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1.
Environ Res ; 261: 119720, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39096986

RESUMO

Activated carbon (AC) is a porous, amorphous form of carbon known for its strong adsorption capacity, making it highly effective for use in wastewater treatment. In this investigation, AC-based nanocomposites (NCs) loaded with zirconium dioxide and cerium dioxide nanoparticles (ZrO2/CeO2 NPs) were successfully synthesized for the effective elimination of methylene blue (MB) and tetracycline hydrochloride (TCH). The AC-ZrO2/CeO2 NCs have a size of 231.83 nm, a zeta potential of -20.07 mV, and a PDI value of 0.160. The adsorption capacities of AC-ZrO2/CeO2 NCs for MB and TCH were proved in agreement with the Langmuir isotherm and pseudo 1st order kinetic model, respectively. The maximum adsorption capacities were determined to be 75.54 mg/g for MB and 26.75 mg/g for TCH. Notably, AC-ZrO2/CeO2 NCs exhibited superior photocatalytic degradation efficiency for MB and TCH under sunlight irradiation with removal efficiencies reaching up to 97.91% and 82.40% within 90 min, respectively. The t1/2 for the photo-degradation process of MB and TCH were 11.55 min and 44.37 min. Analysis of active species trapping confirmed the involvement of hole (h+), superoxide anion (•O2-), and hydroxyl radical (•OH) in the degradation mechanism. Furthermore, the residual solution post-contaminant removal exhibited minimal toxicity towards Artemia salina and NIH3T3 cells. Importantly, the NCs did not exhibit antibacterial activity against tested pathogens post-absorption/degradation of TCH. Thus, AC-ZrO2/CeO2 NCs could be a promising nanomaterial for wastewater treatment applications.

2.
Int J Biol Macromol ; 279(Pt 1): 135113, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39208903

RESUMO

Tetracycline hydrochloride (TCH) removal from wastewater has drawn much attention recently, although it still remains challenging. Herein, Fe-based metal-organic frameworks (MOFs) incorporated nanofibrous membranes were prepared by green electrospinning and applied as adsorbents to remove TCH. The presence of MOFs noticeably improved specific surface area of the nanofibrous membranes, and adsorption capability increased with the amount of MOFs within membranes. As the temperature increased, the amount of TCH that was adsorbed continuously reduced, and the maximum adsorption capacity (248.5 mg/g) was attained at 273 K. The adsorption behavior of the nanofibrous membranes followed Langmuir isotherm model and pseudo-second-order kinetic model. Thermodynamic parameters suggested that the adsorption process was spontaneous and exothermic. A series of interactions between the membrane and TCH, such as pore filling, coordination bonding, π-π interaction, hydrogen bonding interaction and electrostatic interaction, combined to enhance the adsorption performance. Good stability and adsorption capability were demonstrated by the nanofibrous membranes, suggesting that they could be used for effective and affordable water purification.

3.
Adv Sci (Weinh) ; : e2406381, 2024 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-39206871

RESUMO

Traditional light-driven metal-organic-frameworks (MOFs)-based micromotors (MOFtors) are typically constrained to two-dimensional (2D) motion under ultraviolet or near-infrared light and often demonstrate instability and susceptibility to ions in high-saline environments. This limitation is particularly relevant to employing micromotors in water purification, as real wastewater is frequently coupled with high salinity. In response to these challenges, ultrastable MOFtors capable of three-dimensional (3D) motion under a broad spectrum of light through thermophoresis and electrophoresis are successfully synthesized. The MOFtors integrated photocatalytic porphyrin MOFs (PCN-224) with a photothermal component made of polypyrrole (PPy) by three distinct methodologies, resulting in micromotors with different motion behavior and catalytic performance. Impressively, the optimized MOFtors display exceptional maximum velocity of 1305 ± 327 µm s-1 under blue light and 2357 ± 453 µm s-1 under UV light. In harsh saline environments, these MOFtors are not only maintain high motility but also exhibit superior tetracycline hydrochloride (TCH) removal efficiency of 3578 ± 510 mg g-1, coupling with sulfate radical-based advanced oxidation processes and peroxymonosulfate. This research underscores the significant potential of highly efficient MOFtors with robust photocatalytic activity in effectively removing TCH in challenging saline conditions, representing a substantial advancement in applying MOFtors within real-world water treatment technologies.

4.
Int J Biol Macromol ; 274(Pt 2): 133385, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38914402

RESUMO

This study synthesized a carboxymethyl chitosan-modified bimetallic Co/Zn-ZIF (CZ@CMC) with strong hydrophilicity and adsorption performance via the one-pot method. Tetracycline hydrochloride (TCH) was used as the model contaminant to evaluate the adsorption and peroxymonosulfate (PMS) activation properties of CZ@CMC. Mechanism showed that the adsorption behavior occurred through pore filling, electrostatic attraction, surface complexation, hydrogen bonding, and π-π stacking. In addition, a CZ@CMC/PMS system was constructed, which had excellent catalytic performance. The hydrophilicity and selective adsorption properties of CMC conferred a greatly accelerated CZ@CMC in catalyzing the PMS process with kobs of 0.095 min-1, in which OH, 1O2, SO4-, O2-, and Co(III) were the main ROS which quenching tests, EPR, and chemical probe experiments verified. In addition, the degradation pathways of TCH were obtained utilizing DFT and HPLC-MS and analyzed to show that the system possessed a good detoxification capacity. This work is expected to provide a green, efficient, and stable strategy to enhance the adsorption properties of catalytic materials and subsequently their co-catalytic properties.


Assuntos
Quitosana , Cobalto , Estruturas Metalorgânicas , Tetraciclina , Zinco , Quitosana/química , Quitosana/análogos & derivados , Cobalto/química , Tetraciclina/química , Adsorção , Estruturas Metalorgânicas/química , Zinco/química , Catálise , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Interações Hidrofóbicas e Hidrofílicas , Peróxidos
5.
Front Chem ; 12: 1412457, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38863675

RESUMO

Water pollution caused by antibiotics is a growing problem and photodegradation by efficient catalysts is an environmentally friendly technology that can effectively degrade organic pollutants in water. Here, a novel method was innovatively used to synthesize niobium oxyfluoride (Nb3O7F) nanosheets decorated with Au nanoparticles, which is the first report for the composites of Au and Nb3O7F. We prepared the Nb3O7F nanosheets via hydrothermal synthesis followed by deposition of Au nanoparticles on their surface using HAuCl4. The prepared samples were characterized by XRD, HRTEM, XPS, and UV-Vis. The diameters of most Au NPs are ranging from 5 to 25 nm with an average size of about 16.9 nm, as well as the Nb3O7F nanosheets in size ranging from 200 nm to 700 nm. The chemical composition of the Au-Nb3O7F showed a Au/Nb atomic ratio of 1/10, as well as a Nb/O/F ratio of 3/7/1. UV-Vis spectrum reveals a largest absorption peak at 520 nm for the Au-Nb3O7F nanosheets. The prepared Au-Nb3O7F nanomaterials were applied to the visible-light photodegradation of tetracycline hydrochloride, with the photocatalytic degradation rate reached more than 50% under the optimal conditions within 1 h. Capture experiments indicated that h+ and •O2 - are the main active substances involved during the course of the photodegradation. Furthermore, the proposed mechanism for the photodegradation of the novel Au-Nb3O7F nanosheets was given.

6.
Environ Res ; 259: 119504, 2024 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-38945514

RESUMO

While treating zinc-containing wastewater, recovering zinc for reuse as a secondary resource has significant environmental and economic benefits. Herein, based on the alkali-activated tourmaline tailings geopolymers (TTG) after adsorption of zinc ions (Zn (II)), a series of new composites with in-situ construction ZnS nanoparticles on TTG (ZnS/TTG) were synthesized, and used as photocatalysts for the photodegradation of tetracycline hydrochloride (TCH) in solution. Specifically, ZnS nanoparticles were uniformly and stably distributed in the layered structure of TTG, interweaving with each other to generate an interfacial electric field, which could induce more photocarrier generation. Meanwhile, TTG acted as an electron acceptor to accelerate the electron transfer at the interface, thus enhancing the photodegradation activity for TCH. The active radical quenching experiments combined with the ESR indicated that the active species produced during the photocatalytic degradation of TCH by ZnS/TTG composites were •O2- and photogenerated h+. When the initial concentration of Zn (II) was 60 mg/L, the synthesized 60-ZnS/TTG composites (0.5 g/L) reached 91.53% degradation efficiency of TCH (10 mg/L) at pH = 6. Furthermore, the possible pathways and mechanism of 60-ZnS/TTG composites photodegraded TCH were revealed with the aid of degraded intermediates. This report not only proposed valuable references for reusing heavy metal ions and removing TCH from wastewater, but also provided promising ideas for realizing the conversion of used adsorbents into high-efficiency photocatalysts.


Assuntos
Fotólise , Tetraciclina , Águas Residuárias , Poluentes Químicos da Água , Compostos de Zinco , Zinco , Tetraciclina/química , Águas Residuárias/química , Zinco/química , Poluentes Químicos da Água/química , Compostos de Zinco/química , Sulfetos/química , Polímeros/química , Eliminação de Resíduos Líquidos/métodos
7.
Environ Sci Pollut Res Int ; 31(29): 42075-42087, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38861065

RESUMO

Highly active catalysts with salt and acid/alkali resistance are desired in peroxymonosulfate (PMS) activation processes and marine environment applications. F- and Cl-doped graphene (F-GN and Cl-GN) were prepared via electronegative and atom radius adjustment for tetracycline hydrochloride (TCH) pollution removal to satisfy these requirements. The introduction of special F and Cl functionalities into graphene exhibits superior electron transfer properties for PMS activation, considering the experimental and density functional theory (DFT) calculation results. The TCH degradation efficiency reached up to 80% under various pH and salt disturbance conditions with F-GN and Cl-GN. Cl-GN exhibited an activity superior to F-GN due to the higher electron polarization effect of C atoms adjacent to Cl atoms. The presence of more positive charged C sites in Cl-GN (around Cl doping) is more favorable for PMS attachment and sequence radical generation than F-GN. In addition, the main active species functionalized during reaction included ·OH and SO4-·, and the stability of F-GN and Cl-GN was confirmed to be over 60% by recycle test. Final research results provide an effective strategy for designing and preparing PMS activators resistant to salt, acid, and alkali, thereby expanding their application potential.


Assuntos
Grafite , Peróxidos , Tetraciclina , Tetraciclina/química , Grafite/química , Catálise , Peróxidos/química
8.
J Environ Manage ; 365: 121608, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38943751

RESUMO

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/química
9.
Pharmaceutics ; 16(6)2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38931950

RESUMO

The high prevalence of acne, which affects nearly 85% of adolescents and young adults, underscores the importance of exploring new therapeutic solutions. The aim of the present study was to design a stable hydrogel formulation containing tetracycline hydrochloride (TC) in the presence of ethanol at various concentration levels. The antibiotic stability was assessed over a period of 84 days using the HPLC method. The rheological properties of the formulations and their microbiological activity were also evaluated. Hydrogels without ethanol and those containing 5% and 25% alcohol showed similar rheological properties and high stability of the antibiotic throughout the observation period. The formulation with the highest ethanol content of 50% differed significantly from the others in terms of rheological properties. Although the flow and viscosity curves were like those of the other formulations, the viscosity values were significantly lower. The stability of tetracycline in this formulation was also significantly lower, and by the 84th day of observation, the concentration of the drug had decreased to almost 45% of its initial content. The formulations containing the highest concentration of ethanol displayed the highest activity against the biofilm of the acne-causing agent, Cutibacterium acnes. The study demonstrated the possibility of developing stable and antimicrobial effective hydrogel formulations with tetracycline and ethanol as a substance enhancing drug penetration into the hair follicles.

10.
J Hazard Mater ; 472: 134526, 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38704908

RESUMO

The proliferation of toxic organisms caused by changes in the marine environment, coupled with the rising human activities along the coastal lines, has resulted in an increasing number of stinging incidents, posing a serious threat to public health. Here, we evaluated the systemic toxicity of the venom in jellyfish Chrysaora quinquecirrha at both cellular and animal levels, and found that jellyfish tentacle extract (TE) has strong lethality accompanied by abnormal elevation of blood biochemical indicators and pathological changes. Joint analysis of transcriptome and proteome indicated that metalloproteinases are the predominant toxins in jellyfish. Specially, two key metalloproteinases DN6695_c0_g3 and DN8184_c0_g7 were identified by mass spectrometry of the red blood cell membrane and tetracycline hydrochloride (Tch) inhibition models. Structurally, molecular docking and kinetic analysis are employed and observed that Tch could inhibit the enzyme activity by binding to the hydrophobic pocket of the catalytic center. In this study, we demonstrated that Tch impedes the metalloproteinase activity thereby reducing the lethal effect of jellyfish, which suggests a potential strategy for combating the health threat of marine toxic jellyfish.


Assuntos
Venenos de Cnidários , Metaloproteases , Simulação de Acoplamento Molecular , Cifozoários , Animais , Metaloproteases/química , Metaloproteases/metabolismo , Venenos de Cnidários/química , Tetraciclina/toxicidade , Transcriptoma/efeitos dos fármacos
11.
Environ Sci Pollut Res Int ; 31(26): 38399-38415, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38805135

RESUMO

In this paper, a novel CeO2/Co3[Co(CN)6]2 (CeO2/PBACo-Co) composite was prepared with co-precipitation and utilized to activate peroxymonosulfate (PMS) to eliminate tetracycline hydrochloride (TCH). Catalyst screening showed that the composite with a CeO2:PBACo-Co mass ratio of 1:5 (namely, 0.2-CeO2/PBACo-Co) had the best performance. The degradation efficiency of TCH in 0.2-CeO2/PBACo-Co/Oxone system was investigated. The experimental results illustrated that 98% of 50 mg/L TCH and 48.5% of TOC were degraded by 50 mg/L 0.2-CeO2/PBACo-Co and 400 mg/L Oxone within 120 min at 25 °C and initial pH 5.3. Recycling studies showed that the elimination rate of TCH can still achieve 85.8% after five cycles, suggesting that 0.2-CeO2/PBACo-Co composite processes good reusability. Trapping experiments and EPR tests revealed that the reaction system produced multiple active species (1O2, O2•-, SO4•-, and •OH). We proposed the catalytic mechanism of 0.2-CeO2/PBACo-Co for PMS activation, which mainly involves the promoted Co3+/Co2+ cycle by Ce3+ donated electrons. These results indicate that CeO2/PBACo-Co composite is an effective catalyst for wastewater remediation.


Assuntos
Cério , Tetraciclina , Poluentes Químicos da Água , Cério/química , Catálise , Tetraciclina/química , Poluentes Químicos da Água/química , Cobalto/química , Peróxidos/química , Purificação da Água/métodos
12.
Environ Sci Pollut Res Int ; 31(21): 31562-31576, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38632202

RESUMO

The escalating demand for the antibiotic drug tetracycline hydrochloride (TCH) contributes to an increased release of its residues into land and water bodies, which poses risks to both aquatic life and human health. Therefore, it is precedence to effectively degrade TCH residues to protect environment from their long-term impacts. In this aspect, the present study entails the synthesis of zirconia (ZrO2) nanostructures and focuses on the enhancement in the catalytic performance of ZrO2 nanostructures by employing reduced graphene oxide (RGO) as a solid support to synthesize ZrO2-enriched RGO-based photocatalysts (ZrO2-RGO) for the degradation of TCH. The study delves into comprehensive spectroscopic and microscopic investigations and their photodegradation assessments. Powder XRD and HR-TEM studies depicted the phase crystallinity and also displayed uniform distribution of ZrO2 nanostructures with spherical morphology within ZrO2-RGO. This corresponds to high surface-to-volume ratios, providing a substantial number of active sites for light absorption and generation of e--h+ pairs. Moreover, the heterojunctions created between RGO and ZrO2 nanostructures promoted the interspecies electron transfer which prolonged the recombination time of e- and h+ than pure ZrO2 nanostructures, accounted for enhanced degradation of TCH using ZrO2-RGO. The photocatalytic activity of as-synthesized materials were examined under visible and UV light irradiation. The degradation efficiency of ~ 73.82% was achieved using ZrO2-RGO-based photocatalyst with rate constant k = 0.007023 min-1 under visible-light illumination. Moreover, under UV-light, the degradation rate was explicated to be k = 0.01017 min-1 with ~ 85.56% degradation of TCH antibiotics within 180 mins. Hence, the synthesized ZrO2-enriched RGO-based photocatalysts represents a promising potential for the effective degradation of pharmaceutical compounds, particularly TCH under visible and UV-light irradiation.


Assuntos
Grafite , Nanoestruturas , Fotólise , Tetraciclina , Zircônio , Grafite/química , Tetraciclina/química , Zircônio/química , Nanoestruturas/química , Catálise
13.
Small ; : e2309656, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38686693

RESUMO

Bi/CeO2 (BC-x) photocatalysts are successfully prepared by solvothermal loading Bi nanoparticles and Bi-doped CeO2 derived by Ce-MOF (Ce-BTC). Formaldehyde gas (HCHO) and tetracycline hydrochloride (HTC) are used to evaluate the photocatalytic activity of the synthesized Bi/CeO2. For BC-1000 photocatalyst, the degradation of HTC by 420 nm < λ < 780 nm light reaches 91.89% for 90 min, and HCHO by 350 nm < λ < 780 nm light reaches 94.66% for 120 min. The photocatalytic cycle experiments prove that BC-1000 has good cyclic stability and repeatability. The results of photoluminescence spectra, fluorescence lifetime, photocurrent response, and electrochemical impedance spectroscopy showed that the SPR (Surface Plasmon Resonance) effect of Bi nanoparticles acted as a bridge and promoted electron transfer and enhanced the response-ability of Bi/CeO2 to visible light. Bi-doping produced more oxygen vacancies to provide adsorption sites for adsorbing oxygen and generated more ·O2 - thus promoting photocatalytic reactions. The mechanism of photocatalytic degradation is analyzed in detail utilizing active free radical capture experiments and electron paramagnetic resonance (EPR) characterization. The experimental results indicate that ·O2 - and h+ active free radicals significantly promote the degradation of pollutants.

14.
Environ Res ; 251(Pt 1): 118566, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38447606

RESUMO

Both g-C3N4 and Bi2O2CO3 are good photocatalysts for the removal of antibiotic pollutants, but their morphological modulation and catalytic performance need to be further improved. In this study, the calcination-hydrothermal method is used to prepare a O-g-C3N4@Bi2O2CO3 (CN@BCO) composite photocatalyst from dicyandiamide and bismuth nitrate. The prepared catalyst is characterized through various methods, including X-ray diffraction (XRD) and transmission electron microscopy (TEM). Further, the effects of different parameters, such as catalyst concentration and initial pH of the reaction solution, on its photocatalytic activity are investigated. The results show that the CN@BCO sample achieves an optimal degradation rate of 98.1% for tetracycline hydrochloride (TCH) with a concentration of 20 mg/L and a removal rate of 69.4% for total organic carbon (TOC) at 40 min. The quenching experiments show that ·O2-, h+, and ·OH participate in the photocatalytic process, with ·O2- being the most dominant active species. The toxicity of the predicted TCH degradation intermediates is analyzed using Toxicity Estimation Software Tool (TEST). Overall, the CN@BCO composite exhibits excellent photocatalytic performance, making it a promising candidate for environmental purification and wastewater treatment.


Assuntos
Bismuto , Tetraciclina , Águas Residuárias , Poluentes Químicos da Água , Tetraciclina/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Águas Residuárias/química , Bismuto/química , Catálise , Antibacterianos/química , Nanofios/química , Compostos de Nitrogênio/química , Nitrilas/química , Porosidade , Grafite
15.
J Hazard Mater ; 469: 134045, 2024 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-38492388

RESUMO

Tetracycline hydrochloride (TCH), a prevalent antibiotic in aquaculture for treating bacterial infections, poses challenges for on-site detection. This study employed the reversed-phase microemulsion method to synthesize a uniform nano metal-organic framework (MOF) material, europium-benzene-p-dicarboxylic acid (Eu-BDC), doped with Tb3+ to form a dual-emission fluorescence probe. By leveraging the combined a-photoinduced electron-transfer (a-PET) and inner filter effect (IFE) mechanisms, high-sensitivity TCH detection in Carassius auratus and Ruditapes philippinarum was achieved. The detection range for TCH is 0.380-75 µM, with a low limit of detection (LOD) at 0.115 µM. Upon TCH binding, Eu-BDC fluorescence rapidly decreased, while Tb3+ fluorescence remained constant, establishing a ratiometric fluorescence change. Investigation into the TCH quenching mechanism on Eu-BDC was conducted using time-dependent density functional theory (TD-DFT) calculations and fluorescence quenching kinetic equations, suggesting a mixed quenching mechanism. Furthermore, a novel photoelectric conversion fluorescence detection device (FL-2) was developed and evaluated in conjunction with high-performance liquid chromatography-diode-array detection (HPLC-DAD). This is the first dedicated fluorescence device for TCH detection, showcasing superior photoelectric conversion performance and stability that reduces experimental errors associated with smartphone photography methods, presenting a promising avenue for on-site rapid TCH detection.


Assuntos
Estruturas Metalorgânicas , Tetraciclina , Animais , Espectrometria de Fluorescência/métodos , Antibacterianos , Európio , Corantes Fluorescentes , Água Doce
16.
J Colloid Interface Sci ; 664: 520-532, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38484520

RESUMO

The instability and high electron-hole recombination have limited the application of black phosphorus (BP) as an excellent photocatalyst. To address these challenges, poly dimethyl diallyl ammonium chloride (PDDA), poly (allylamine hydrochloride) (PAH), and polyethyleneimine (PEI) are introduced to the functionalization of BP (F-BP), which can not only enhance its stability, but also boost the carrier transfer. Furthermore, a high-performance heterojunction photocatalyst is fabricated using F-BP and titania nanosheets (TNs) via a layer-by-layer self-assembly approach. The experimental outcomes unequivocally indicate that F-BP exhibits fast charge migration compared to BP. The density functional theory (DFT), in situ Kelvin-probe force microscopy (KPFM) and other advanced characterization techniques collectively unfold that PDDA modified BP can notably boost separation and propagation of charges, along with an enhanced carrier abundance. In summary, this novel strategy of using polyelectrolytes to enhance the electron transfer and the stability of BP permits immense potential in building next-generation BP-based high efficiency photocatalysts.

17.
Environ Res ; 249: 118362, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38325787

RESUMO

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.


Assuntos
Ferro , Peróxidos , Tetraciclina , Poluentes Químicos da Água , Tetraciclina/química , Poluentes Químicos da Água/química , Peróxidos/química , Ferro/química , Níquel/química , Antibacterianos/química , Oxirredução , Purificação da Água/métodos
18.
Molecules ; 29(4)2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38398521

RESUMO

Oily sludge-derived activated carbon was prepared using the potassium hydroxide (KOH) activation method using oily sludge as a raw material, and one-factor experiments determined the best conditions for preparing activated carbon. The activated carbon's morphological structure and surface chemical properties were analyzed by scanning different characterization tools, and the adsorption behavior of tetracycline hydrochloride was investigated. The results showed that the optimum conditions for preparing oily sludge-derived activated carbon were an activation temperature of 400 °C, activation time of 30 min, activator concentration of 1 mol/L, and impregnation ratio of 2 mL/g. After activation, the activated carbon had more pores and a more orderly crystal structure arrangement, the specific surface area was 2.07 times higher than that before activation, and the surface was rich in functional groups such as -HO, -C-O, -C=C, and -C-H, which increased the active sites of activated carbon. Physicochemical effects dominated the adsorption process. It belonged to the spontaneous heat absorption process under the quasi-secondary kinetic and Langmuir isothermal models. The maximum monolayer adsorption capacity of KOH-activated carbon was 205.1 mg·g-1.


Assuntos
Hidróxidos , Compostos de Potássio , Esgotos , Poluentes Químicos da Água , Esgotos/química , Carvão Vegetal/química , Tetraciclina , Adsorção , Óleos , Cinética , Poluentes Químicos da Água/química
19.
J Hazard Mater ; 468: 133816, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38377912

RESUMO

Developing eco-friendly and efficient technologies for treating antibiotic wastewater is crucial. Traditional methods face challenges in incomplete removal, high costs, and secondary pollution. Heterogeneous peroxymonosulfate (PMS) activation assisted by visible light shows promise, but suitable activators remain a huge challenge. Here, we synthesized cost-effective carbon nitride/bismuth bromide oxide (CN/BiOBr) heterojunctions. Such a heterojunction achieved rapid PMS activation, achieving over 90.00% tetracycline (TC) removal only within 1 min (kobs of 2.23 min-1), surpassing previous systems by nearly 1-2 orders of magnitude and even remarkably superior to the popular single-atom catalysts. The system exhibited self-cleaning properties, maintaining activity after 8 cycles and stability across a wide pH range (3.01 to 9.03). Quenching experiments and theoretical calculations elucidated the exclusive •O2- species involvement and removal pathways. Eco-toxicity assessment and total organic carbon results confirmed simultaneous degradation, detoxification, and mineralization. This system also showed excellent resistance to environmental factors, e.g., coexisting anions, varying pH, and water sources, and demonstrated potential in coking and medical wastewater purification. This study presents a novel technique for rapidly decontaminating antibiotic wastewater through visible light-assisted PMS activation and introduces innovative bionic catalytic oxidation combining light and darkness for practical applications.


Assuntos
Antibacterianos , Águas Residuárias , Peróxidos/química , Tetraciclina , Luz
20.
Talanta ; 271: 125707, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38280265

RESUMO

The synergistic effect of sodium dodecyl sulfate (SDS) and Mg2+ could significantly enhance the fluorescence intensity of enoxacin (ENO) at λex/λem = 269.2 nm/385.6 nm, ofloxacin (OFL) at λex/λem = 290.8 nm/466.2 nm and tetracycline hydrochloride (TCH) at λex/λem = 372.6 nm/514.8 nm. Moreover, when the wavelength difference (Δλ) was chosen 135 nm, the synchronous fluorescence spectra of the three antibiotic complexes could be well separated and the interference of the samples matrix were eliminated primely. Therefore, only one synchronous fluorescence scan was needed to simultaneously determine the three antibiotics. Based on these facts, a synchronous fluorescence spectrometry combining fluorescence sensitization for highly sensitive and selective determination of ENO, OFL and TCH residues in wastewater was developed for the first time. The experimental results showed that the concentrations of ENO, OFL and TCH in the range of 0.5-550 ng mL-1, 1-1500 ng mL-1 and 10-5500 ng mL-1 showed a good linear relationship with fluorescence intensity. The limits of detection were 0.0599 ng mL-1, 0.115 ng mL-1 and 0.151 ng mL-1, respectively. The recoveries of the actual sample were 87.50%-99.99 %, 93.00%-98.50 % and 85.70%-98.42 %, respectively. Overall, the novel synchronous fluorescence spectrometry established in the experiment has the advantages of high sensitivity, good selectivity, fast detection speed and high accuracy. It has been successfully applied to the detection of residual amounts of ENO, OFL and TCH in wastewater with satisfactory results.


Assuntos
Enoxacino , Ofloxacino , Tetraciclina , Águas Residuárias , Espectrometria de Fluorescência/métodos , Antibacterianos
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