RESUMO
NH2-MIL-125(Ti) materials had great potential for photocatalytic applications but had low activity due to exciton effect and narrow absorption range of visible light. The surface oxygen-containing negative functional groups of boron nitride quantum dots (BNQDs) could overcome these defects, but due to the low load capacity, a higher specific surface area of the substrate was usually required. In this paper, a hollow Ti-MOF material was developed by etching technology. The hollow structure formed by tannic acid etching broadened the absorption range of visable light and provided more alternative surfaces for loading BNQDs. The 85.2% of high tetracycline (TC) removal efficiency for the best sample (BNQDs-5@20-Ti-MOF + PMS) was obtained, which was about 56.8 and 1.9 times of the 20-Ti-MOF and BNQDs-5@20-Ti-MOF, respectively. BNQDs-5@20-Ti-MOF + PMS system showed a great TC degradation efficiency in a wide pH range (pH = 5-9). In addition, reaction temperature and the inorganic ions did not show significant inhibition effect for TC removal. Both free radical and non-free radical pathways were involved in the TC degration by BNQDs-5@20-Ti-MOF + PMS system, among which O2â¢- and 1O2 played the key roles. Interestingly, multiple 1O2 production paths contributed to the high efficiency and stability of BNQDs-5@20-Ti-MOF + PMS system. This study revealed a reasonable combination of Ti-MOF and BNQDs, which provided a new efficient photocatalyst for environmental remediation.
Assuntos
Compostos de Boro , Pontos Quânticos , Taninos , Tetraciclina , Tetraciclina/química , Pontos Quânticos/química , Catálise , Taninos/química , Compostos de Boro/química , Estruturas Metalorgânicas/química , Peróxido de Hidrogênio/química , Luz , Ferro/química , Poluentes Químicos da Água/química , Processos Fotoquímicos , Titânio/química , PolifenóisRESUMO
The influences of the positive Fe3+ and the negative Cr2O72- on the tetracycline (TC) photodegradation by N-doped dissolved black carbon (NDBC) have been investigated in this work. A series of samples (NDBC300, NDBC400 and NDBC500) have been extracted from the corresponding biochar. NDBC400 has the best photodegradation performance (79%) for TC under visible light irradiation. Adding Cr2O72- and Fe3+ can reduces TC photodegradation efficiency into 37% and 53%, respectively. This maybe from that Cr2O72- has stronger interaction with NDBC400 than Fe3+ since it can quench more fluorescence intensity of NDBC400 than Fe3+. Furthermore, Cr2O72- can reduce the steady-state concentration of 3NDBC400*, 1O2 and â¢OH, whereas Fe3+can just reduce the steady-state concentration of 3NDBC400* and increase the concentration of â¢OH. This may explain why Cr2O72- has stronger inhibit performance of TC photodegradation by NDBC400 than Fe3+. The band structures of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- are constructed. And the VB of NDBC400-Fe3+ has a stronger ability to produce â¢OH than NDBC400. In summary, coupling interaction and band structure characterization of NDBC400, NDBC400-Fe3+ and NDBC400-Cr2O72- can explain well why Cr2O72 has stronger inhibition effect than Fe3+ and Fe3+ can increase the concentration of â¢OH. This work provides a deep insight for the photochemical behavior of dissolved black carbon and the transformation behavior of the co-existed metal ions and antibiotics.
Assuntos
Antibacterianos , Cromo , Ferro , Nitrogênio , Fotólise , Cromo/química , Antibacterianos/química , Nitrogênio/química , Ferro/química , Fuligem/química , Tetraciclina/química , Carbono/química , LuzRESUMO
Tetracycline (TC) contamination in water is one of the key issues in global environmental protection, and traditional water treatment methods are difficult to remove antibiotic pollutants.Therefore, efficient and environmentally friendly treatment technologies are urgently needed. In this study, activated persulfate (PS) using a biochar-loaded nano zero-valent iron (BC-nZVI) advanced oxidation system was used to investigate the degradation effect, influencing factors, and mechanism of TC. BC-nZVI was prepared using the liquid-phase reduction method, and its structure and properties were analyzed by various characterization means. The results showed that nZVI was uniformly distributed on the surface or in the pores of BC, forming a stable complex. Degradation experiments showed that the BC-nZVI/PS system could degrade TC up to 99.57% under optimal conditions. The experiments under different conditions revealed that the iron-carbon ratio, dosing amount, PS concentration, and pH value all affected the degradation efficiency. Free radical burst and electron paramagnetic resonance (EPR) experiments confirmed the dominant roles of hydroxyl and sulfate radicals in the degradation process, and LC-MS experiments revealed the multi-step reaction process of TC degradation. This study provides a scientific basis for the efficient treatment of TC pollution in water.
Assuntos
Carvão Vegetal , Ferro , Sulfatos , Tetraciclina , Poluentes Químicos da Água , Purificação da Água , Carvão Vegetal/química , Ferro/química , Tetraciclina/química , Poluentes Químicos da Água/química , Sulfatos/química , Purificação da Água/métodos , Oxirredução , Concentração de Íons de Hidrogênio , Água/químicaRESUMO
Fe3O4 has the advantages of unique magnetic stability and low biological toxicity, which can improve pollutants separation efficiency. MXenes are two-dimensional materials and easy surface functionalization that can provide suitable carriers for Fe3O4. In this work, we synthesized magnetic MXene composites by a one-pot method that relies on doping Fe3O4 particles onto Ti3C2 MXene nanosheets by heat treatment. The Fe3O4/Ti3C2 MXene was analyzed by SEM, XRD, FTIR and XPS techniques, which showed that the material has good tetracycline (TC) removal properties and magnetic separation ability. The results showed that the adsorption capacity of it was 46.42 mg g-1, and the removal efficiency of 0.06 g adsorbent for 50 mL of 30 mg L-1 TC could reach 92.1% in a wide pH range of 4-10, when the adsorption temperature was 25 °C, and the adsorption time was 3 h. The adsorption data were consistent with Langmuir and the proposed second-order kinetic model, and the thermodynamic experiments confirmed that the adsorption of TC was a monolayer physicochemical adsorption coexisting heat-trapping process (ΔH = 15.72 kJ mol-1). In addition, the adsorption of TC by Fe3O4/Ti3C2 MXene was attributed to the synergistic effect of electrostatic attraction, hydrogen bonding and π-π packing. In conclusion, the saturation magnetization of Fe3O4/Ti3C2 MXene is 27.3 emu/g and it can not only be separated from water using its strong magnetic properties to avoid secondary contamination, but also can be used as a promising material to effectively remove antibiotics from aqueous media.
Assuntos
Tetraciclina , Titânio , Poluentes Químicos da Água , Purificação da Água , Titânio/química , Tetraciclina/química , Tetraciclina/isolamento & purificação , Poluentes Químicos da Água/química , Adsorção , Purificação da Água/métodos , Cinética , Compostos Férricos/química , Termodinâmica , Concentração de Íons de HidrogênioRESUMO
In this study, a potassium ferrate (K2FeO4)-modified biochar (Fe-BC) was prepared and characterized. Afterwards, Fe-BC was applied to activated periodate (PI) to degrade tetracycline (TC), an antibiotic widely used in animal farming. The degradation effects of different systems on TC were compared and the influencing factors were investigated. In addition, several reactive oxygen species (ROS) generated by the Fe-BC/PI system were identified, and TC degradation pathways were analyzed. Moreover, the reuse performance of Fe-BC was evaluated. The results exhibited that the Fe-BC/PI system could remove almost 100% of TC under optimal conditions of [BC] = 1.09 g/L, initial [PI] = 3.29 g/L, and initial [TC] = 20.3 mg/L. Cl-, HCO3-, NO3-, and humic acid inhibited TC degradation to varying degrees in the Fe-BC/PI system due to their quenching effects on ROS. TC was degraded into intermediates and even water and carbon dioxide by the synergistic effect of ROS generated and Fe on the BC surface. Fe-BC was reused four times, and the removal rate of TC was still maintained above 80%, indicating the stable nature of Fe-BC.
Assuntos
Carvão Vegetal , Ferro , Tetraciclina , Poluentes Químicos da Água , Tetraciclina/química , Ferro/química , Carvão Vegetal/química , Poluentes Químicos da Água/química , Espécies Reativas de Oxigênio/metabolismo , Purificação da Água/métodos , Antibacterianos/química , Antibacterianos/farmacologia , Compostos de Potássio , Compostos de FerroRESUMO
Lanthanum nickelate (LaNiO3), known for its high visible-light absorption, is a promising photocatalyst for water purification. However, the low conduction band position and high photogenerated carrier complexation rate of pure LaNiO3 limit its photocatalytic activity. To address this issue, we investigated the synergistic effects of doping and constructing heterojunctions. A La0.9Sr0.1NiO3 (20%)/g-C3N4 (L2CN8) heterojunction was successfully created. In addition, various characterisation techniques were then employed to analyse the structure-performance relationships of these heterojunction photocatalysts in degrading organic dyes. Results revealed that at a 10% Sr doping level, the oxygen vacancy content was 0.68, which is significantly higher than that of LaNiO3 (0.05). The increased number of oxygen vacancies enhanced the electron capture ability and improved the separation efficiency of photogenerated carriers. Furthermore, the optimised L2CN8 (20 mg) achieved 81.2% and 73.8% removal of methylene blue (50.0 mL, 10 mg L-1) and tetracycline (50.0 mL, 10 mg L-1) under simulated visible-light irradiation (λ > 420 nm). Furthermore, an active species capture experiment confirmed the significant role of superoxide radicals (·O2-) in the degradation process. Based on these experimental findings, we proposed a rational Z-type charge transfer mechanism. This study holds great importance for water pollution control and environmental protection.
Assuntos
Lantânio , Luz , Poluentes Químicos da Água , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Catálise , Lantânio/química , Níquel/química , Azul de Metileno/química , Fotólise , Processos Fotoquímicos , Compostos de Nitrogênio/química , Tetraciclina/química , Nitrilas/química , GrafiteRESUMO
Elemental doping is a promising way for enhancing the electrocatalytic activity of metal oxides. Herein, we fabricate Ti/ Ti4O7-CB-Ce anode materials by the modification means of carbon black and cerium co-doped Ti4O7, and this shift effectively improves the interfacial charge transfer rate of Ti4O7 and â¢OH yield in the electrocatalytic process. Remarkably, the Ti4O7-CB-Ce anode exhibits excellent efficiency of minocycline (MNC) wastewater treatment (100% removal within 20 min), and the removal rate reduces from 100 to 98.5% after five cycles, which is comparable to BDD electrode. â¢OH and 1O2 are identified as the active species in the reaction. Meanwhile, it is discovered that Ti/ Ti4O7-CB-Ce anodes can effectively improve the biochemical properties of the non-biodegradable pharmaceutical wastewater (B/C values from 0.25 to 0.44) and significantly reduce the toxicity of the wastewater (luminescent bacteria inhibition rate from 100 to 26.6%). This work paves an effective strategy for designing superior metal oxides electrocatalysts.
Assuntos
Antibacterianos , Cério , Oxirredução , Fuligem , Águas Residuárias , Cério/química , Antibacterianos/química , Águas Residuárias/química , Catálise , Fuligem/química , Eletrodos , Titânio/química , Tetraciclina/química , Poluentes Químicos da Água/químicaRESUMO
Sensor array methods have received much attention in recent years. In this study, a colorimetric sensor array consisting of three kinds of steel slag-based composites (including porphyrin-functionalized non-magnetic steel slag (NMSS-Por), alkali-excited steel slag (A-SS), and platinum modified steel slag (ALANH-Pt)) was developed for the detection and recognition of tetracycline antibiotics (TCs) such as tetracycline (TC), oxytetracycline (OTC) and doxycycline (DOX). Linear discriminant analysis (LDA) and hierarchical cluster analysis (HCA) showed that the colorimetric sensor array has excellent recognition ability for TCs. The detection limits of this sensor array for TC, OTC, and DOX were 0.059 µM, 0.111 µM and 0.118 µM, respectively, which provided higher sensitivity compared to the colorimetric sensors composed of a single steel slag-based composite material. At the same time, the array sensor has anti-interference ability, and this study provides a new application route for steel slag.
Assuntos
Antibacterianos , Colorimetria , Aço , Colorimetria/métodos , Colorimetria/instrumentação , Aço/química , Antibacterianos/análise , Limite de Detecção , Tetraciclina/análise , Tetraciclina/química , Tetraciclinas/análise , Doxiciclina/análise , Doxiciclina/química , Análise DiscriminanteRESUMO
Development of carbon materials with high activity was important for rapid degradation of emerging pollutants. In this paper, a novel nanoscale zero-valent iron-copper bimetallic biochar (nZVIC-BC) was synthesized by carbothermal reduction of waste pine wood and copper-iron layered double hydroxides (LDHs). Characterization and analysis of its structural, elemental, crystalline, and compositional aspects using XRD, FT-IR, SEM, and TEM confirmed the successful preparation of nZVIC-BC and the high dispersion of Fe-Cu nanoparticles in an ordered carbon matrix. The experimental results showed that the catalytic activity of nZVIC-BC (Kobs of 0.0219 min-1) in the degradation of tetracycline (TC) in anoxic water environment was much higher than that of Fe-BC and Cu-BC; the effective degradation rate reached 85%. It was worth noting that the negative effects of Ca2+, Mg2+, and H2PO4- on TC degradation at ionic strengths greater than 15 mg/L were due to competition for active sites. Good stability and reusability were demonstrated in five consecutive cycle tests for low leaching of iron and copper. Combined with free radical quenching experiments and XPS analyses, the degradation of TC under air conditions was only 62%, with hydroxyl radicals (·OH) playing a dominant role. The synergistic interaction between Fe2+/Fe3+ and Cu0/Cu+/Cu2+ under nitrogen atmosphere enhances the redox cycling process; π-π adsorption, electron transfer processes, and active [H] were crucial for the degradation of TC; and possible degradation pathways of TC were deduced by LC-MS, which identified seven major aromatic degradation by-products. This study will provide new ideas and materials for the treatment of TC.
Assuntos
Carvão Vegetal , Cobre , Água Subterrânea , Ferro , Tetraciclina , Poluentes Químicos da Água , Cobre/química , Carvão Vegetal/química , Ferro/química , Poluentes Químicos da Água/química , Tetraciclina/química , Água Subterrânea/químicaRESUMO
Sodium alginate (SA) biopolymeric films have various limitations such as poor mechanical properties, high vapor permeability, lack of antibacterial activity, excessive burst release, and weak cell adhesion. To overcome these limitations, a strategy involving the integration of nanofillers into an SA film matrix is explored. In this context, a cost-effective iron-containing carbon nano biocomposite (FeCNB) nanofiller is developed using a solvent-free technique. This nanocomposite is successfully incorporated into the alginate film matrix at varying concentrations (0.05, 0.1, and 0.15%) aimed at enhancing its physicochemical and biological properties for biomedical applications. Characterization through FESEM and BET analyses confirms the porous nature of the FeCNB. EDX shows the FeCNB's uniform distribution upon its integration into the film matrix, albeit without strong chemical interaction with SA. Instead, hydrogen bonding interactions become apparent in the FTIR spectra. By incorporating the FeCNB, the mechanical attributes of the films are improved and the water vapor permeability approaches the desired range (2000-2500 g/m2day). The film's swelling ratio reduction contributes to a decrease in water permeability. The antibacterial activity and sustained release property of the FeCNB-incorporated film are established using tetracycline hydrochloride (TCl), a model drug. The drug release profile resembled Korsmeyer-Peppas's release pattern. In vitro assessments via the MTT assay and scratch assay on NIH-3T3 cells reveal that FeCNB has no adverse effects on the biocompatibility of alginate films. The cell proliferation and adhesion to the SA film are significantly enhanced after infusion of the FeCNB. The in vivo study performed on the rat model demonstrates improved wound healing by FeCNB-impregnated films. Based on the comprehensive findings, the proposed FeCNB-incorporated alginate films prove to be a promising candidate for robust skin repair.
Assuntos
Alginatos , Antibacterianos , Ferro , Animais , Alginatos/química , Ferro/química , Antibacterianos/química , Antibacterianos/farmacologia , Ratos , Pele/efeitos dos fármacos , Nanocompostos/química , Cicatrização/efeitos dos fármacos , Camundongos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Staphylococcus aureus/efeitos dos fármacos , Permeabilidade , Tetraciclina/química , Tetraciclina/farmacologiaRESUMO
In this work, a novel double-chamber system (PFC-Fenton), combined photocatalytic fuel cell (PFC) with Fenton, was constructed for tetracycline hydrochloride (TCH) and hexavalent chromium (Cr(VI)) removal and electricity production. Therein, Zn5(OH)6(CO3)2/Fe2O3/BiVO4/fluorine-doped SnO2 (ZIO/BiVO4/FTO) and carboxylated carbon nanotubes/polypyrrole/graphite felt (CCNTs/Ppy/GF) were served as photoanode and cathode, respectively. Under light irradiation, the removal efficiencies of TCH and Cr(VI) with the addition of H2O2 (2 mL) could reach 93.1% and 80.4%, respectively. Moreover, the first-order kinetic constants (7.37 × 10-3 min-1 of TCH and 3.94 × 10-3 min-1 of Cr(VI)) were 5.26 and 5.57 times as much as the absence of H2O2. Simultaneously, the maximum power density could be obtained 0.022 mW/cm2 at a current density of 0.353 mA/cm2. Therein, the main contribution of TCH degradation was ·OH and holes in anode chamber. The synergistic effect of photoelectrons, generated ·O2-, and H2O2 played a crucial role in the reduction of Cr(VI) in cathode chamber. The high-performance liquid chromatography-mass spectrometry indicated that TCH could be partially mineralized into CO2 and H2O. X-ray photoelectron spectroscope and X-ray absorption near-edge structure spectra showed that Cr(VI) could be reduced to Cr(III). After 5 times of cycling, the removal efficiencies of TCH and Cr(VI) were still greater than 70%, indicating the remarkable stability of the PFC-Fenton system. Overall, this system could remove TCH/Cr(VI) and generate power simultaneously without iron sludge formation, demonstrating a promising method to further develop PFC-Fenton technology.
Assuntos
Cromo , Peróxido de Hidrogênio , Tetraciclina , Cromo/química , Tetraciclina/química , Peróxido de Hidrogênio/química , Catálise , Ferro/químicaRESUMO
The interfacial charge transfer ability is a decisive factor influencing the photocatalytic performance of composite photocatalysts. Compared with heterojunctions that combine two or more semiconductors with different properties, homojunctions that combine two semiconductors with similar properties can accelerate the interfacial charge shift and achieve higher photocatalyticability. In this study, a Zn3In2S6/ZnIn2S4 homojunction photocatalyst (ZIS-5) with a Zn3In2S6 to ZnIn2S4 molar ratio of 5:1 was synthesized by selecting Zn3In2S6 nano-microspheres as the substrate material and growing ZnIn2S4 flocs on the nano-microspheres. The photocatalytic performance of the ZIS-5 homojunction was assessed by using tetracycline (TC) as a typical pollutant. The photocatalytic performance and mineralization rate of the ZIS-5 homojunction were significantly improved compared with those of Zn3In2S6 and ZnIn2S4, and its photocatalytic performance was increased by 10.2% and 20.9%, compared with Zn3In2S6 and ZnIn2S4, respectively, while the mineralization rate was enhanced by 22.78% and 43.28%, respectively. The results of the comparison experiment revealed that the interfacial electron transfer ability of the ZIS-5 homojunction is 1.6 times that of the g-C3N4/ZnIn2S4-5 heterojunction. The density functional theory (DFT) computation and Mott-Schottky plots verified the formation of an internal electric field. The toxicity analysis showed that the ZIS-5 homojunction system effectively reduced the toxicity of TC. This work supplies a valuable route for inventing catalysts with efficient photocatalytic performances.
Assuntos
Tetraciclina , Catálise , Tetraciclina/química , Luz , Zinco/químicaRESUMO
A MOF-on-MOF composite derivative material named ZIF-67@Ce-MOF-600 was designed and synthesized. The preparation of ZIF-67@Ce-MOF-600 was optimized from the aspects of the ratio of metal and ligand, heat-treatment temperature. It was demonstrated by XRD, FT-IR, SEM-EDS and TEM. The optimum conditions for the activation of PMS by ZIF-67@Ce-MOF-600 for the degradation of tetracycline (TC) were investigated by adjusting the catalyst dosage, TC, pH, peoxymonosulfate (PMS) concentration, and different kinds of water, co-existing anions and pollution. Under optimal conditions (20 mg catalysts and 50 mg PMS added) in 100 mL of tetracyclines (TC) solvent (20 mg TC/L), the removal rate could reach up to 99.2% and after five cycles was 70.5%. The EPR results indicated the presence of free radicals and non-free radical, among which free radicals intended to play a major role in the degradation process. Its possible degradation pathways and attack sites were analyzed by liquid-phase mass spectrometry and DFT analysis.
Assuntos
Estruturas Metalorgânicas , Peróxidos , Tetraciclina , Poluentes Químicos da Água , Estruturas Metalorgânicas/química , Poluentes Químicos da Água/química , Tetraciclina/química , Peróxidos/química , Purificação da Água/métodos , Catálise , Água/químicaRESUMO
Iron (hydr)oxides are abundant in surface environment, and actively participate in the transformation of organic pollutants due to their large specific surface areas and redox activity. This work investigated the transformation of tetracycline (TC) in the presence of three common iron (hydr)oxides, hematite (Hem), goethite (Goe), and ferrihydrite (Fh), under simulated sunlight irradiation. These iron (hydr)oxides exhibited photoactivity and facilitated the transformation of TC with the initial phototransformation rates decreasing in the order of: Hem > Fh > Goe. The linear correlation between TC removal efficiency and the yield of HO⢠suggests that HO⢠dominated TC transformation. The HO⢠was produced by UV-induced decomposition of self-generated H2O2 and surface Fe2+-triggered photo-Fenton reaction. The experimental results indicate that the generation of HO⢠was controlled by H2O2, while surface Fe2+ was in excess. Sunlight-driven H2O2 production in the presence of the highly crystalline Hem and Goe occurred through a one-step two-electron reduction pathway, while the process was contributed by both O2-induced Fe2+ oxidation and direct reduction of O2 by electrons on the conduction band in the presence of the poorly crystalline Fh. These findings demonstrate that sunlight may significantly accelerate the degradation of organic pollutants in the presence of iron (hydr)oxides.
Assuntos
Compostos Férricos , Peróxido de Hidrogênio , Luz Solar , Tetraciclina , Peróxido de Hidrogênio/química , Compostos Férricos/química , Tetraciclina/química , Compostos de Ferro/química , Oxirredução , Minerais/química , Poluentes Químicos da Água/química , Ferro/químicaRESUMO
Tetracycline (TC), as a widely used antibiotic, is very useful in treating bacterial infections. However, its residues in animal foodstuffs can enter the human body through the food cycle and causes severe and chronic diseases. On the other hand, due to its weak non-biodegradability, it is considered a threat to the environment. In this regard, the development of sensing methods to detect and measure TC is need of the hour. Herein, a dual-emission fluorescence sensor based on porous aluminosilicate structure (ASS) with rough surface hexagonal shape morphology and pore diameter less than 2 nm was prepared. The porous AAS was modified by post-modification method with blue carbon dots (CDT) and rhodamine B (RB) as two fluorophores to develop the ratiometric fluorescence (RF) sensor (CDT-AAS/RB). Nanostructured CDT-AAS/RB emitted two resolved peaks at 445 and 585 nm , which were dramatically quenched in the presence of TC. The RF sensor, with excellent sensitivity, was able to measure TC over the linear range of 0.001-150 µM with a limit of detection of 5.4 nM in the aqueous phosphate buffer. Moreover, the AAS component granted high selectivity and anti-interference ability to the sensor. In addition, the stability of the sensor was greatly improved due to the non-accumulation of CDT nanoparticles and RB molecules in the presence of the AAS. The proposed method was able to determine TC in complex real samples with satisfactory recovery, and the obtained results were validated with standard high-performance liquid chromatography technique.
Assuntos
Silicatos de Alumínio , Carbono , Corantes Fluorescentes , Pontos Quânticos , Rodaminas , Saccharum , Tetraciclina , Pontos Quânticos/química , Carbono/química , Tetraciclina/análise , Tetraciclina/química , Rodaminas/química , Corantes Fluorescentes/química , Saccharum/química , Silicatos de Alumínio/química , Celulose/química , Nanoestruturas/química , Espectrometria de Fluorescência/métodos , Limite de Detecção , Antibacterianos/análise , Antibacterianos/químicaRESUMO
Steel mill wastewater sludge, as an iron-enriched solid waste, was expected to be converted into iron-enriched biochar with acceptable environmental risk by pyrolysis. The purpose of our study was to evaluate the chemical speciation transformation of heavy metals in biochar under various pyrolysis temperatures and its reutilization for tetracycline (TC) removal. The experimental data indicated that pyrolysis temperature was a key factor affecting the heavy metals speciation and bioavailability in biochar, and biochar with pyrolysis temperature at 450 °C was the most feasible for reutilization without potential risk. The endogenous iron-enriched biochar (FSB450) showed highly efficient adsorption towards TC, and its maximum adsorption capacity could reach 240.38 mg g-1, which should be attributed to its excellent mesoporous structure, abundant functional groups and endogenous iron cycling. The endogenous iron was converted to a stable iron oxide crystalline phase (Fe3O4 and MgFe2O4) by pyrolysis, which underwent a valence transition to form a coordination complex with TC by electron shuttling in the FSB450 matrix. The study provides a win-win approach for resource utilization of steel wastewater sludge and treatment of antibiotic contamination in wastewater.
Assuntos
Carvão Vegetal , Ferro , Metais Pesados , Esgotos , Aço , Tetraciclina , Águas Residuárias , Poluentes Químicos da Água , Carvão Vegetal/química , Tetraciclina/química , Adsorção , Ferro/química , Águas Residuárias/química , Metais Pesados/química , Metais Pesados/análise , Esgotos/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Aço/química , Eliminação de Resíduos Líquidos/métodos , Pirólise , Antibacterianos/química , Antibacterianos/análiseRESUMO
The omnipresence of microplastics (MPs) around the world has attracted extensive attention in the past decade with more focuses on the interactions of standard MPs without additives in regular shapes and individual pollutant, whereas the actual MPs containing various additives in irregular shapes and complex pollutants are often co-occurrence in the environments. In this paper, the adsorption performance of disposable polypropylene (PP) cups-based MPs subjected to ultraviolet irradiation was investigated in unitary and binary water matrices. The surface characteristics were analyzed and the experimental data of adsorption were fitted by various kinetic and isotherm models, and the results indicated that more cracks and oxygen-containing functional groups with decreased hydrophobicity were produced with aging, and electrostatic attraction and hydrogen bonding dominated methylene blue (MB) and tetracycline (TC) capture in the individual system. Moreover, pseudo-second order kinetic model better described the adsorption processes. In the binary system, the co-existence of TC promoted MB uptake, while the presence of MB inhibited TC capture. In addition, TC adsorption was enhanced by Ca2+, maybe due to its complexation effect, while the presence of mono- and divalent inorganic salts inhibited MB capture. This research provides useful insights for the fate of PP-MPs and organic pollutants in the complex environments.
Assuntos
Azul de Metileno , Microplásticos , Polipropilenos , Tetraciclina , Poluentes Químicos da Água , Azul de Metileno/química , Adsorção , Tetraciclina/química , Poluentes Químicos da Água/química , Polipropilenos/química , Microplásticos/química , CinéticaRESUMO
Alternanthera sessilis (AS) leaf extract was used to synthesize zinc oxide nanoparticles (ZnO NPs). Bioanalytical characterization techniques such as X-ray diffraction (XRD) and field emission scanning electron microscope (FESEM) confirmed the formation of crystalline ZnO NPs with average sizes of 40 nm. The AS-ZnO NPs antimicrobial activity was analyzed under dark (D) and white light (WL) conditions. The improved antimicrobial activity was observed against Escherichia coli, Staphylococcus aureus and Bacillus subtilis at the minimal inhibitory concentration (MIC) of 125 and 62.5 µg/mL under WL than the D at 125 and 250 µg/mL for E. coli, B. subtilis, and Pseudomonas aeruginosa, respectively. In contrast, the growth of P. aeruginosa and S. aureus was not completely inhibited until 1 mg/mL AS-ZnO NPs under WL and D. Similarly, AS-ZnO NPs displayed a weaker inhibitory effect against carbapenem-sensitive P. aeruginosa (CSPA) and carbapenem-resistant P. aeruginosa (CRPA) strains of PAC023, PAC041 and PAC032, PAC045 under D. Interestingly, the distinct inhibitory effect was recorded against CSPA PAC041 and CRPA PAC032 in which the bacteria growth was inhibited 99.9% at 250, 500 µg/mL under WL. The cytotoxicity results suggested AS-ZnO NPs demonstrated higher toxicity to MCF-7 breast cancer cells than the RAW264.7 macrophage cells. Further, AS-ZnO NPs exhibited higher catalytic potential against tetracycline hydrochloride (TC-H) degradation at 65.6% and 60.8% under WL than the dark at 59.35% and 48.6% within 120 min. Therefore, AS-ZnO NPs can be used to design a photo-improved antimicrobial formulation and environmental catalyst for removing TC-H from wastewater.
Assuntos
Antineoplásicos , Pseudomonas aeruginosa , Tetraciclina , Óxido de Zinco , Óxido de Zinco/química , Óxido de Zinco/farmacologia , Pseudomonas aeruginosa/efeitos dos fármacos , Pseudomonas aeruginosa/crescimento & desenvolvimento , Tetraciclina/farmacologia , Tetraciclina/química , Camundongos , Antineoplásicos/farmacologia , Antineoplásicos/química , Nanopartículas Metálicas/química , Animais , Antibacterianos/farmacologia , Antibacterianos/química , Testes de Sensibilidade Microbiana , Humanos , Extratos Vegetais/química , Extratos Vegetais/farmacologia , Farmacorresistência Bacteriana , Células RAW 264.7 , Nanopartículas/químicaRESUMO
Antibiotics have been considered as a group of emerging contaminants for their stable chemical structure, significant pseudo-persistence, and biological toxicity. Tetracycline (TC), as one of the typical antibiotics frequently detected in environmental media, can cause the dissemination and accumulation of antibiotic resistance gene (ARG), ultimately threatening human health and environmental safety. Herein, a novel ironcalcium di-crosslinked graphene oxide/alginate (GO/SA-Fe3+-Ca2+) aerogel was facilely synthesized for TC uptake. It was found that the introduction of GO nanosheets and Fe3+ sites into composite enormously enhanced TC removal. Specifically, TC can be stably and efficiently eliminated over the wide pH range of 5-8. The fitted maximum qe with Liu isotherm model at 308 K reached 1664.05 mg/g, surpassing almost all reported sorbents. The pseudo-second-order kinetic model with chemical sorption characteristics better fitted TC adsorption process, which was endothermic and spontaneous in nature. Multifarious adsorptive sites of GO/SA-Fe3+-Ca2+ synergically participated in TC uptake through multi-mechanisms (e.g., π-π EDA, cation-π bonding, H-bonding, Fe3+-coordination, and electrostatic attraction, etc.). The as-prepared composite showed satisfactory TC removal in several runs of adsorption-desorption operations, high salinity, and model aquaculture wastewater. Moreover, the packed-column could continuously run for >200 h until adsorption saturation was achieved with a dynamic adsorption capacity of 216.69 mg/g, manifesting its scale-up engineering applications. All above merits make as-constructed composite an alternative sorbent for eliminating TC from complex wastewater.
Assuntos
Grafite , Águas Residuárias , Poluentes Químicos da Água , Humanos , Cálcio , Microesferas , Alginatos/química , Poluentes Químicos da Água/química , Antibacterianos/farmacologia , Antibacterianos/química , Tetraciclina/química , Adsorção , Cinética , Concentração de Íons de HidrogênioRESUMO
Sulfate radical-based advanced oxidation processes with (SR-AOPs) are widely employed to degrade organic pollutants due to their high efficiency, cost-effectiveness and safety. In this study, a highly active and stable FeNiP was successfully prepared by reduction and heat treatment. FeNiP exhibited high performance of peroxymonosulfate (PMS) activation for tetracycline hydrochloride (TC) removal. Over a wide pH range, an impressive TC degaradation efficiency 97.86% was achieved within 60 min employing 0.1 g/L FeNiP and 0.2 g/L PMS at room temperature. Both free radicals of SO4·-, ·OH, ·O2- and non-free radicals of 1O2 participated the TC degradation in the FeNiP/PMS system. The PMS activation ability was greatly enhanced by the cycling between Ni and Fe bimetal, and the active site regeneration was achieved due to the existence of the negatively charged Pn-. Moreover, the FeNiP/PMS system exhibited substantial TC degradation levels in both simulated real-world disturbance scenarios and practical water tests. Cycling experiments further affirmed the robust stability of FeNiP catalyst, demonstrating sustained degradation efficiency of approximately 80% even after four cycles. These findings illuminate its promising potential across natural water bodies, presenting an innovative catalyst construction approach for PMS activation in the degradation of antibiotic pollutants.