Heterogeneous Photocatalysis of Metronidazole in Aquatic Samples.
Ontology highlight
ABSTRACT:
SUBMITTER: Stando K
PROVIDER: S-EPMC8708392 | biostudies-literature |
REPOSITORIES: biostudies-literature
Similar Datasets
Project description:The synergy between photocatalysis and continuous flow chemical reactors has shifted the paradigms of photochemistry, opening new avenues of research with safer and scalable processes that can be readily implemented in academia and industry. Current state-of-the-art photocatalysts are homogeneous transition metal complexes that have favourable photophysical properties, wide electrochemical redox potentials, and photostability. However, these photocatalysts present serious drawbacks, such as toxicity, limited availability, and the overall cost of rare transition metal elements. This reduces their long-term viability, especially at an industrial scale. Heterogeneous photocatalysts (HPCats) are an attractive alternative, as the requirement for the separation and purification is largely removed, but typically at the cost of efficiency. Flow chemical reactors can, to a large extent, mitigate the loss in efficiency through reactor designs that enhance mass transport and irradiation. Herein, we review some important developments of heterogeneous photocatalytic materials and their application in flow reactors for sustainable organic synthesis. Further, the application of continuous flow heterogeneous photocatalysis in environmental remediation is briefly discussed to present some interesting reactor designs that could be implemented to enhance organic synthesis.
| S-EPMC7323633 | biostudies-literature
Project description:A long-term exposition of antibiotics represents a serious problem for the environment, especially for human health. Heterogeneous photocatalysis opens a green way for their removal. Here, we correlated the structural-textural properties of TiO2 photocatalysts with their photocatalytic performance in ampicillin abatement. The tested nanoparticles included anatase and rutile and their defined mixtures. The nominal size range varied from 5 to 800 nm, Aeroxide P25 serving as an industrial benchmark reference. The degradation mechanism of photocatalytic ampicillin abatement was studied by employing both experimental (UPLC/MS/MS, hydroxyl radical scavenger) and theoretical (quantum calculations) approaches. Photocatalytic activity increased with the increasing particle size, generally, anatase being more active than rutile. Interestingly, in the dark, the ampicillin concentration decreased as well, especially in the presence of very small nanoparticles. Even if the photolysis of ampicillin was negligible, a very high degree of mineralization of antibiotic was achieved photocatalytically using the smallest nanoparticles of both allotropes and their mixtures. Furthermore, for anatase samples, the reaction rate constant increases with increasing crystallite size, while the degree of mineralization decreases. Importantly, the suggested degradation pathway mechanism determined by DFT modeling was in very good agreement with experimentally detected reaction products.
| S-EPMC8399517 | biostudies-literature
Project description:The dynamics and activities of microbes colonizing organic particles (hereafter particles) greatly determine the efficiency of the aquatic carbon pump. Current understanding is that particle composition, structure and surface properties, determined mostly by the forming organisms and organic matter, dictate initial microbial colonization and the subsequent rapid succession events taking place as organic matter lability and nutrient content change with microbial degradation. We applied a transcriptomic approach to assess the role of stochastic events on initial microbial colonization of particles. Furthermore, we asked whether gene expression corroborates rapid changes in carbon-quality. Commonly used size fractionated filtration averages thousands of particles of different sizes, sources, and ages. To overcome this drawback, we used replicate samples consisting each of 3-4 particles of identical source and age and further evaluated the consequences of averaging 10-1000s of particles. Using flow-through rolling tanks we conducted long-term experiments at near in situ conditions minimizing the biasing effects of closed incubation approaches often referred to as "the bottle-effect." In our open flow-through rolling tank system, however, active microbial communities were highly heterogeneous despite an identical particle source, suggesting random initial colonization. Contrasting previous reports using closed incubation systems, expression of carbon utilization genes didn't change after 1 week of incubation. Consequently, we suggest that in nature, changes in particle-associated community related to carbon availability are much slower (days to weeks) due to constant supply of labile, easily degradable organic matter. Initial, random particle colonization seems to be subsequently altered by multiple organismic interactions shaping microbial community interactions and functional dynamics. Comparative analysis of thousands particles pooled togethers as well as pooled samples suggests that mechanistic studies of microbial dynamics should be done on single particles. The observed microbial heterogeneity and inter-organismic interactions may have important implications for evolution and biogeochemistry in aquatic systems.
| S-EPMC6212488 | biostudies-literature
Project description:Heterogeneous photocatalysis using titanium dioxide as catalyst is an attractive advanced oxidation process due to its high chemical stability, good performance and low cost. When immobilized in a supporting material, additional benefits are achieved in the treatment. The purpose of this study was to develop a simple protocol for impregnation of TiO2-P25 on borosilicate glass spheres and evaluate its efficiency in the photocatalytic degradation using an oxidizable substrate (methylene blue), in a Compound Parabolic Concentrator (CPC) reactor. The assays were conducted at lab-scale using radiation, which simulated the solar spectrum. TiO2 leaching from the glass and the catalyst regeneration were both demonstrated. A very low leaching ratio (0.03%) was observed after 24 h of treatment, suggesting that deposition of TiO2 resulted in good adhesion and stability of the photocatalyst on the surface of borosilicate. This deposition was successfully achieved after calcination of the photocatalyst at 400 °C (TiO2-400 °C). The TiO2 film was immobilized on glass spheres and the powder was characterized by scanning electron microscopy (SEM), X-ray diffraction and BET. This characterization suggested that thermal treatment did not introduce substantial changes in the measured microstructural characteristics of the photocatalyst. The immobilized photocatalyst degraded more than 96% of the MB in up to 90 min of reaction. The photocatalytic activity decreased after four photocatalytic cycles, but it was recovered by the removal of contaminants adsorbed on the active sites after washing in water under UV-Vis irradiation. Based on these results, the TiO2-400 °C coated on glass spheres is potentially a very attractive option for removal of persistent contaminants present in the environment.
| S-EPMC5844248 | biostudies-literature
Project description:Several methods have been developed to measure dynamic functional connectivity (dFC) in fMRI data. These methods are often based on a sliding-window analysis, which aims to capture how the brain's functional organization varies over the course of a scan. The aim of many studies is to compare dFC across groups, such as younger versus older people. However, spurious group differences in measured dFC may be caused by other sources of heterogeneity between people. For example, the shape of the haemodynamic response function (HRF) and levels of measurement noise have been found to vary with age. We use a generic simulation framework for fMRI data to investigate the effect of such heterogeneity on estimates of dFC. Our findings show that, despite no differences in true dFC, individual differences in measured dFC can result from other (non-dynamic) features of the data, such as differences in neural autocorrelation, HRF shape, connectivity strength and measurement noise. We also find that common dFC methods such as k-means and multilayer modularity approaches can detect spurious group differences in dynamic connectivity due to inappropriate setting of their hyperparameters. fMRI studies therefore need to consider alternative sources of heterogeneity across individuals before concluding differences in dFC.
| S-EPMC5590721 | biostudies-literature
Project description:Metal-organic frameworks (MOFs) are commended as photocatalysts for H2 evolution and CO2 reduction as they combine light-harvesting and catalytic functions with excellent reactant adsorption capabilities. For dynamic processes in liquid phase, the accessibility of active sites becomes a critical parameter as reactant diffusion is limited by the inherently small micropores. Our strategy is to introduce additional mesopores by selectively removing one ligand in mixed-ligand MOFs via thermolysis. Here we report photoactive MOFs of the MIL-125-Ti family with two distinct mesopore architectures resembling either large cavities or branching fractures. The ligand removal is highly selective and follows a 2-step process tunable by temperature and time. The introduction of mesopores and the associated formation of new active sites have improved the HER rates of the MOFs by up to 500%. We envision that this strategy will allow the purposeful engineering of hierarchical MOFs and advance their applicability in environmental and energy technologies.
| S-EPMC8755752 | biostudies-literature
Project description:Riparian spiders are being used increasingly to track spatial patterns of contaminants in and fluxing from aquatic ecosystems. However, our understanding of the circumstances under which spiders are effective sentinels of aquatic pollution is limited. The present study tests the hypothesis that riparian spiders may be effectively used to track spatial patterns of sediment pollution by polychlorinated biphenyls (PCBs) in aquatic ecosystems with high habitat heterogeneity. The spatial pattern of ?PCB concentrations in 2 common families of riparian spiders sampled in 2011 to 2013 generally tracked spatial variation in sediment ?PCBs across all sites within the Manistique River Great Lakes Area of Concern (AOC), a rivermouth ecosystem located on the south shore of the Upper Peninsula, Manistique (MI, USA) that includes harbor, river, backwater, and lake habitats. Sediment ?PCB concentrations normalized for total organic carbon explained 41% of the variation in lipid-normalized spider ?PCB concentrations across 11 sites. Furthermore, 2 common riparian spider taxa (Araneidae and Tetragnathidae) were highly correlated (r2 ?>?0.78) and had similar mean ?PCB concentrations when averaged across all years. The results indicate that riparian spiders may be useful sentinels of relative PCB availability to aquatic and riparian food webs in heterogeneous aquatic ecosystems like rivermouths where habitat and contaminant variability may make the use of aquatic taxa less effective. Furthermore, the present approach appears robust to heterogeneity in shoreline development and riparian vegetation that support different families of large web-building spiders. Environ Toxicol Chem 2017;36:1278-1286. Published 2016 Wiley Periodicals, Inc. on behalf of SETAC. This article is a US government work and, as such, is in the public domain in the United States of America.
| S-EPMC7362337 | biostudies-literature
Project description:A periodic mesoporous organosilica (PMO) containing 2,2'-bipyridine groups (BPy-PMO) has been shown to possess a unique pore wall structure in which the 2,2'-bipyridine groups are densely and regularly packed. The surface 2,2'-bipyridine groups can function as chelating ligands for the formation of metal complexes, thus generating molecularly-defined catalytic sites that are exposed on the surface of the material. We here report the construction of a heterogeneous water oxidation photocatalyst by immobilizing several types of tris(2,2'-bipyridine)ruthenium complexes on BPy-PMO where they function as photosensitizers in conjunction with iridium oxide as a catalyst. The Ru complexes produced on BPy-PMO in this work were composed of three bipyridine ligands, including the BPy in the PMO framework and two X2bpy, denoted herein as Ru(X)-BPy-PMO where X is H (2,2'-bipyridine), Me (4,4'-dimethyl-2,2'-bipyridine), t-Bu(4,4'-di-tert-butyl-2,2'-bipyridine) or CO2Me (4,4'-dimethoxycarbonyl-2,2'-bipyridine). Efficient photocatalytic water oxidation was achieved by tuning the photochemical properties of the Ru complexes on the BPy-PMO through the incorporation of electron-donating or electron-withdrawing functionalities. The reaction turnover number based on the amount of the Ru complex was improved to 20, which is higher than values previously obtained from PMO systems acting as water oxidation photocatalysts.
| S-EPMC9051631 | biostudies-literature
Project description:The β-Lactam antibiotic amoxicillin is among the most widely used antibiotics in human and veterinary medicine. Consequently, amoxicillin is abundant in natural waters and can undergo diverse abiotic reactions to form degradation compounds under environmental conditions. Yet, little is known about these decay pathways and mineralogical impacts on environmental amoxicillin degradation. The current study focuses on understanding the mineralogical influences of amoxicillin degradation under ecological conditions. We studied the role of anatase and kaolinite on amoxicillin degradation under irradiated and non-irradiated conditions. Anatase increases amoxicillin degradation by 4.5-fold in the presence of light compared to just being exposed to sunlight. Interestingly, anatase also showed a higher degradation rate under dark than light controls. Conversely, kaolinite diminishes the amoxicillin degradation under irradiation. The formation of degradation compounds was mineralogy-controlled, while no mineralization was observed. Further, we irradiated amoxicillin with a high-intensity light to evaluate its removal from wastewater. The formation of varying amoxicillin degradation products with high-intensity light will limit its removal from wastewater. Our study emphasizes that the mineralogical impact on amoxicillin degradation is diverse, and the role of anatase is significant. Consequently, the increased addition of manufactured titanium nanoparticles to the environment can further enhance these effects.
| S-EPMC9498904 | biostudies-literature
Project description:Transcriptome deconvolution in cancer and other heterogeneous tissues remains challenging. Available methods lack the ability to estimate both component-specific proportions and expression profiles for individual samples. We present DeMixT, a new tool to deconvolve high-dimensional data from mixtures of more than two components. DeMixT implements an iterated conditional mode algorithm and a novel gene-set-based component merging approach to improve accuracy. In a series of experimental validation studies and application to TCGA data, DeMixT showed high accuracy. Improved deconvolution is an important step toward linking tumor transcriptomic data with clinical outcomes. An R package, scripts, and data are available: https://github.com/wwylab/DeMixTallmaterials.
| S-EPMC6249353 | biostudies-literature