(2)),titanium-based ruthenium-iridium-platinum(Ti/Pt-RuO_(2)-IrO_(2)),and titanium-based tin-antimony(Ti/SnO_(2)-Sb_(2)O_(3))were employed as an-odes in the electrocatalytic oxidation system,with titanium and stainless steel plates serving as cathodes,to construct the optimal two-dimensional electrocatalytic oxidation system(2D-ECO)through cross-comparison ex-periments.Subsequently,using granular activated carbon(GAC),coconut shell biochar(CBC),walnut shell carbon(WBC),and bamboo charcoal(BBC)as particle electrodes,a 3D-ECO system was developed.The influence of var-ious operational parameters on treating TC-containing LL was investigated.The optimal operating parameters obtained from the study was:pH=5,current density of 30 mA/cm^(2),particle dosage of 7 g/L,particle size ranging from 1.70 to 2.00 mm,and electrode spacing of 4 cm.Under these conditions,the COD removal rate of 3D-ECO within three hours was 90.25%,the TC removal rate was 72.41%,and the NH_(3)-N removal rate was 39.52%.The removal of TC followed a pseudo-first-order kinetic model.Additionally,degradation mechanisms were elucidated through electron paramagnetic resonance(EPR)spectrometer and Tert-Butanol(TBA)quenching experiments,indicating that the degradation primarily occurred through a non-radical(1O_(2))pathway.This re-search offers a comprehensive analysis of the simultaneous breakdown of intricate LL matrices and TC,enhancing our comprehension of the degradation processes and underlying mechanisms.
基金supported byHainan Provincial Natural Science Foundation of China(Nos.422RC600,519QN175)National Natural Science Foundation ofChina(Nos.52160018,21801053,52400206,52500209)High-Level Talent Program of Hainan Province(Nos.XJ2400008202,XJ2400011473).
文摘Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.
文摘AgVO_(3)/ZIF-8 composites with enhanced photocatalytic effect were prepared by the combination of AgVO_(3)and ZIF-8.X-ray diffraction(XRD),scanning electron microscopy(SEM),high-power transmission electron microscopy(HRTEM),X-ray photoelectron spectroscopy(XPS),ultraviolet-visible diffuse reflectance spectroscopy(UV-Vis DRS),photoluminescence(PL)spectroscopy,electron spin resonance(ESR)spectroscopy,transient photocurrent and electrochemical impedance spectroscopy(EIS)were used to characterize binary composites.Tetracycline(TC)was used as a substrate to study the performance efficiency of the degradation of photocatalysts under light conditions,and the degradation effect of TC was also evaluated under different mass concentrations and ionic contents.In addition,we further investigated the photocatalytic mechanism of the binary composite material AgVO_(3)/ZIF-8 and identified the key active components responsible for the catalytic degradation of this new photocatalyst.The experimental results show that the degradation efficiency of 10%-AZ,prepared with a molar ratio of 10%AgVO_(3)and ZIF-8 to TC,was 75.0%.This indicates that the photocatalytic activity can be maintained even under a certain ionic content,making it a suitable photocatalyst for optimal use.In addition,the photocatalytic mechanism of binary composites was further studied by the active species trapping experiment.
基金Project supported by the National Natural Science Foundation of China(22206080)the Natural Science Foundation of Jiangsu(SBK2022041070)+1 种基金the Science and Technology Project of Henan Province(232102321050,232102321035)the International Science,Innovators,Technology Cooperation Projects of Henan Province(232102521009)。
文摘Metal-organic frameworks(MOFs)and their derivatives have gained significant attention in recent years for their ability to catalyze the advanced oxidation of persulfates.Cerium-doped MOFs,in particular,have shown promise due to their high catalytic efficiency,practical applicability,and cost-effectiveness.However,their structure,catalytic properties,and mechanisms are not yet fully understood.ZIF-8 was chosen as the raw material to prepare cerium-doped hollow carbon nano fibers(Ce-HCNFs)using the electrostatic spinning-calcination method.The objective is to investigate the structure,catalytic performance,and catalytic mechanism of Ce-HCNFs.The results show that Ce-HCNFs catalyzed the degradation of tetracycline(TC)by persulfate up to 76.9%,Quenching experiments and electron paramagnetic resonance experiments indicate the dominant role of single-linear oxygen.Furthermore,the experiments on the influence factor and cycling demonstrate the exceptional stability and recycling capability of Ce-HCNFs in real-world water environments.
基金Project supported by the Science and Technology Project of Henan Province(242102321048,242102321045,232102320211)National Natural Science Foundation of China(22206080)+2 种基金Natural Science Foundation of Jiangsu(SBK2022041070)International Science and Technology Cooperation Projects of Henan Province(232102521009)Natural Science Youth Foundation of Henan Province(232300420336)。
文摘A series of CeO_(2)@MnO_(2)composites was prepared by deposition-precipitation methods.These materials were used to activate sodium persulfate(PDS)for the oxidation of tetracycline.It is found that the composites,especially the CeO_(2)@MnO_(2)-1:4 composites,exhibit better tetracycline removal rates than the pure components.X-ray diffraction(XRD),Raman and scanning electron microscopy(SEM)analyses all indicate that the composite has been successfully prepared with high purity and high crystalline.The XPS analysis shows that the strong interaction between the components promotes the electron transfer.Additionally,the kinetic rate constants of CeO_(2)@MnO_(2)-1:4 after 60 min are 3.8 and 12.7 times higher than pure CeO_(2)and MnO_(2),respectively.CeO_(2)@MnO_(2-)1:4 composite also exhibits excellent catalytic activity for individual and hybrid pollutants.The effects of wastewater matrix,pH,circulation and ion stre ngth on the degradation of tetracycline were investigated.It is found that CeO_(2)@MnO_(2)-1:4 composite has good practical application prospects.CeO_(2)@MnO_(2)composites with synergistic adsorption catalysis can activate PDS and peroxymo no sulfate(PMS)for efficient organic catalytic oxidation.This paper provides the theoretical basis and data support for the practical application of the CeO_(2)@MnO_(2)composite materials.
基金supported by the Natural Science Foundation of Tianjin(Nos.18JCQNJC72400 and 22JCQNJC01510).
文摘Tetracycline(TC)is a broad-spectrum antibiotic,and its residues in the environment and food are harmful to human health.Therefore,it is essential to rapidly,sensitively,and conveniently detect TC.In this work,we developed a portable silicon nanoparticles chelated Europium(Ⅲ)-based polyacrylonitrile(Eu-SiNPs/PAN)nanofiber membrane for rapid,sensitive,and convenient detection of TC.The Eu-SiNPs were synthesized with a facile one-pot method.The Eu-SiNPs/PAN nanofiber membrane was fabricated by electrospinning,combining Eu-SiNPs and PAN with three-dimensional porous membrane structures and UV resistance.Both the Eu-SiNPs and the Eu-SiNPs/PAN nanofiber membranes have good selectivity and anti-interference ability towards TC.The combined merits of rapid response,long storage life,easy portability,and naked-eye recognition of TC make the Eu-SiNPs/PAN nanofiber membrane a promising material for convenient TC detection applications.The practicability of these nanofiber membranes was further verified by detecting TC in real samples,such as lake water,drinking water and honey,and achieved quantitative detection.
文摘A novel nitrogen-doped graphene(NG)supporting magnetic nanoparticles(Fe and Fe_(3)C)was synthesized from g-C_(3)N_(4)and Fe(C_(5)H_(5))_(2).When used as a photocatalyst exposed to visible light,the material was excellent in degrading tetracycline(TC)in aqueous solutions.Scanning electron microscopy indicated that it had a folded sheet structure,with numerous nanoparticles observed on graphene sheets.Raman spectroscopy confirmed the presence of significant defects in the material,which suppressed the recombination of photogenerated electron-hole pairs.The performance and degradation mechanism of the photocatalyst was verified using a series of optical and electrochemical experiments and theoretical calculations.The degradation efficiency of the catalyst for TC was as high as 97.1%in 120 min under visible light irradiation,which is superior to other reported catalysts.A mechanism study showed that TC is rapidly degraded into CO_(2),H_(2)O and other small inorganic molecules,with holes(h^(+))serving as the primary driving force.The catalyst had an outstanding stability and reusability,and could be easily recovered using an external magnetic field.
文摘Herein,a luminescent europium-based metal-organic framework(Eu-MOF,[Eu_(3)(L)(HL)(NO_(3))_(2)(DMF)_(2)]·4DMF·5H_(2)O,H_(4)L=5,5′-(pyrazine-2,6-diyl)diisophthalic acid,DMF=N,N-dimethylformamide)was developed for the dual-functional detection of environmental pollutants.This fluorescence-quenching-based sensor exhibited excep-tional sensitivity for both 2,4,6-trinitrophenol(TNP)and tetracycline(TC),achieving remarkably low detection lim-its of 1.96×10^(-6)and 1.71×10^(-7)mol·L^(-1),respectively.Notably,the system exhibited 99%fluorescence quenching ef-ficiency for TC,indicating ultra-efficient analyte recognition.The detection performance surpasses most reported lu-minescent MOF sensors,attributed to synergistic mechanisms of fluorescence resonance energy transfer(FRET)and photoinduced electron transfer(PET).CCDC:2446483.
基金supported by the National Natural Science Foundation of China(Nos.22136003 and 21972073)the Opening foundation of the Engineering Research Center of Ecoenvironment in Three Gorges Reservoir Region,Ministry of Education(No.KF2023-01)the Natural Science Foundation of Yichang City(No.A22-3-005)。
文摘The synergetic technology of hydrodynamic cavitation(HC)and peroxydisulfate(PDS)has been adopted for the treatment of organic pollutants,while the rationale behind the thermal-activation of PDS in this process remains lacking.This paper presented investigation on the degradation of tetracycline under two types of operating conditions,including“internal reaction conditions”(pH value and TC/PDS molar ratio)and“external physical conditions”(hole shape,solution temperature and inlet pressure).Special emphasis was paid on the analysis of thermal effects through a robust modeling approach.The results showed that a synergy index of 6.26 and a degradation rate of 56.71%could be obtained by the HC-PDS process,respectively,when the reaction conditions were optimized.Quenching experiment revealed that·OH and·SO_(4)^(-)were the predominant free radicals and their contribution to the degradation was 75.4%and 24.6%respectively,since a part of·SO_(4)^(-)was transformed into·OH in the solution.The thermal activation of PDS mainly occurred near the hole where the fitting temperature was around 340 K,while·OH was generated in the bubble collapse region downstream the hole,where the temperature was much higher and favorable for the cleavage of water molecular.The average temperature under different external physical conditions was in good consistence with the degradation rates.This research developed a useful method to effectively evaluate the activation extent of PDS by HC and could provide reliable guidance for further development of cavitational reactors to treat organic pollutants based on this hybrid approach.
文摘Tetracyclines (TCs) are the second most commonly used antibiotics worldwide, utilized in medical treatments and animal husbandry. Although effective against various infectious diseases, TC residues persist in the environment and contribute to the emergence of antibiotic-resistant pathogens, posing significant risks to human health. This study employed the heterogeneous Fenton process to degrade TC using soybean residue-derived magnetic biochar (Fe-SoyB) as the catalyst. The Fe-SoyB sample was characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and superconducting quantum interference device (SQUID) techniques. The effects of key parameters, including pH, H2O2 concentration, catalyst dosage, and initial TC concentration, on TC degradation were investigated. The results indicated that the TC removal efficiency decreased with increasing initial TC concentration, while it was improved with higher H2O2 concentrations and greater catalyst dosages. The optimal conditions for the Fenton-like process were determined: a pH of 3, a H2O2 concentration of 245 mmol/L, an initial TC concentration of 800 mg/L, and a catalyst dosage of 0.75 g/L, achieving a removal efficiency of 90.0% after 150 min. Additionally, the TC removal efficiency of the Fe-SoyB system varied significantly across different water matrices, with 87.1% for deionized water, 78.5% for tap water, and 72.5% for river water. The catalyst demonstrated notable stability, maintaining a TC removal efficiency of 79.7% after three cycles of use. Overall, Fe-SoyB shows promise as a cost-effective catalyst for the elimination of organic pollutants in aqueous solutions.
基金supported by the National Natural Science Foundation of China(No.21908085).
文摘Eliminating highly concentrated antibiotic wastewater by transition metal catalyst-assisted AOPs is challenging.Herein,by varying the metal precursor composition(Co/Fe ratios of 1/1,1.5/2/3),alloyed Co_(7)Fe_(3)nanocrystals or spinel-like CoFe_(2)O_(4)can be switched and both confined within the porous N-doped graphitic carbon fibers by electrospinning and controlled graphitization.Impressively,iron precursors played a dual role in working as reactive centers and main activators for the creation of porous carbon networks affording improved accessibility to catalytic sites and easy tetracycline(TC)diffusion effect.The catalytic activity of the resulting materials was closely related to surface metal valence and composition.Notably,the CoFe_(2)O_(4)exhibited a significant improvement in peroxymonosulfate(PMS)adsorption and activation,explained by the present electron-deficient Co and Fe synergetic sites together with the interesting Jahn-Teller effect.Fe_(1)Co_(2)/CNF demonstrated the highest efficiency in degrading TC,achieving a reaction rate constant of 0.4647 min^(-1)with a low activation energy of 9.3 kJ·mol^(-1),nearly a 7.5-fold enhancement compared to Fe_(1)Co_(3)/CNF(0.062 min^(-1)).The reaction mechanism and the role of reactive oxidative species revealed a synergy of·SO_(4)^(-),·OH,·O_(2)^(-)and^(1)O_(2).Wherein,·O_(2)^(-)plays a more dominant role in the degradation of TC than other reactive species.Additionally,a reinforced electron-transfer pathway in the Fe_(1)Co_(2)/CNF system during PMS interaction was demonstrated.Furthermore,the degradation routes of TC were unraveled,and the toxicity of various intermediate by-products was assessed.Importantly,our continuous flow-type TC degradation process and light-driven photothermal strengthened reaction process demonstrated consistent performance,thereby offering a promising approach for tackling highly concentrated antibiotic wastewater.
基金supported by the National Natural Science Foundation of China(Nos.52100062,and 52230001)China Postdoctoral Science Foundation(No.2023M732785).
文摘This study introduced a microwave-assisted pyrolysis method for the rapid and efficientpreparation of boron-doped porous biochar. The resulting biochar exhibited a large specificsurface area (933.39 m^(2)/g), a rich porous structure (1.044 cm3/g), and abundant active sites.Consequently, the prepared boron-doped porous biochar exhibited higher efficiency in adsorbingtetracycline with a maximum adsorption capacity of 413.223 mg/g, which significantlyexceeded that of unmodified biochar andmost commercial and reported adsorbents.The correlation analysis between the adsorption capacity and adsorbent characteristics revealedthat the formation of the –BCO_(2) group enhanced π–π electron donor–acceptor interactionsbetween boron-doped porous biochar and tetracycline. This mechanism mainlycontributed to the enhanced adsorption of tetracycline by boron-doped porous biochar. Additionally,the as-prepared boron-doped porous biochar exhibited broad applications in removingantibiotics (tetracycline), phenolics (bisphenol A), and dyes (methylene blue andrhodamine B). Moreover, the boron-doped porous biochar exhibited satisfactory stability,and its adsorption capacity can be nearly completely regenerated through simple heat treatment.This study provides new insights into the effectiveness of boron-doped carbonaceousmaterials in removing antibiotic contaminants.
基金supported by the National Natural Science Foundation of China(No.U21A20293).
文摘Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
基金supported by the National Natural Science Foundation of China(No.41977315)the Fundamental Research Funds for the Central Universities of China(No.201964004).
文摘Mariculture tailwater typically contains a certain concentration of antibiotics;however,conventional biological treatment methods struggle to effectively remove these antibiotics.Therefore,in this study,we modified the carbon felt(CF)anode in sediment microbial fuel cells(SMFCs)to enhance tetracycline(TC)removal in mariculture systems.We fabricated a novel composite material by integrating instant freeze-drying technology with the solvothermal reaction method to combine graphene oxide(GO)and nanoscale SiO_(2).Subsequently,the composite material was incorporated into CF for anodic modification,resulting in improved performance of SMFCs in TC removal and electricity generation.The maximum power density achieved was 63.72 mW/m^(2),nearly 2.9 times higher than that of the unmodified anode.Modified SMFCs exhibited a twofold increase in the degradation rate of tetracycline compared to natural degradation alone and showed significant improvements compared to both the control group and conditions with only GO addition.Furthermore,the modified anode effectively enriched populations of Leisingera,Oceanimonas,and Halomonas,thereby significantly enhancing the electrochemical performance of the SMFCs.This study successfully demonstrates the application of a modified-anode SMFC using a composite material consisting of GO and SiO_(2)for on-site removal of TC from mariculture environments.
基金supported by the National Natural Science Foundation of China(No.U20A20133)the National Key Research and Development Program of China(No.2022YFF0606703).
文摘The arbitrary discharge of tetracycline(TC)residuals has seriously influenced the ecosystem and human health.Laccase(Lac)-based biodegradation technology is considered a more effective way to remove TC due to its high catalytic efficiency and less by-product.Nevertheless,free Lac suffers from poor stability,easy inactivation and difficult recovery,restricting its application.Immobilization of Lac is considered an efficient strategy for addressing these obstacles.In this study,a magnetic metal-organic framework of Fe_(3)O_(4)@SiO_(2)@UiO-66-NH_(2)(MMOF)was prepared and used as a carrier to immobilize Lac(Lac@MMOF)for TC degradation.Benefiting from the multiple binding sites,adsorption,and protection effect of MMOF,Lac@MMOF displayed a wider pH application range(2–7)and better thermal(15–85℃),repeatability,and storage stability than free Lac.Furthermore,owing to the synergism of MOF adsorption and Lac biocatalysis,the removal rate of Lac@MMOF for TC could be up to 98%at pH=7 within 1 hr,which was 1.29 and 1.24 times that of free Lac and MMOF,respectively.More importantly,Lac@MMOF could easily be separated from aqueous solution under a magnetic field and maintained good removal performance(80%)after five cycles.The degradation products were identified by applying LC-MS/MS,and possible degradation mechanisms and pathways were proposed.Finally,the antibacterial activity of intermediate products was evaluated using Escherichia coli,which revealed that the toxicity of TC was reduced effectively by the degradation of Lac@MMOF.Overall,Lac@MMOF is a green alternative for residual antibiotic removal in water.
基金Project(23-2-1-107-zyyd-jch)supported by the Qingdao Natural Science Foundation,ChinaProject(ZR2022QE236)supported by the Natural Science Foundation of Shandong Province Youth Project,China+2 种基金Project(SDCX-ZG-202400211,SDCX-ZG-202203052)supported by the Shandong Postdoctoral Science Foundation,ChinaProject(ZD2023K03)supported by the Engineering Research Center of Non-metallic Minerals of Zhejiang Province,ChinaProject(01020240806)supported by the Qingdao Postdoctoral Program for Applied Research,China。
文摘Developing a low-cost stable and high-performance peroxymonosulfate(PMS)catalyst to degrade refractory organic pollutants is still an urgent problem.Herein,this study reported FeVO_(4)nanorods decorated sepiolite(FeVO_(4)/sepiolite)through simple hydrothermal method as an adsorptive-catalyst for PMS activation to degrade tetracycline(TC).Benefiting from the introduction of sepiolite support,FeVO_(4)nanorods could be uniformly immobilized onto fibrous sepiolite surface.As a result,FeVO_(4)/sepiolite composite was endowed with excellent adsorption properties,rich surface hydroxyl groups,more reaction active sites,and the stable redox cycle of Fe^(3+)/Fe^(2+)and V5^(+)/V4^(+).Therefore,higher TC degradation efficiency(91.19%within 40 min)and larger reaction rate constant(0.1649 min^(-1))were obtained in FeVO_(4)/sepiolite/PMS system than in FeVO_(4)/PMS system.Besides,the composite presented good stability and reusability,and the effects of application parameters on TC degradation were investigated in detail.Through quenching experiment and electron paramagentic resonance(EPR)test,it was found that both radical and non-radical species participates in TC degradation,and ^(1)O_(2) were the main active species.The PMS activation mechanism was proposed,and the possible degradation pathway was also analyzed according to the high performance liquid chromatography-mass spectrometry(HPLC-MS)results.Overall,this work provides meaningful insights for designing natural mineral based PMS activators to effectively remediate antibiotic wastewater.
基金supported by National Natural Science Foundation of China(32172760)the Open Fund of Sichuan Engineering Technology Research Center for High Salt Wastewater Treatment and Resource Utilization,Sichuan University of Science and Engineering(SCGCY2302).
文摘Two-dimensional luminescent metal-organic frameworks(2D LMOFs),have garnered significant attention for their unique fluorescent properties and highly accessible active sites,yet designing these LMOFs with target-dependent fluorescence for sensing remains a challenging endeavor.Herein,a zinc tetra(4-carboxyphenyl)porphine(Zn-TCPP)LMOF was prepared and first applied to the fast and sensitive sensing of tetracycline hydrochloride(TCH).Upon TCH exposure,the signature red fluorescence of Zn-TCPP at 609 nm diminishes,accompanied by the emergence of a 520 nm peak,which were originated from photo-induced electron transfer(PET)of Zn-TCPP to TCH and inner filter effect(IFE)of TCH towards Zn-TCPP,and the triggers of Zn-TCPP on the instinct fluorescence of TCH,respectively.Notably,the I_(520)nm/I_(609)nm fluorescence intensity ratio showed good linearity over a wide range of TCH concentrations(0.1–25μmol/L),with a limit of detection(LOD)of 65.4 nmol/L.Additionally,the Zn-TCPP probe showed good TCH selectivity and anti-interference properties.The probe's practicability was also validated by detecting TCH in spiked tap water,milk and chicken samples.Furthermore,test papers impregnated with the Zn-TCPP probe were prepared,allowing the visual detection of TCH with a smartphone.Results suggest the developed method is suitable for practical TCH detection.
