The rapid acceleration of industrialization and urbanization has exacerbated water pollution, which is primarily caused by the presence of highly toxic, non-biodegradable contaminants in industrial waste and effluents. In response to this urgent issue, a novel nanobiocomposite film with titanium dioxide (TiO2) loaded onto a poly(3-hydroxybutyrate-co-18 mol% 3-hydroxyhexanoate) (18PHBH) matrix was developed to serve as an effective dual-function material with photocatalytic and antibacterial properties. Through Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR), Diffuse reflectance ultraviolet-visible (DRUV-Vis), Scanning Electron Microscope (SEM), and X-ray diffraction (XRD) analyses, the physicochemical properties of the TiO2/Gly/18PHBH nanobiocomposite film were exhaustively characterized, revealing effective TiO2 loading and uniform distribution on the film's surface. The film exhibited extraordinary photocatalytic degradation of methylene blue (MB) dye, with the 5TiO2/Gly/18PHBH film demonstrating the greatest efficiency. In addition, antibacterial testing revealed that the film was effective against 99.8 % of Staphylococcus aureus and 96.9 % of Pseudomonas aeruginosa. These results demonstrate the potential of polyhydroxyalkanoate-based films as exceptional nanoparticle matrices and position the 5TiO2/Gly/18PHBH film as a versatile candidate for applications in photocatalysis and antibacterial interventions, providing innovative solutions to critical environmental challenges.
One of the most crucial attributes of synthetic organic chemistry is to design organic reactions under the facets of green chemistry for the sustainable production of chemicals. Thus, due to the intensified environmental and safety concern, the need for new technologies for conducting chemical transformation has grown. In this regard, there is enormous interest in the use of heterogeneous catalysts as they generally avoid the generation of waste, require fewer toxic reagents, as well as entail easier separation and recycling of the catalyst. α,β-Unsaturated acids have been widely used in various industrial applications and have been identified as one of the most promising chemicals obtained via the Knoevenagel condensation reaction. This review aims to discuss the most pertinent heterogeneous catalytic systems such as zeolites, mesoporous silica, ionic liquids, metal oxides, and graphitic carbon nitride-based catalysts in the Knoevenagel reaction. Ultimately, this review focuses not only on the catalyst but also provides an overall idea and guide for the preparation of new catalysts with outstanding properties by looking at the chemical and engineering aspects such as the reaction conditions and the mechanisms.
Recent foodborne outbreaks in multiple locations necessitate the continuous development of highly sensitive and specific biosensors that offer rapid detection of foodborne biological hazards. This work focuses on the development of a reduced graphene oxide‑titanium dioxide (rGO-TiO2) nanocomposite based aptasensor to detect Salmonella enterica serovar Typhimurium. A label-free aptamer was immobilized on a rGO-TiO2 nanocomposite matrix through electrostatic interactions. The changes in electrical conductivity on the electrode surface were evaluated using electroanalytical methods. DNA aptamer adsorbed on the rGO-TiO2 surface bound to the bacterial cells at the electrode interface causing a physical barrier inhibiting the electron transfer. This interaction decreased the DPV signal of the electrode proportional to decreasing concentrations of the bacterial cells. The optimized aptasensor exhibited high sensitivity with a wide detection range (108 to 101 cfu mL-1), a low detection limit of 101 cfu mL-1 and good selectivity for Salmonella bacteria. This rGO-TiO2 aptasensor is an excellent biosensing platform that offers a reliable, rapid and sensitive alternative for foodborne pathogen detection.
Correction for 'A review of the recent progress on heterogeneous catalysts for Knoevenagel condensation' by Jimmy Nelson Appaturi et al., Dalton Trans., 2021, 50, 4445-4469, DOI: 10.1039/d1dt00456e.
The Prins cyclization of styrene (SE) with paraformaldehyde (PFCHO) was conducted with mesoporous ZnAlMCM-41 catalysts for the synthesis of 4-phenyl-1,3-dioxane (4-PDO) using a liquid phase heterogeneous catalytic method. For a comparison study, the Prins cyclization reaction was also conducted over different nanoporous catalysts, e.g. mesoporous solid acid catalysts, AlMCM-41(21) and ZnMCM-41(21), and microporous catalysts, USY, Hβ, HZSM-5, and H-mordenite. The recyclable mesoporous ZnAlMCM-41 catalysts were reused in this reaction to evaluate their catalytic stabilities. Since ZnAlMCM-41(75) has higher catalytic activity than other solid acid catalysts, washed ZnAlMCM-41(75)/W-ZnAlMCM-41(75) was prepared using an efficient chemical treatment method and used with various reaction parameters to find an optimal parameter for the highly selective synthesis of 4-PDO. W-ZnAlMCM-41(75) was also used in the Prins cyclization of olefins with PFCHO and formalin (FN, 37% aqueous solution of formaldehyde (FCHO)) under different reaction conditions to obtain 1,3-dioxanes, which are widely used as solvents or intermediates in organic synthesis. Based on the nature of catalysts used under different reaction conditions, a reasonable plausible reaction mechanism for the Prins cyclization of SE with PFCHO is proposed. Notably, it can be seen from the catalytic results of all catalysts that the W-ZnAlMCM-41(75) catalyst has higher 4-PDO selectivity with exceptional catalytic activity than other microporous and mesoporous catalysts.
Recent advances in the field of nanotechnology contributed to the increasing use of nanomaterials in the engineering, health and biological sectors. Graphene oxide (GO) has great potentials as it could be fine-tuned to be adapted into various applications, especially in the electrical, electronic, industrial and clinical fields. One of the important applications of GO is its use as an antibacterial material due to its promising activity against a broad range of bacteria. However, our understanding of the mechanism of action of GO towards bacteria is still lacking and is often less described. Therefore, a comprehensive overview of bactericidal mechanistic actions of GO and the roles of physicochemical factors including size, aggregation, functionalization and adsorption behavior contributing to its antibacterial activities are described in this review. As the use of GO is expected to increase exponentially in the health sector, the cytotoxicity of GO among the cell lines is also discussed. Thus, this review emphasizes the physicochemical characteristics of GO that can be tailored for optimal antibacterial properties that is of importance to the health industry.
Brain-eating amoebae (Acanthamoeba spp., Balamuthia mandrillaris, Naegleria fowleri) have gained increasing attention owing to their capacity to produce severe human and animal infections involving the brain. Early detection is a pre-requisite in successful prognosis. Here, we developed a nanoPCR assay for the rapid detection of brain-eating amoebae using various nanoparticles. Graphene oxide, copper and alumina nanoparticles used in this study were characterized using Raman spectroscopy measurements through excitation with a He-Ne laser, while powder X-ray diffraction patterns were taken on a PANanalytical, X'Pert HighScore diffractometer and the morphology of the materials was confirmed using high-resolution transmission electron microscopy (HRTEM). Using nanoparticle-assisted PCR, the results revealed that graphene oxide, copper oxide and alumina nanoparticles significantly enhanced PCR efficiency in the detection of pathogenic free-living amoebae using genus-specific probes. The optimal concentration of graphene oxide, copper oxide and alumina nanoparticles for Acanthamoeba spp. was determined at 0.4, 0.04 and 0.4 μg per mL respectively. For B. mandrillaris, the optimal concentration was determined at 0.4 μg per mL for graphene oxide, copper oxide and alumina nanoparticles, and for Naegleria, the optimal concentration was 0.04, 4.0 and 0.04 μg per mL respectively. Moreover, combinations of these nanoparticles proved to further enhance PCR efficiency. The addition of metal oxide nanoparticles leads to excellent surface effect, while thermal conductivity property of the nanoparticles enhances PCR productivity. These findings suggest that nanoPCR assay has tremendous potential in the clinical diagnosis of parasitic infections as well as for studying epidemiology and pathology and environmental monitoring of other microbes.
Graphene oxide (GO) has displayed antibacterial activity that has been investigated in the past, however, information on synergistic activity of GO with conventional antibiotics is still lacking. The objectives of the study were to determine the combinatorial actions of GO and antibiotics against Gram-positive and Gram-negative bacteria and the toxicological effects of GO towards human epidermal keratinocytes (HaCaT). Interactions at molecular level between GO and antibiotics were analyzed using Attenuated Total Reflectance-Fourier-transform infrared spectroscopy (ATR-FTIR). Changes in the antibacterial activity of antibiotics towards bacteria through the addition of GO was investigated. Toxicity of GO towards HaCaT cells were examined as skin cells play a role as the first line of defense of the human body. The ATR-FTIR characterizations of GO and antibiotics showed adsorption of tested antibiotics onto GO. The combinatorial antibacterial activity of GO and antibiotics were found to increase when compared to GO or antibiotic alone. This was attributed to the ability of GO to disrupt bacterial membrane to allow for better adsorption of antibiotics. Cytotoxicity of GO was found to be dose-dependent towards HaCaT cell line, it is found to impose negligible toxic effects against the skin cells at concentration below 100 μg/mL.
Rapid detection of foodborne pathogens is crucial as ingestion of contaminated food products may endanger human health. Thus, the objective of this study was to develop a biosensor using reduced graphene oxide-carbon nanotubes (rGO-CNT) nanocomposite via the hydrothermal method for accurate and rapid label-free electrochemical detection of pathogenic bacteria such as Salmonella enterica. The rGO-CNT nanocomposite was characterized using Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray diffraction and transmission electron microscopy. The nanocomposite was dropped cast on the glassy carbon electrode and further modified with amino-modified DNA aptamer. The resultant ssDNA/rGO-CNT/GCE aptasensor was then used to detect bacteria by using differential pulse voltammetry (DPV) technique. Synergistic effects of aptasensor was evident through the combination of enhanced electrical properties and facile chemical functionality of both rGO and CNT for the stable interface. Under optimal experimental conditions, the aptasensor could detect S. Typhimurium in a wide linear dynamic range from 101 until 108 cfu mL-1 with a 101 cfu mL-1 of the limit of detection. This aptasensor also showed good sensitivity, selectivity and specificity for the detection of microorganisms. Furthermore, we have successfully applied the aptasensor for S. Typhimurium detection in real food samples.
The antibacterial nature of graphene oxide (GO) has stimulated wide interest in the medical field. Although the antibacterial activity of GO towards bacteria has been well studied, a deeper understanding of the mechanism of action of GO is still lacking. The objective of the study was to elucidate the difference in the interactions of GO towards Gram-positive and Gram-negative bacteria. The synthesized GO was characterized by Ultraviolet-visible spectroscopy (UV-vis), Raman and Attenuated Total Reflectance-Fourier-transform infrared spectroscopy (ATR-FTIR). Viability, time-kill and Lactose Dehydrogenase (LDH) release assays were carried out along with FESEM, TEM and ATR-FTIR analysis of GO treated bacterial cells. Characterizations of synthesized GO confirmed the transition of graphene to GO and the antibacterial activity of GO was concentration and time-dependent. Loss of membrane integrity in bacteria was enhanced with increasing GO concentrations and this corresponded to the elevated release of LDH in the reaction medium. Surface morphology of GO treated bacterial culture showed apparent differences in the mechanism of action of GO towards Gram-positive and Gram-negative bacteria where cell entrapment was mainly observed for Gram-positive Staphylococcus aureus and Enterococcus faecalis whereas membrane disruption due to physical contact was noted for Gram-negative Escherichia coli and Pseudomonas aeruginosa. ATR-FTIR characterizations of the GO treated bacterial cells showed changes in the fatty acids, amide I and amide II of proteins, peptides and amino acid regions compared to untreated bacterial cells. Therefore, the data generated further enhance our understanding of the antibacterial activity of GO towards bacteria.
A sustainable method was used to produce aromatic ketones by the solvent-free benzylic oxidation of aromatics over mesoporous Cu(II)-containing propylsalicylaldimine anchored on the surface of Santa Barbara Amorphous type material-15 (CPSA-SBA-15) catalysts. For comparison, mesoporous Cu(II)-containing propylsalicylaldimine anchored with Mobil Composition of Matter-41 (CPSA-MCM-41) was assessed for these reactions under similar reaction conditions. The washed CPSA-SBA-15(0.2) (W-CPSA-SBA-15(0.2)) catalyst was prepared using an easy chemical method for the complete removal of non-framework CuO nanoparticle species on the surface of pristine CPSA-SBA-15(0.2) (p-CPSA-SBA-15(0.2) prepared with 0.2 wt% of Cu, and its catalytic activity was evaluated with different reaction parameters, oxidants and solvents. In order to confirm the catalytic stability, the recyclability was assessed, and the performance of hot-filtration experiments was also evaluated. All the catalysts used for these catalytic reactions were characterized using many instrumental techniques to pinpoint the mesoporous nature and active sites of the catalysts. The proposed reaction mechanism has been well documented on the basis of catalytic results obtained for solvent-free oxidation of aromatics. Based on the catalytic results, we found that W-CPSA-SBA-15(0.2) is a very ecofriendly catalyst with exceptional catalytic activity.
The most common material used for blood bags is PVC, which requires the addition of DEHP to increase its flexibility. DEHP is known to cross the polymer barrier and move into the stored blood and, ultimately, the patient's bloodstream. In this work, an alternative prototype composed of SEBS/PP was fabricated through blow-moulding and compared with the commercially available PVC-based blood bag which was designated as the control. The blow-moulded sample layers were welded together using CO2 lasers and optimized to obtain complete sealing of the sides. The samples' performance characteristics were analyzed using water permeability, oxygen permeability, shelf-life, and bioburden tests. The SEBS/PP sample exhibited the highest oxygen permeability rate of 1486.6 cc/m2/24 h after 40 days of ageing, indicating that the sample is conducive for red blood cell (RBC) respiration. On the other hand, the SEBS/PP sample showcased a lower water permeability rate of 0.098 g/h m2 after 40 days of aging, indicating a high-water barrier property and thus preventing water loss during storage. In comparison, the oxygen and water permeability rates of PVC-DEHP were found to be distinctly lower in performance (662.7 cc/m2/24 h and 0.221 g/h m2, respectively). In addition, shelf-life analyses revealed that after 40 days of ageing, polymer samples exhibited no visual damage or degradation. The optimal parameters to obtain adequate welding of the SEBS/PP were determined to be power of 60% (18 W), speed of 70 in/sec and 500 Pulse Per Inch (PPI). Furthermore, the bioburden estimates of SEBS/PP of 115 CFU are markedly lower compared to the bioburden estimate of PVC-DEHP of 213 CFU. The SEBS/PP prototype can potentially be an effective alternative to PVC-based blood bags, particularly for high-risk patients in order to reduce the likelihood of medical issues.
The present study compares the surface, textural, and catalytic properties of porous silica doped with bimetallic metal ions that was made from rice husk (RH) biomass. Due to the use of a surfactant during the synthesis process, porous RH-silica (RHS) was derived. In situ doping of silver/copper and ruthenium/copper has been achieved via the xerogel and hydrogel formation methods. The prepared catalysts have been analyzed by various methods, such as surface area and narrow pore size distribution, to confirm their porosity. Powder X-ray diffraction, Fourier transform infrared, and electron microscopy examination were further performed for physicochemical characterization of the synthesized materials. Transmission electron microscopy images showed that ruthenium and copper ions were incorporated perfectly, forming a hexagonal mesoporous (MCM-41) texture due to hydrogel formation and the method of preparation. Copper oxide nanoparticles with silver incorporation in RHS form cube-shaped particles for CuO formation on the surface of the silica matrix instead due to the method of preparation. In this case, ruthenium/copper-doped porous silica forms hexagon-shaped particles of RuO formation in the mesoporous matrix. Finally, the acetylation of glycerol using acetic acid on as-prepared catalysts has been studied. The catalytic activity increases with an increase in temperature and optimization of the molar ratio of glycerol and acetic acid. Increases in temperature result in higher selectivity toward triacetin formation instead of the conventional formation of monoacetin. Hence, we compared the surface physicochemical properties, catalytic conversion, and selectivity nature of bimetallic metal (Ru/Cu and Ag/Cu) ions incorporated in RHS prepared by different synthetic routes.
In this study, an amino-modified aptasensor using multi-walled carbon nanotubes (MWCNTs)-deposited ITO electrode was prepared and evaluated for the detection of pathogenic Salmonella bacteria. An amino-modified aptamer (ssDNA) which binds selectively to whole-cell Salmonella was immobilised on the COOH-rich MWCNTs to produce the ssDNA/MWCNT/ITO electrode. The morphology of the MWCNT before and after interaction with the aptamers were observed using scanning electron microscopy (SEM). Cyclic voltammetry and electrochemical impedance spectroscopy techniques were used to investigate the electrochemical properties and conductivity of the aptasensor. The results showed that the impedance measured at the ssDNA/MWCNT/ITO electrode surface increased after exposure to Salmonella cells, which indicated successful binding of Salmonella on the aptamer-functionalised surface. The developed ssDNA/MWCNT/ITO aptasensor was stable and maintained linearity when the scan rate was increased from 10 mV s-1 to 90 mV s-1. The detection limit of the ssDNA/MWCNT/ITO aptasensor, determined from the sensitivity analysis, was found to be 5.5 × 101 cfu mL-1 and 6.7 × 101 cfu mL-1 for S. Enteritidis and S. Typhimurium, respectively. The specificity test demonstrated that Salmonella bound specifically to the ssDNA/MWCNT/ITO aptasensor surface, when compared with non-Salmonella spp. The prepared aptasensor was successfully applied for the detection of Salmonella in food samples.
Methane is a greenhouse gas which poses a great threat to life on earth as its emissions directly contribute to global warming and methane has a 28-fold higher warming potential over that of carbon dioxide. Ruminants have been identified as a major source of methane emission as a result of methanogenesis by their respective gut microbiomes. Various plants produce highly bioactive compounds which can be investigated to find a potential inhibitor of methyl-coenzyme M reductase (the target protein for methanogenesis). To speed up the process and to limit the use of laboratory resources, the present study uses an in-silico molecular docking approach to explore the anti-methanogenic properties of phytochemicals from Cymbopogon citratus, Origanum vulgare, Lavandula officinalis, Cinnamomum zeylanicum, Piper betle, Cuminum cyminum, Ocimum gratissimum, Salvia sclarea, Allium sativum, Rosmarinus officinalis and Thymus vulgaris. A total of 168 compounds from 11 plants were virtually screened. Finally, 25 scrutinized compounds were evaluated against methyl-coenzyme M reductase (MCR) protein using the AutoDock 4.0 program. In conclusion, the study identified 21 out of 25 compounds against inhibition of the MCR protein. Particularly, five compounds: rosmarinic acid (-10.71 kcal/mol), biotin (-9.38 kcal/mol), α-cadinol (-8.16 kcal/mol), (3R,3aS,6R,6aR)-3-(2H-1,3-benzodioxol-4-yl)-6-(2H-1,3-benzodioxol-5-yl)-hexahydrofuro[3,4-c]furan-1-one (-12.21 kcal/mol), and 2,4,7,9-tetramethyl-5decyn4,7diol (-9.02 kcal/mol) showed higher binding energy towards the MCR protein. In turn, these compounds have potential utility as rumen methanogenic inhibitors in the proposed methane inhibitor program. Ultimately, molecular dynamics simulations of rosmarinic acid and (3R,3aS,6R,6aR)-3-(2H-1,3-benzodioxol-4-yl)-6-(2H-1,3-benzodioxol-5-yl)-hexahydrofuro[3,4-c]furan-1-one yielded the best possible interaction and stability with the active site of 5A8K protein for 20 ns.
Acetylation of glycerol to yield monoacetin (MAT), diacetin (DAT), and triacetin (TAT) over NiO-supported CeO2 (xNiO/CeO2) catalysts is reported. The catalysts were synthesized utilizing a sol-gel technique, whereby different quantities of NiO (x = 9, 27, and 45 wt%) were supported onto the CeO2 substrate, and hexadecyltrimethylammonium bromide (CTABr) served as a porogen. The utilization of EDX elemental mapping analysis confirmed the existence of evenly distributed Ni2+ ion and octahedral NiO nanoparticles on the CeO2 surface through the DRS UV-Vis spectroscopy. The most active catalyst is 27NiO/CeO2 based on TAT selectivity in the glycerol acetylation with ethanoic acid, attaining 97.6% glycerol conversion with 70.5% selectivity to TAT at 170 °C with a 1:10 glycerol/ethanoic acid molar ratio for 30 min using a non-microwave instant heating reactor. The 27NiO/CeO2 is reusable without significant decline in catalytic performance after ten consecutive reaction cycles, indicating high structure stability with accessible active acidity.
Each year, 50 to 70 million tonnes of lignin are produced worldwide as by-products from pulp industries and biorefineries through numerous processes. Nevertheless, about 98% of lignin is directly burnt to produce steam to generate energy for the pulp mills and only a handful of isolated lignin is used as a raw material for the chemical conversion and for the preparation of various substances as well as modification of lignin into nanomaterials. Thus, thanks to its complex structure, the conversion of lignin to nanolignin, attracting growing attention and generating considerable interest in the scientific community. The objective of this review is to provide a complete understanding and knowledge of the synthesis methods and functionalization of various lignin nanoparticles (LNP). The characterization of LNP such as structural, thermal, molecular weight properties together with macromolecule and quantification assessments are also reviewed. In particular, emerging applications in different areas such as UV barriers, antimicrobials, drug administration, agriculture, anticorrosives, the environment, wood protection, enzymatic immobilization and others were highlighted. In addition, future perspectives and challenges related to the development of LNP are discussed.