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1.
Mikrochim Acta ; 191(8): 441, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38954045

RESUMO

A ratiometric SERS aptasensor based on catalytic hairpin self-assembly (CHA) mediated cyclic signal amplification strategy was developed for the rapid and reliable determination of Escherichia coli O157:H7. The recognition probe was synthesized by modifying magnetic beads with blocked aptamers, and the SERS probe was constructed by functionalizing gold nanoparticles (Au NPs) with hairpin structured DNA and 4-mercaptobenzonitrile (4-MBN). The recognition probe captured E. coli O157:H7 specifically and released the blocker DNA, which activated the CHA reaction on the SERS probe and turned on the SERS signal of 6-carboxyl-x-rhodamine (ROX). Meanwhile, 4-MBN was used as an internal reference to calibrate the matrix interference. Thus, sensitive and reliable determination and quantification of E. coli O157:H7 was established using the ratio of the SERS signal intensities of ROX to 4-MBN. This aptasensor enabled detection of 2.44 × 102 CFU/mL of E. coli O157:H7 in approximately 3 h without pre-culture and DNA extraction. In addition, good reliability and excellent reproducibility were observed for the determination of E. coli O157:H7 in spiked water and milk samples. This study offered a new solution for the design of rapid, sensitive, and reliable SERS aptasensors.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Escherichia coli O157 , Ouro , Limite de Detecção , Nanopartículas Metálicas , Leite , Análise Espectral Raman , Escherichia coli O157/isolamento & purificação , Aptâmeros de Nucleotídeos/química , Nanopartículas Metálicas/química , Ouro/química , Leite/microbiologia , Leite/química , Análise Espectral Raman/métodos , Técnicas Biossensoriais/métodos , Animais , Catálise , Sequências Repetidas Invertidas , Contaminação de Alimentos/análise , Microbiologia da Água , Reprodutibilidade dos Testes
2.
Environ Geochem Health ; 46(8): 266, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38954124

RESUMO

Recently, the hazardous effects of antibiotic micropollutants on the environment and human health have become a major concern. To address this challenge, semiconductor-based photocatalysis has emerged as a promising solution for environmental remediation. Our study has developed Bi2WO6/g-C3N4 (BWCN) photocatalyst with unique characteristics such as reactive surface sites, enhanced charge transfer efficiency, and accelerated separation of photogenerated electron-hole pairs. BWCN was utilized for the oxidation of tetracycline antibiotic (TCA) in different water sources. It displayed remarkable TCA removal efficiencies in the following order: surface water (99.8%) > sewage water (88.2%) > hospital water (80.7%). Further, reusability tests demonstrated sustained performance of BWCN after three cycles with removal efficiencies of 87.3, 71.2 and 65.9% in surface water, sewage, and hospital water, respectively. A proposed photocatalytic mechanism was delineated, focusing on the interaction between reactive radicals and TCA molecules. Besides, the transformation products generated during the photodegradation of TCA were determined, along with the discussion on the potential risk assessment of antibiotic pollutants. This study introduces an approach for utilizing BWCN photocatalyst, with promising applications in the treatment of TCA from various wastewater sources.


Assuntos
Antibacterianos , Oxirredução , Tetraciclina , Poluentes Químicos da Água , Poluentes Químicos da Água/química , Antibacterianos/química , Tetraciclina/química , Catálise , Águas Residuárias/química , Bismuto/química , Grafite/química , Compostos de Nitrogênio/química , Compostos de Tungstênio/química , Fotólise , Purificação da Água/métodos , Esgotos/química
3.
Mikrochim Acta ; 191(7): 438, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38951285

RESUMO

A dual-recognition strategy is reported to construct a one-step washing and highly efficient signal-transduction tag system for high-sensitivity colorimetric detection of Staphylococcus aureus (S. aureus). The porous (gold core)@(platinum shell) nanozymes (Au@PtNEs) as the signal labels show highly efficient peroxidase mimetic activity and are robust. For the sake of simplicity the detection involved the use of a vancomycin-immobilized magnetic bead (MB) and aptamer-functionalized Au@PtNEs for dual-recognition detection in the presence of S. aureus. In addition, we designed a magnetic plate to fit the 96-well microplate to ensure consistent magnetic properties of each well, which can quickly remove unreacted Au@PtNEs and sample matrix while avoiding tedious washing steps. Subsequently, Au@PtNEs catalyze hydrogen peroxide (H2O2) to oxidize 3,3',5,5'-tetramethylbenzidine (TMB) generating a color signal. Finally, the developed Au@PtNEs-based dual-recognition washing-free colorimetric assay displayed a response in the range of S. aureus of 5 × 101-5 × 105 CFU/mL, and the detection limit was 40 CFU/mL within 1.5 h. In addition, S. aureus-fortified samples were analyzed to further evaluate the performance of the proposed method, which yielded average recoveries ranging from 93.66 to 112.44% and coefficients of variation (CVs) within the range 2.72-9.01%. These results furnish a novel horizon for the exploitation of a different mode of recognition and inexpensive enzyme-free assay platforms as an alternative to traditional enzyme-based immunoassays for the detection of other Gram-positive pathogenic bacteria.


Assuntos
Benzidinas , Colorimetria , Ouro , Peróxido de Hidrogênio , Limite de Detecção , Platina , Staphylococcus aureus , Staphylococcus aureus/isolamento & purificação , Colorimetria/métodos , Ouro/química , Platina/química , Porosidade , Benzidinas/química , Peróxido de Hidrogênio/química , Aptâmeros de Nucleotídeos/química , Nanopartículas Metálicas/química , Vancomicina/química , Técnicas Biossensoriais/métodos , Catálise , Humanos
4.
Environ Sci Technol ; 58(26): 11843-11854, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38952299

RESUMO

Advanced oxidation processes (AOPs) are the most efficient water cleaning technologies, but their applications face critical challenges in terms of mass/electron transfer limitations and catalyst loss/deactivation. Bipolar electrochemistry (BPE) is a wireless technique that is promising for energy and environmental applications. However, the synergy between AOPs and BPE has not been explored. In this study, by combining BPE with AOPs, we develop a general approach of using carbon nanotubes (CNTs) as electric-field-induced bipolar electrodes to control electron transfer for efficient water purification. This approach can be used for permanganate and peroxide activation, with superior performances in the degradation of refractory organic pollutants and excellent durability in recycling and scale-up experiments. Theoretical calculations, in situ measurements, and physical experiments showed that an electric field could substantially reduce the energy barrier of electron transfer over CNTs and induce them to produce bipolar electrodes via electrochemical polarization or to form monopolar electrodes through a single particle collision effect with feeding electrodes. This approach can continuously provide activated electrons from one pole of bipolar electrodes and simultaneously achieve "self-cleaning" of catalysts through CNT-mediated direct oxidation from another pole of bipolar electrodes. This study provides a fundamental scientific understanding of BPE, expands its scope in the environmental field, and offers a general methodology for water purification.


Assuntos
Eletrodos , Nanotubos de Carbono , Oxirredução , Purificação da Água , Nanotubos de Carbono/química , Purificação da Água/métodos , Catálise
5.
Environ Geochem Health ; 46(7): 250, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38877278

RESUMO

The release of industrial wastewater has adverse effects on both aquatic ecosystems and the environment. Discharging untreated organic dyes into aquatic environments significantly amplifies pollution levels in these ecosystems. Ensuring the appropriate disposal of organic colorants and their derivatives before introducing them into wastewater streams is essential to prevent environmental contamination. This study aimed to develop an eco-friendly and sustainable approach to synthesize a chitosan-functionalized silver (Ag) nanocomposite using Solanum trilobatum for color pollutant mitigation. The synthesized CS-Ag nanocomposite was analyzed using various techniques such as UV-visible, FTIR, TEM, and EDS. TEM analysis revealed that the CS-Ag nanocomposite had a spherical nanostructure, with diameters ranging from 17.4 to 43.9 nm. These nanocomposites were tested under visible light irradiation to analyze their photocatalytic character against Congo red (CR). The nanocomposite exhibited a remarkable dye removal efficiency of over 93.6% within 105 min under irradiation. In the experimental recycling study, the CS-Ag nanocomposites demonstrated remarkable stability and reusability. Furthermore, the CS-Ag nanocomposite exhibited promising inhibition activity against bacterial pathogens. Our research revealed that the synthesized nanocomposite has the potential to act as a highly effective photocatalyst and bactericidal agent in various industrial and clinical applications.


Assuntos
Antibacterianos , Quitosana , Corantes , Nanocompostos , Prata , Poluentes Químicos da Água , Quitosana/química , Nanocompostos/química , Prata/química , Antibacterianos/farmacologia , Antibacterianos/química , Corantes/química , Poluentes Químicos da Água/química , Catálise , Vermelho Congo/química , Recuperação e Remediação Ambiental/métodos , Águas Residuárias/química , Luz
6.
Water Sci Technol ; 89(11): 3047-3078, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38877630

RESUMO

Graphitic carbon nitride (g-C3N4) is a widely studied visible-light-active photocatalyst for low cost, non-toxicity, and facile synthesis. Nonetheless, its photocatalytic efficiency is below par, due to fast recombination of charge carriers, low surface area, and insufficient visible light absorption. Thus, the research on the modification of g-C3N4 targeting at enhanced photocatalytic performance has attracted extensive interest. A considerable amount of review articles have been published on the modification of g-C3N4 for applications. However, limited effort has been specially contributed to providing an overview and comparison on available modification strategies for improved photocatalytic activity of g-C3N4-based catalysts in antibiotics removal. There has been no attempt on the comparison of photocatalytic performances in antibiotics removal between modified g-C3N4 and other known catalysts. To address these, our study reviewed strategies that have been reported to modify g-C3N4, including metal/non-metal doping, defect tuning, structural engineering, heterostructure formation, etc. as well as compared their performances for antibiotics removal. The heterostructure formation was the most widely studied and promising route to modify g-C3N4 with superior activity. As compared to other known photocatalysts, the heterojunction g-C3N4 showed competitive performances in degradation of selected antibiotics. Related mechanisms were discussed, and finally, we revealed current challenges in practical application.


Assuntos
Antibacterianos , Grafite , Luz , Compostos de Nitrogênio , Poluentes Químicos da Água , Antibacterianos/química , Grafite/química , Catálise , Compostos de Nitrogênio/química , Poluentes Químicos da Água/química , Fotólise , Processos Fotoquímicos , Nitrilas
7.
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
8.
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
9.
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
10.
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
11.
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
12.
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
13.
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
14.
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
15.
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
16.
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
17.
Chem Biol Drug Des ; 103(6): e14555, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38862260

RESUMO

Click chemistry is widely used for the efficient synthesis of 1,4-disubstituted-1,2,3-triazole, a well-known scaffold with widespread biological activity in the pharmaceutical sciences. In recent years, this magic ring has attracted the attention of scientists for its potential in designing and synthesizing new antifungal agents. Despite scientific and medical advances, fungal infections still account for more than 1.5 million deaths globally per year, especially in people with compromised immune function. This increasing trend is definitely related to a raise in the incidence of fungal infections and prevalence of antifungal drug resistance. In this condition, an urgent need for new alternative antifungals is undeniable. By focusing on the main aspects of reaction conditions in click chemistry, this review was conducted to classify antifungal 1,4-disubstituted-1,2,3-triazole hybrids based on their chemical structures and introduce the most effective triazole antifungal derivatives. It was notable that in all reactions studied, Cu(I) catalysts generated in situ by the reduction in Cu(II) salts or used copper(I) salts directly, as well as mixed solvents of t-BuOH/H2O and DMF/H2O had most application in the synthesis of triazole ring. The most effective antifungal activity was also observed in fluconazole analogs containing 1,2,3-triazole moiety and benzo-fused five/six-membered heterocyclic conjugates with a 1,2,3-triazole ring, even with better activity than fluconazole. The findings of structure-activity relationship and molecular docking of antifungal derivatives synthesized with copper-catalyzed azide-alkyne cycloaddition (CuAAC) could offer medicinal chemistry scientists valuable data on designing and synthesizing novel triazole antifungals with more potent biological activities in their future research.


Assuntos
Antifúngicos , Química Click , Reação de Cicloadição , Triazóis , Antifúngicos/farmacologia , Antifúngicos/síntese química , Antifúngicos/química , Catálise , Triazóis/química , Triazóis/farmacologia , Triazóis/síntese química , Química Verde , Cobre/química , Humanos
18.
Int J Biol Macromol ; 272(Pt 1): 132922, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38844292

RESUMO

Converting lignin into specific aromatic chemicals for utilization through depolymerization of lignin is an effective way to achieve high-value applications. There are many depolymerization methods that can do this, but there are problems such as harsh reaction conditions, low depolymerization efficiency and uncontrollable target products that need to be solved. This study reports a novel system for the oxidative depolymerization of alkali lignin using Fe- and Mn- modified TS-1 as a catalyst to assist in the highly selective production of vanillin. We also proposed a possible reaction pathway for the oxidative depolymerization of alkali lignin to produce vanillin catalyzed by Fe-Mn/TS-1 catalyst. The catalytic effects of TS-1, Fe/TS-1, and Fe-Mn/TS-1 catalysts on the oxidative depolymerization of lignin to produce phenolic monomers and vanillin were investigated. The results show that the modified catalysts can effectively improve the efficiency of linkage bond breaking in lignin, especially the ß-O-4 bond, in which the inter-band transitions of Fe and Mn play an important role. The synergistic effect of the bimetallic-loaded catalyst (Fe-Mn/TS-1) could catalyze the oxidative depolymerization of lignin more efficiently than the monometallic-loaded catalyst (Fe/TS-1). This lignin oxidative depolymerization system produced 40.59 wt% bio-oil including 12.24 wt% phenolic monomers and 16.17 wt% re-lignin after the addition of Fe-Mn/TS-1 catalyst, owning the highest phenolic monomer yield. Surprisingly, this lignin oxidative depolymerization system exhibited high yield for vanillin (8.36 wt%) production. These results demonstrated that the Fe-Mn/TS-1 catalytic system has potential to produce vanillin from lignin under mild conditions.


Assuntos
Benzaldeídos , Ferro , Lignina , Manganês , Oxirredução , Polimerização , Zeolitas , Lignina/química , Benzaldeídos/química , Manganês/química , Catálise , Ferro/química , Zeolitas/química
19.
Carbohydr Res ; 541: 109167, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38823063

RESUMO

This paper describes a mild and efficient catalytic deprotection method for isopropylidene ketals and benzylidene acetals using AcOH/H2O/DME(1,2-Dimethoxyethane). The method effectively removes ketal and acetal protecting groups from 2-deoxyglycosides which are prone to hydrolysis under acidic conditions. Moreover, it enables the selective removal of the terminal ketal over an internal one.


Assuntos
Glicosídeos , Glicosídeos/química , Glicosídeos/síntese química , Água/química , Estereoisomerismo , Cetonas/química , Catálise , Acetais/química , Estrutura Molecular
20.
Org Lett ; 26(23): 4958-4962, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38833318

RESUMO

Inspired by previous selection outcomes, we investigated and developed a rhodium-promoted C-H activation/annulation reaction of DNA-linked terminal alkynes and aromatic acids. This reaction exhibits excellent efficiency with high conversions and a broad substrate scope. Most importantly, the unique DEL-compatible conditions provide a better scenario for yielding an isocoumarin scaffold compared to conventional organic reaction conditions, and this newly developed on-DNA method has confirmed its feasibility in preparing DNA-encoded libraries.


Assuntos
Alcinos , DNA , Ródio , Ródio/química , Alcinos/química , Estrutura Molecular , DNA/química , Catálise , Isocumarinas/química , Isocumarinas/síntese química
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