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1.
J Environ Sci (China) ; 145: 107-116, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38844311

RESUMO

High energy consumption has seriously hindered the development of Fenton-like reactions for the removal of refractory organic pollutants in water. To solve this problem, we designed a novel Fenton-like catalyst (Cu-PAN3) by coprecipitation and carbon thermal reduction. The catalyst exhibits excellent Fenton-like catalytic activity and stability for the degradation of various pollutants with low H2O2 consumption. The experimental results indicate that the dual reaction centers (DRCs) are composed of Cu-N-C and Cu-O-C bridges between copper and graphene-like carbon, which form electron-poor/rich centers on the catalyst surface. H2O2 is mainly reduced at electron-rich Cu centers to free radicals for pollutant degradation. Meanwhile, pollutants can be oxidized by donating electrons to the electron-poor C centers of the catalyst, which inhibits the ineffective decomposition of H2O2 at the electron-poor centers. This therefore significantly reduces the consumption of H2O2 and reduces energy consumption.


Assuntos
Peróxido de Hidrogênio , Poluentes Químicos da Água , Peróxido de Hidrogênio/química , Catálise , Poluentes Químicos da Água/química , Ferro/química , Oxirredução , Cobre/química , Modelos Químicos
2.
J Environ Sci (China) ; 145: 128-138, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38844313

RESUMO

Zeolites are a promising support for Pd catalysts in lean methane (CH4) combustion. Herein, three types of zeolites (H-MOR, H-ZSM-5 and H-Y) were selected to estimate their structural effects and deactivation mechanisms in CH4 combustion. We show that variations in zeolite structure and surface acidity led to distinct changes in Pd states. Pd/H-MOR with external high-dispersing Pd nanoparticles exhibited the best apparent activity, with activation energy (Ea) at 73 kJ/mol, while Pd/H-ZSM-5 displayed the highest turnover frequency (TOF) at 19.6 × 10-3 sec-1, presumably owing to its large particles with more step sites providing active sites in one particle for CH4 activation. Pd/H-Y with dispersed PdO within pore channels and/or Pd2+ ions on ion-exchange sites yielded the lowest apparent activity and TOF. Furthermore, Pd/H-MOR and Pd/H-ZSM-5 were both stable under a dry condition, but introducing 3 vol.% H2O caused the CH4 conversion rate on Pd/H-MOR drop from 100% to 63% and that on Pd/H-ZSM-5 decreased remarkably from 82% to 36%. The former was shown to originate from zeolite structural dealumination, and the latter principally owed to Pd aggregation and the loss of active PdO.


Assuntos
Metano , Paládio , Zeolitas , Zeolitas/química , Metano/química , Catálise , Paládio/química , Modelos Químicos
3.
J Environ Sci (China) ; 145: 216-231, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38844321

RESUMO

Catalytic ozonation is an effective wastewater purification process. However, the low ozone mass transfer in packed bubble columns leads to low ozone utilization efficiency (OUE), poor organic degradation performance, and high energy consumption. Therefore, there is an urgent need to develop efficient supported catalysts that can enhance mass transfer and performance. However, the reaction mechanism of the support on ozone mass transfer remains unclear, which hinders the development of catalytic ozonation applications. In this study, lava rocks (LR)-supported catalysts, specifically CuMn2O4@LR and MnO2Co3O4@LR, were proposed for catalytic ozonation of IBP degradation due to their superior catalytic activity, stability, and high OUE. Addition of CuMn2O4@LR or MnO2Co3O4@LR increased IBP removal efficiency from 85% to 91% or 88%, and reduced energy consumption from 2.86 to 2.14 kWh/m3 or 2.60 kWh/m3, respectively. This improvement was attributed to LR-supported catalysts enhancing mass transfer and promoting O3 decomposition to generate •OH and •O2-, leading to IBP degradation. Furthermore, this study investigated the effects of ozone dose, supporter sizes, and catalyst components on ozone-liquid mass transfer. The results revealed that the size of the supporter influenced stacked porosity and consequently affected ozone mass transfer. Larger-sized LR (kLa= 0.172 min-1) exhibited better mass transfer compared to smaller-sized supports. Based on these findings, it was concluded that both CuMn2O4@LR and MnO2Co3O4@LR are potential catalysts for catalytic ozonation in residual IBP degradation of pharmaceutical wastewater, and LR showed good credibility as a catalyst supporter. Understanding the effects of supporters and active components on ozone mass transfer provides a fundamental principle for designing supported catalysts in catalytic ozonation applications.


Assuntos
Ibuprofeno , Ozônio , Eliminação de Resíduos Líquidos , Poluentes Químicos da Água , Ozônio/química , Catálise , Poluentes Químicos da Água/química , Ibuprofeno/química , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Purificação da Água/métodos
4.
Sci Rep ; 14(1): 12818, 2024 06 04.
Artigo em Inglês | MEDLINE | ID: mdl-38834602

RESUMO

Recent years have seen an increase in research on biodiesel, an environmentally benign and renewable fuel alternative for traditional fossil fuels. Biodiesel might become more cost-effective and competitive with diesel if a solid heterogeneous catalyst is used in its production. One way to make biodiesel more affordable and competitive with diesel is to employ a solid heterogeneous catalyst in its manufacturing. Based on X-ray diffraction (XRD) and Fourier Transform infrared spectroscopy (FTIR), the researchers in this study proved their hypothesis that iron oxide core-shell nanoparticles were generated during the green synthesis of iron-based nanoparticles (FeNPs) from Camellia Sinensis leaves. The fabrication of spherical iron nanoparticles was successfully confirmed using scanning electron microscopy (SEM). As a heterogeneous catalyst, the synthesised catalyst has shown potential in facilitating the conversion of algae oil into biodiesel. With the optimal parameters (0.5 weight percent catalytic load, 1:6 oil-methanol ratio, 60 °C reaction temperature, and 1 h and 30 min reaction duration), a 93.33% yield was attained. This may be due to its acid-base property, chemical stability, stronger metal support interaction. Furthermore, the catalyst was employed for transesterification reactions five times after regeneration with n-hexane washing followed by calcination at 650 °C for 3 h.


Assuntos
Biocombustíveis , Camellia sinensis , Folhas de Planta , Folhas de Planta/química , Catálise , Camellia sinensis/química , Ferro/química , Nanopartículas Metálicas/química , Difração de Raios X , Esterificação , Espectroscopia de Infravermelho com Transformada de Fourier
5.
Sci Rep ; 14(1): 12877, 2024 06 05.
Artigo em Inglês | MEDLINE | ID: mdl-38834648

RESUMO

This study reports the antibacterial and antibiofilm activities of Magnesium ferrite nanoparticles (MgFe2O4) against gram-positive and gram-negative bacteria. The photocatalytic degradation of Carbol Fuchsin (CF) dye (a class of dyestuffs that are resistant to biodegradation) under the influence of UV-light irradiation is also studied. The crystalline magnesium ferrite (MgFe2O4) nanoparticles were synthesized using the co-precipitation method. The morphology of the resulting nanocomposite was examined using scanning electron microscopy (SEM), while transmission electron microscopy (TEM) was employed for further characterization of particle morphology and size. Fourier transform infrared (FTIR) spectroscopy and X-ray diffraction (XRD) were utilized to analyze the crystalline structure, chemical composition, and surface area, respectively. Optical properties were evaluated using UV-Vis spectroscopy. The UV-assisted photocatalytic performance of MgFe2O4 nanoparticles was assessed by studying the decolorization of Carbol fuchsin (CF) azo dye. The crystallite size of the MgFe2O4 nanoparticles at the (311) plane, the most prominent peak, was determined to be 28.5 nm. The photocatalytic degradation of 10 ppm CF using 15 mg of MgFe2O4 nanoparticles resulted in a significant 96% reduction after 135 min at ambient temperature (25 °C) and a pH value of 9. Additionally, MgFe2O4 nanoparticles exhibited potent antibacterial activity against E. coli and S. aureus in a dose dependent manner with maximum utilized concentration of 30 µg/ml. Specifically, MgFe2O4 nanoparticles demonstrated substantial antibacterial activity via disk diffusion and microbroth dilution tests with zones of inhibition and minimum inhibitory concentrations (MIC) for E. coli (26.0 mm, 1.25 µg/ml) and S. aureus (23.0 mm, 2.5 µg/ml), respectively. Moreover, 10.0 µg/ml of MgFe2O4 nanoparticles elicited marked percent reduction in biofilm formation by E. coli (89%) followed by S. aureus (78.5%) after treatment. In conclusion, MgFe2O4 nanoparticles demonstrated efficient dye removal capabilities along with significant antimicrobial and antibiofilm activity against gram-positive and gram-negative bacterial strains suggesting their potential as promising antimicrobial and detoxifying agents.


Assuntos
Antibacterianos , Biofilmes , Compostos Férricos , Nanopartículas de Magnetita , Biofilmes/efeitos dos fármacos , Compostos Férricos/química , Compostos Férricos/farmacologia , Catálise , Nanopartículas de Magnetita/química , Antibacterianos/farmacologia , Antibacterianos/química , Testes de Sensibilidade Microbiana , Escherichia coli/efeitos dos fármacos , Raios Ultravioleta , Staphylococcus aureus/efeitos dos fármacos , Magnésio/química , Magnésio/farmacologia , Espectroscopia de Infravermelho com Transformada de Fourier
6.
Luminescence ; 39(6): e4799, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38858760

RESUMO

In this study, tellurium-doped and undoped metal oxide nanoparticles (NPs) (ZnO, Mn3O4, SnO2) are compared, and a practical method for their synthesis is presented. Nanocomposites were created using the coprecipitation process, and comparisons between the three material categories under study were made using a range of characterization methods. The produced materials were subjected to structural, morphological, elemental composition, and functional group analyses using XRD, FESEM in combination with EDS, and FTIR. The optical characteristics in terms of cutoff wavelength were evaluated using UV-visible spectroscopy. Catalyzing the breakdown of methylene blue (MB) dye, the isolated nanocomposites demonstrated very consistent behavior when utilized as catalysts. Regarding both doped and undoped ZnO NPs, the maximum percentage of degradation was found to be 98% when exposed to solar Escherichia coli and Staphylococcus aureus, which stand for gram-positive and gram-negative bacteria, respectively, and were chosen as model strains for both groups using the disk diffusion technique in the context of in vitro antibacterial testing. Doped and undoped ZnO NPs exhibited greater antibacterial efficacy, with significant inhibition zones measuring 31.5 and 37.8 mm, compared with other metal oxide NPs.


Assuntos
Antibacterianos , Escherichia coli , Nanopartículas Metálicas , Testes de Sensibilidade Microbiana , Staphylococcus aureus , Telúrio , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/síntese química , Telúrio/química , Telúrio/farmacologia , Staphylococcus aureus/efeitos dos fármacos , Catálise , Nanopartículas Metálicas/química , Escherichia coli/efeitos dos fármacos , Processos Fotoquímicos , Azul de Metileno/química , Azul de Metileno/farmacologia , Óxido de Zinco/química , Óxido de Zinco/farmacologia , Manganês/química , Manganês/farmacologia , Estanho/química , Estanho/farmacologia , Tamanho da Partícula , Óxidos/química , Óxidos/farmacologia
7.
Environ Geochem Health ; 46(7): 246, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38864996

RESUMO

In the pursuit of efficient photocatalytic materials for environmental applications, a new series of g-C3N4/N-doped CeO2 nanocomposites (g-C3N4/N-CeO2 NCs) was synthesized using a straightforward dispersion method. These nanocomposites were systematically characterized to understand their structural, optical, and chemical properties. The photocatalytic performance of g-C3N4/N-CeO2 NCs was evaluated by investigating their ability to degrade methylene blue (MB) dye, a model organic pollutant. The results demonstrate that the integration of g-C3N4 with N-doped CeO2 NCs reduces the optical energy gap compared to pristine N-doped CeO2, leading to enhanced photocatalytic efficiency. It is benefited from the existence of g-C3N4/N-CeO2 NCs not only in promoting the charge separation and inhibits the fast charge recombination but also in improving photocatalytic oxidation performance. Hence, this study highlights the potential of g-C3N4/N-CeO2 NCs as promising candidates for various photocatalytic applications, contributing to the advancement of sustainable environmental remediation technologies.


Assuntos
Cério , Luz , Azul de Metileno , Nanocompostos , Azul de Metileno/química , Cério/química , Nanocompostos/química , Catálise , Poluentes Químicos da Água/química , Grafite/química , Processos Fotoquímicos , Fotólise , Compostos de Nitrogênio
8.
Mikrochim Acta ; 191(6): 361, 2024 06 01.
Artigo em Inglês | MEDLINE | ID: mdl-38822891

RESUMO

A one-shot CO2 laser-based strategy to generate conductive reduced graphene oxide (rGO) decorated with nanoceria (nCe) is proposed. The 2D/0D rGO-nCe films, integrated as catalytic sensing layers in paper-based sensors, were employed for on-site monitoring of indoor fogging treatments against Listeria monocytogenes (Lm), a ubiquitous pathogenic bacterium. The rGO-nCe laser-assisted synthesis was optimized to preserve the rGO film morphological and electron-transfer features and simultaneously integrate catalytic nCe. The films were characterized by microscopical (SEM), spectroscopical (EDX, Raman, and FTIR), and electrochemical techniques. The most performing film was integrated into a nitrocellulose substrate, and the complete sensor was assembled via a combination of xurography and stencil printing. The rGO-nCe sensor's catalytic activity was proved toward the detection of H2O2, obtaining sensitive determination (LOD = 0.3 µM) and an extended linear range (0.5-1500 µM). Eventually, the rGO-nCe sensor was challenged for the real-time continuous monitoring of hydrogen peroxide aerosol during no-touch fogging treatment conducted following the EU's recommendation for biocidal product use. Treatment effectiveness was proved toward three Lm strains characterized by different origins, i.e., type strain ATCC 7644, clinical strain 338, and food strain 641/6II. The sensor allows for discrimination and quantification treatments at different environmental biocidal amounts and fogging times, and correlates with the microbiological inhibition, promoting the proposed sensor as a useful tool to modulate and monitor no-touch treatments.


Assuntos
Desinfecção , Grafite , Peróxido de Hidrogênio , Lasers , Listeria monocytogenes , Papel , Grafite/química , Peróxido de Hidrogênio/química , Listeria monocytogenes/efeitos dos fármacos , Listeria monocytogenes/isolamento & purificação , Desinfecção/métodos , Cério/química , Limite de Detecção , Técnicas Eletroquímicas/métodos , Técnicas Eletroquímicas/instrumentação , Catálise
9.
J Environ Manage ; 362: 121338, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38823296

RESUMO

A series of Fe3O4@CuCr-LDH hybrids decorated with different amount of ZIF-8 (FLZ, 10-40 wt%) was prepared using simple methods and characterized with different techniques. The activity of the synthesized nanocomposites was investigated in the sonocatalytic degradation of tetracycline (TC) antibiotic from wastewater. When the content of ZIF-8 in the nanocomposite structure was 20 wt%, the FLZ-20 sonocatalyst exhibited the high performance in the sonocatalytic removal of TC. At optimum conditions (0.7 g/L catalyst dosage, pH of 7, 50 mg/L initial concentration of antibiotic, and 15 min sonication time) of the sonocatalytic removal of TC approached to 91.4% under ultrasonic irradiation (USI) using FLZ-20. This efficiency was much higher than those of obtained results by Fe3O4@CuCr-LDH and pristine ZIF-8. The formed ●OH and ●O2- exhibited the major roles in the sonocatalytic TC degradation process. The excellent performance of FLZ-20 can be attributed to the heterojunctions created between composite components, which could improve the electron transfer ability and effectively separate e-/h+ pairs. In addition, FLZ-20 showed the superior reusability and stability during three successive recycling. Moreover, the facile magnetically separation of the sonocatalyst from the aqueous solution was another outstanding feature, which prevents the formation of secondary pollutants. It can be concluded that the fabrication of heterojunctions is an efficient procedure to promote the sonocatalytic acting of the catalyst.


Assuntos
Tetraciclina , Tetraciclina/química , Catálise , Hidróxidos/química , Águas Residuárias/química , Nanocompostos/química , Poluentes Químicos da Água/química
10.
J Environ Manage ; 362: 121346, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38824884

RESUMO

The conversion of NO3--N to N2 is of great significance for zero discharge of industrial wastewater. Pd-Cu hydrogenation catalysis has high application prospects for the reduction of NO3--N to N2, but the existing form of Pd-Cu, the Pd-Cu mass ratio and the H2 evolution rate can affect the coverage of active hydrogen (*H) on the surface of Pd, thereby affecting N2 selectivity. In this work, mesoporous carbon (MC) is used as support to disperse Pd-Cu catalyst and is applied in an in-situ electrocatalytic H2 evolution system for NO3--N removal. The Pd-Cu particles with the average size of 6 nm are uniformly encapsulated in the mesopores of MC. Electrochemical in-situ H2 evolution can not only reduce the amount of H2 used, but the H2 bubbles can also be efficiently dispersed when PPy coated nickel foam (PPy/NF) is used as cathode. Moreover, the mesoporous structure of MC can further split H2 bubbles, reducing the coverage of *H on Pd. The highest 77% N2 selectivity and a relatively faster NO3--N removal rate constant (0.10362 min-1) can be achieved under the optimal conditions, which is superior to most reported Pd-Cu catalytic systems. The prepared catalyst is further applied to the denitrification of actual deplating wastewater. NO3--N with the initial concentration of 650 mg L-1 can be completely removed after 180 min of treatment, and the TN removal can be maintained at 72%.


Assuntos
Carbono , Hidrogênio , Nitratos , Nitrogênio , Águas Residuárias , Nitrogênio/química , Águas Residuárias/química , Hidrogênio/química , Carbono/química , Catálise , Nitratos/química , Cobre/química , Paládio/química , Poluentes Químicos da Água/química
11.
J Environ Manage ; 362: 121334, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38824890

RESUMO

A series of V-xCe/Ti catalysts was prepared by a step impregnation method with gradual increased Ce amount. Compared to the commercial V-W/Ti catalysts, the V-xCe/Ti catalysts exhibited considerably higher COx selectivity during the oxidation of naphthalene (Nap), and less intermediates or by-products were detected both in gas phase and on the surface of the catalysts. Through a series of characterizations, it was found that abundance of weak basic sites in the form of OH was introduced by Ce, as well as the oxygen vacancies caused by the redox cycle of V4++Ce4+↔V5++Ce3+. The weak basic sites introduced by Ce could greatly enhance the Nap adsorption, and the Nap adsorbed was quickly converted to naphthol on Ce-OH. Furthermore, V existed at a high valence with the interaction of V and Ce, and the oxygen vacancies also increased the Oads and OOH. It improved the redox ability and the regeneration of Ce-OH on V-xCe/Ti catalysts. The intermediates could be further oxidized, and the Ce-OH consumed in the reaction could recover quickly. Therefore, almost 100% Nap conversion and a high COx selectivity was observed in the V-xCe/Ti catalysts system.


Assuntos
Naftalenos , Oxirredução , Naftalenos/química , Catálise , Adsorção
12.
Phys Chem Chem Phys ; 26(23): 16529-16539, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38828872

RESUMO

This study reports on the effects of conformationally controlled amphiphilicity of antimicrobial peptides (AMPs) on their ability to coat TiO2 nanoparticles (NPs) and boost the photocatalytic antimicrobial effects of such NPs. For this, TiO2 NPs were combined with AMP EFK17 (EFKRIVQRIKDFLRNLV), displaying a disordered conformation in aqueous solution but helix formation on interaction with bacterial membranes. The membrane-bound helix is amphiphilic, with all polar and charged amino acid residues located at one side and all non-polar and hydrophobic residues on the other. In contrast, the d-enantiomer variant EFK17-d (E(dF)KR(dI)VQR(dI)KD(dF)LRNLV) is unable to form the amphiphilic helix on bacterial membrane interaction, whereas the W-residues in EFK17-W (EWKRWVQRWKDFLRNLV) boost hydrophobic interactions of the amphiphilic helix. Circular dichroism results showed the effects displayed for the free peptide, to also be present for peptide-coated TiO2 NPs, causing peptide binding to decrease in the order EFK17-W > EFK17 > EFK17-d. Notably, the formation of reactive oxygen species (ROS) by the TiO2 NPs was essentially unaffected by the presence of peptide coating, for all the peptides investigated, and the coatings stabilized over hours of UV exposure. Photocatalytic membrane degradation from TiO2 NPs coated with EFK17-W and EFK17 was promoted for bacteria-like model bilayers containing anionic phosphatidylglycerol but suppressed in mammalian-like bilayers formed by zwitterionic phosphatidylcholine and cholesterol. Structural aspects of these effects were further investigated by neutron reflectometry with clear variations observed between the bacteria- and mammalian-like model bilayers for the three peptides. Mirroring these results in bacteria-like model membranes, combining TiO2 NPs with EFK17-W and EFK17, but not with non-adsorbing EFK17-d, resulted in boosted antimicrobial effects of the resulting cationic composite NPs already in darkness, effects enhanced further on UV illumination.


Assuntos
Titânio , Titânio/química , Titânio/farmacologia , Catálise , Nanopartículas/química , Peptídeos Antimicrobianos/química , Peptídeos Antimicrobianos/farmacologia , Espécies Reativas de Oxigênio/metabolismo , Interações Hidrofóbicas e Hidrofílicas , Antibacterianos/química , Antibacterianos/farmacologia , Membrana Celular/efeitos dos fármacos , Membrana Celular/metabolismo , Anti-Infecciosos/química , Anti-Infecciosos/farmacologia
13.
Biochem J ; 481(12): 779-791, 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38829839

RESUMO

ent-Kaurene is a biosynthetic intermediate diterpene of phytohormone gibberellins, and is biosynthesized from geranylgeranyl diphosphate via ent-copalyl diphosphate (ent-CDP). The successive cyclization is catalyzed by two distinct diterpene synthases, ent-CDP synthase (ent-CPS) and ent-kaurene synthase (KS). Homologs of these diterpene synthase genes have been reported to be involved in the biosynthesis of specialized-metabolic diterpenoids for defense in several plant species, including rice (Oryza sativa). These diterpene synthases consist of three domains, αßγ domains. Active sites of ent-CPS exist at the interface of ß and γ domain, while those of KS are located within the α domain. We herein carried out domain-deletion experiments using several KSs and KS like enzymes (KSLs) to obtain insights into the roles of domains other than active-site domains. As previously reported in taxadiene synthase, deletion of γ or ßγ domains drastically decreased activities of specialized-metabolic OsKSL5, OsKSL8, OsKSL7 and OsKSL10 in O. sativa. However, unexpectedly, only α domains of several gibberellin-biosynthetic KSs, including OsKS1 in O. sativa, AtKS in Arabidopsis thaliana, TaKS in wheat (Triticum aestivum) and BdKS1 in Brachypodium distachyon, retained their original functions. Additionally, the specialized-metabolic OsKSL4, which is closely related to OsKS1, also functioned without its ßγ domains. Domain-swapping experiments showed that replacing ßγ domains in OsKSL7 with those from other KS/KSLs retained the OsKSL7 activity. Moreover, deletion of ßγ domains of bifunctional PpCPS/KS in moss (Physcomitrella patens) drastically impaired its KS-related activity. Thus, we demonstrate that monofunctional gibberellin-biosynthetic KSs are the unique diterpene synthases that retain their functions without ßγ domains.


Assuntos
Alquil e Aril Transferases , Giberelinas , Oryza , Proteínas de Plantas , Giberelinas/metabolismo , Alquil e Aril Transferases/metabolismo , Alquil e Aril Transferases/genética , Alquil e Aril Transferases/química , Oryza/enzimologia , Oryza/genética , Oryza/metabolismo , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Proteínas de Plantas/química , Domínio Catalítico , Diterpenos do Tipo Caurano/metabolismo , Diterpenos do Tipo Caurano/química , Arabidopsis/genética , Arabidopsis/enzimologia , Arabidopsis/metabolismo , Diterpenos/metabolismo , Diterpenos/química , Domínios Proteicos , Catálise
14.
J Environ Manage ; 362: 121342, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38830282

RESUMO

In this study, Ag/Bi2O3/Bi5O7I with s-scheme heterostructures were successfully synthesized in situ by nano-silver modification of CUA-17 and halogenated hydrolysis.The growth rate of Bi2O3 crystals was effectively controlled by adjusting the doping amount of Ag, resulting in the formation of a facet-coupling heterojunctions. Through the investigation of the microstructure and compositional of catalysts, it has been confirmed that an intimate facet coupling between the Bi2O3 (120) facet and the Bi5O7I (312) facet, which provides robust support for charge transfer. Under visible light irradiation, the AgBOI.3 heterojunction photocatalyst exhibited an outstanding degradation rate of 98.2% for Bisphenol A (BPA) with excellent stability. Further characterization using optical, electrochemical, impedance spectroscopy, and electron spin resonance techniques revealed significantly enhanced efficiency in photogenerated charge separation and transfer, and confirming the s-scheme structure of the photocatalyst. Density functional theory calculations was employed to elucidate the mechanism of BPA degradation and the degradation pathway of BPA was investigated by LC-MS. Finally, the toxicity of the degradation intermediates was evaluated using T.E.S.T software.


Assuntos
Compostos Benzidrílicos , Bismuto , Fenóis , Prata , Fenóis/química , Compostos Benzidrílicos/química , Bismuto/química , Catálise , Prata/química
15.
J Environ Manage ; 362: 121349, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38833929

RESUMO

The use of Ni-based catalysts is a common method for eliminating tar through catalytic cracking. Carbon deposition is the main cause of deactivation in Ni/ZSM-5 catalysts, with filamentous MWCNTs being the primary form of carbon deposits. This study investigates the formation and evolution of CNTs during the catalytic process of biomass tar to explore the mechanism behind carbon deposition. The effect of the 9Ni/10MWCNTs/81ZSM-5 on toluene reforming was investigated through a vertical furnace. Gases produced by tar catalysis were evaluated through GC analysis. The physicochemical structure, properties and catalytic performance of the catalyst were also tested. TG analysis was used to assess the accumulation and oxidation reactivity of carbon on the catalyst surface. An analysis was conducted on the mechanism of carbon deposition during catalyst deactivation in tar catalysis. The results showed that the 9Ni/91ZSM-5 had a superior toluene conversion of 60.49%, but also experienced rapid and substantial carbon deposition up to 52.69%. Carbon is mainly deposited as curved filaments on both the surface and pore channels of the catalyst. In some cases, tip growth occurs where both carbon deposition and Ni coexist. Furthermore, specific surface area and micropore volume are reduced to varying degrees due to carbon deposition. With the time increased, the amount of carbon deposited on the catalyst surface increased to 62.81%, which gradually approached saturation, and the overall performance of the catalyst was stabilized. This situation causes toluene molecules to detach from the active sites within the catalyst, hindering gas release, which leads to reduced catalytic activity and further carbon deposition. It provides both a basis for the development of new catalysts and an economically feasible solution for practical tar reduction and removal.


Assuntos
Nanotubos de Carbono , Níquel , Catálise , Nanotubos de Carbono/química , Níquel/química , Alcatrões/química , Carbono/química , Tolueno/química , Oxirredução
16.
J Environ Manage ; 362: 121333, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38833925

RESUMO

The unregulated release of chemical dyes into the environment presents considerable environmental hazards when left untreated. Photocatalytic degradation, acknowledged as an eco-friendly and cost-effective method, has garnered attention for its efficacy in eliminating organic pollutants like dye. Consequently, the development of multifunctional materials with different applications in environmental and catalytic fields emerges as a promising avenue. Recognizing the significance of integrating catalysts and porous materials for enhancing interactions between pollutants and photo-sensitive substances, magnetic hydrochar emerges as a solution offering heightened efficiency, scalability, recyclability, and broad applicability in various environmental processes, notably wastewater treatment, due to its facile separation capability. In this study, Fe3O4-based, super-paramagnetic hydrochar (SMHC) was simultaneously synthesized in a single step using a coconut shell in the subcritical water medium. A thorough analysis was conducted on both raw hydrochar (RHC) and SMHC to unravel the mechanism of interaction between Fe3O4 nanoparticles and the hydrochar matrix. The synthesized hydrochar exhibited super-paramagnetic characteristics, with a saturation magnetization of 23.7 emu/g and a magnetic hysteresis loop. SMHC displayed a BET surface area of 42.6 m2/g and an average pore size of 26.3 nm, indicating a mesoporous structure according to nitrogen adsorption-desorption isotherms. XRD analysis revealed magnetic crystal sizes in the obtained SMHC to be 13.7 nm. The photocatalytic performance of SMHC was evaluated under visible light exposure in the presence of H2O2 for Astrazon yellow (AY) dye degradation, with optimization conducted using response surface methodology (RSM). The most substantial dye removal, reaching 92.83%, was achieved with 0.4% H2O2 at a 20 mg/L dye concentration and an 80-min reaction duration.


Assuntos
Poluentes Químicos da Água , Catálise , Poluentes Químicos da Água/química , Corantes/química , Água/química , Adsorção
17.
J Environ Manage ; 362: 121331, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38833931

RESUMO

This study introduces an innovative LED-IoT photoreactor, representing a significant advancement in response to the demand for sustainable water purification. The integration of LED-IoT installations addresses the challenge of intermittent sunlight availability, employing LEDs with a spectrum mimicking natural sunlight. Passive Infra-Red (PIR) sensors and Internet of things (IoT) technology ensure consistent radiation intensity, with the LED deactivating in ample sunlight and activating in its absence. Utilizing a visible light-absorbing photocatalyst developed through sol-gel synthesis and mild-temperature calcination, this research demonstrates a remarkable carbamazepine removal efficiency exceeding 95% under LED-IoT system illumination, compared to less than 90% efficiency with sunlight alone, within a 6-h exposure period. Moreover, the designed photocatalytic system achieves over 60% mineralization of carbamazepine after 12 h. Notably, the photocatalyst demonstrated excellent stability with no performance loss during five further cycles. Furthermore, integration with renewable energy sources facilitated continuous operation beyond daylight hours, enhancing the system's applicability in real-world water treatment scenarios. A notable application of the LED-IoT system at an operating sewage treatment plant showed nearly 80% efficiency in carbamazepine removal from sewage in the secondary settling tank after 6 h of irradiation, coupled with nearly 40% mineralization efficiency. Additionally, physicochemical analyses such as XPS and STA-FTIR confirm that the carbamazepine photooxidation process does not affect the surface of the photocatalyst, showing no adsorption for degradation products.


Assuntos
Carbamazepina , Energia Solar , Poluentes Químicos da Água , Purificação da Água , Carbamazepina/química , Carbamazepina/isolamento & purificação , Purificação da Água/métodos , Poluentes Químicos da Água/química , Luz Solar , Eliminação de Resíduos Líquidos/métodos , Catálise
18.
Environ Sci Technol ; 58(23): 10388-10397, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38828512

RESUMO

Selective catalytic reduction of nitrogen oxides (NOx) with ammonia (NH3-SCR) is an efficient NOx reduction strategy, while the denitrification (deNOx) catalysts suffer from serious deactivation due to the coexistence of multiple poisoning substances, such as alkali metal (e.g., K), SO2, etc., in industrial flue gases. It is essential to understand the interaction among various poisons and their effects on the deNOx process. Herein, the ZSM-5 zeolite-confined MnSmOx mixed (MnSmOx@ZSM-5) catalyst exhibited better deNOx performance after the poisoning of K, SO2, and/or K&SO2 than the MnSmOx and MnSmOx/ZSM-5 catalysts, the deNOx activity of which at high temperature (H-T) increased significantly (>90% NOx conversion in the range of 220-480 °C). It has been demonstrated that K would occupy both redox and acidic sites, which severely reduced the reactivity of MnSmOx/ZSM-5 catalysts. The most important, K element is preferentially deposited at -OH on the surface of ZSM-5 carrier due to the electrostatic attraction (-O-K). As for the K&SO2 poisoning catalyst, SO2 preferred to be combined with the surface-deposited K (-O-K-SO2ads) according to XPS and density functional theory (DFT) results, the poisoned active sites by K would be released. The K migration behavior was induced by SO2 over K-poisoned MnSmOx@ZSM-5 catalysts, and the balance of surface redox and acidic site was regulated, like a synergistic promoter, which led to K-poisoning buffering and activity recovery. This work contributes to the understanding of the self-detoxification interaction between alkali metals (e.g., K) and SO2 on deNOx catalysts and provides a novel strategy for the adaptive use of one poisoning substance to counter another for practical NOx reduction.


Assuntos
Zeolitas , Zeolitas/química , Catálise , Oxirredução , Óxidos de Nitrogênio/química , Óxidos/química , Amônia/química , Desnitrificação , Metais/química
19.
Water Sci Technol ; 89(10): 2783-2795, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38822614

RESUMO

Photocatalytically active ceramic flat sheet membranes based on a nanostructured titanium dioxide (TiO2) coating were produced for photocatalytic water treatment. The nano-TiO2 layer was produced by a novel combination of magnetron sputtering of a thin titanium layer on silicon carbide (SiC) membranes, followed by electrochemical oxidation (anodization) and subsequent heat treatment (HT). Characterization by Raman spectra and field emission scanning electron microscopy proved the presence of a nanostructured anatase layer on the membranes. The influence of the titanium layer thickness on the TiO2 formation process and the photocatalytic properties were investigated using anodization curves, by using cyclovoltammetry measurements, and by quantifying the generated hydroxyl radicals (OH•) under UV-A irradiation in water. Promising photocatalytic activity and permeability of the nano-TiO2-coated membranes could be demonstrated. A titanium layer of at least 2 µm was necessary for significant photocatalytic effects. The membrane sample with a 10 µm Ti/TiO2 layer had the highest photocatalytic activity showing a formation rate of 1.26 × 10-6 mmol OH• s-1. Furthermore, the membranes were tested several times, and a decrease in radical formation was observed. Assuming that these can be attributed to adsorption processes of the reactants, initial experiments were carried out to reactivate the photocatalyzer.


Assuntos
Compostos Inorgânicos de Carbono , Radical Hidroxila , Membranas Artificiais , Compostos de Silício , Titânio , Purificação da Água , Titânio/química , Radical Hidroxila/química , Purificação da Água/métodos , Catálise , Compostos de Silício/química , Compostos Inorgânicos de Carbono/química , Técnicas Eletroquímicas , Nanoestruturas/química , Processos Fotoquímicos
20.
Mikrochim Acta ; 191(7): 365, 2024 06 04.
Artigo em Inglês | MEDLINE | ID: mdl-38831060

RESUMO

Copper-cobalt bimetallic nitrogen-doped carbon-based nanoenzymatic materials (CuCo@NC) were synthesized using a one-step pyrolysis process. A three-channel colorimetric sensor array was constructed for the detection of seven antioxidants, including cysteine (Cys), uric acid (UA), tea polyphenols (TP), lysine (Lys), ascorbic acid (AA), glutathione (GSH), and dopamine (DA). CuCo@NC with peroxidase activity was used to catalyze the oxidation of TMB by H2O2 at three different ratios of metal sites. The ability of various antioxidants to reduce the oxidation products of TMB (ox TMB) varied, leading to distinct absorbance changes. Linear discriminant analysis (LDA) results showed that the sensor array was capable of detecting seven antioxidants in buffer and serum samples. It could successfully discriminate antioxidants with a minimum concentration of 10 nM. Thus, multifunctional sensor arrays based on CuCo@NC bimetallic nanoenzymes not only offer a promising strategy for identifying various antioxidants but also expand their applications in medical diagnostics and environmental analysis of food.


Assuntos
Antioxidantes , Carbono , Colorimetria , Cobre , Nitrogênio , Nitrogênio/química , Colorimetria/métodos , Carbono/química , Antioxidantes/química , Antioxidantes/análise , Cobre/química , Cobalto/química , Peróxido de Hidrogênio/química , Humanos , Catálise , Limite de Detecção , Glutationa/química , Glutationa/sangue , Dopamina/sangue , Dopamina/análise , Dopamina/química , Benzidinas/química , Polifenóis/química , Polifenóis/análise , Ácido Ascórbico/química , Ácido Ascórbico/sangue , Ácido Ascórbico/análise , Oxirredução , Ácido Úrico/sangue , Ácido Úrico/química , Ácido Úrico/análise , Cisteína/química , Cisteína/sangue
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