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1.
Environ Sci Technol ; 58(37): 16589-16599, 2024 Sep 17.
Artículo en Inglés | MEDLINE | ID: mdl-39238135

RESUMEN

The aqueous FeIV-oxo complex and FeIII-peroxy complex (e.g., ligand-assisted or interfacial FeIII-hydroperoxo intermediates) have been recognized as crucial reactive intermediates for decontamination in iron-based Fenton-like processes. Intermediates with terminal oxo ligands can undergo the oxygen atom exchange process with water molecules, whereas peroxides are unable to induce such exchanges. Therefore, these distinct metal-oxygen complexes can be distinguished based on the above feature. In this study, we identified previously unknown intermediates with a peroxy moiety and cobalt center that were generated during peroxymonosulfate (PMS) activation via aqueous CoII ions under acidic conditions. Results of theoretical calculations and tip-enhanced Raman spectroscopy revealed that the CoII ion tended to coordinate with the PMS anion to form a bidentate complex with a tetrahedral structure. These reactive cobalt intermediates were collectively named the CoII-PMS* complex. Depending on the inherent characteristics of the target contaminants, the CoII-PMS* complex can directly oxidize organic compounds or trigger PMS disproportionation to release hydroxyl radicals and sulfate radicals for collaborative decontamination. This work provides a comparative study between iron- and cobalt-based Fenton-like processes and proposes novel insights from the standpoint of diverse metal-oxygen complexes.


Asunto(s)
Cobalto , Hierro , Oxígeno , Cobalto/química , Hierro/química , Oxígeno/química , Peróxido de Hidrógeno/química , Oxidación-Reducción , Peróxidos/química
2.
J Thorac Dis ; 16(8): 5262-5273, 2024 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-39268134

RESUMEN

Background: The microbial signatures in diabetes with pneumonia and the risk factors of severe pneumonia (SP) in diabetic patients are not clear. Our study explored microbial signatures and the association between clinical characteristics and SP then constructed a risk model to find effective biomarkers for predicting pneumonia severity. Methods: Our study was conducted among 273 patients with pneumonia diagnosed and treated in our hospital from January 2018 to May 2021. Bronchoalveolar lavage fluid (BALF) samples and clinical data were collected. Metagenomic sequencing was applied after extracting the DNA from samples. Appropriate statistical methods were used to compare the microbial signatures and clinical characteristics in patients with or without diabetes mellitus (DM). Results: In total, sixty-one pneumonia patients with diabetes and 212 pneumonia patients without diabetes were included. Sixty-six differential microorganisms were found to be associated with SP in diabetic patients. Some microbes correlated with clinical indicators of SP. The prediction model for SP was established and the receiver operating characteristic (ROC) curve demonstrated its accuracy, with the sensitivity and specificity of 0.82 and 0.91, respectively. Conclusions: Some microorganisms affect the severity of pneumonia. We identified the microbial signatures in the lower airways and the association between clinical characteristics and SP. The predictive model was more accurate in predicting SP by combining microbiological indicators and clinical characteristics, which might be beneficial to the early identification and management of patients with SP.

3.
ACS Omega ; 9(25): 26878-26899, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38947792

RESUMEN

Prostate cancer (PCa) is the second most common cancer in males worldwide. Androgen deprivation therapy (ADT) is the primary treatment method used for PCa. Although more effective androgen synthesis and antiandrogen inhibitors have been developed for clinical practice, hormone resistance increases the incidence of ADT-insensitive prostate cancer and poor prognoses. The tumor microenvironment (TME) has become a research hotspot with efforts to identify treatment targets based on the characteristics of the TME to improve prognosis. Herein, we introduce the basic characteristics of the PCa TME and the side effects of traditional prostate cancer treatments. We further highlight the emergence of novel nanotherapy strategies, their therapeutic mechanisms, and their effects on the PCa microenvironment. With further research, clinical applications of nanotherapy for PCa are expected in the near future. Collectively, this Review provides a valuable resource regarding the various nanotherapy types, demonstrating their broad clinical prospects to improve the quality of life in patients with PCa.

4.
Ecol Evol ; 14(7): e11614, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38952650

RESUMEN

Janzen-Connell (JC) effects, hypothesized to be partially driven by negative plant-soil feedbacks (PSFs), are considered to be a key mechanism that regulates tropical forest plant diversity and coexistence. However, intraspecific variation in JC effects may weaken this mechanism, with the strength of PSFs being a potentially key variable process. We conducted a manipulated experiment with seedlings from two populations of Pometia pinnata (Sapindaceae), a tropical tree species in southwest China. We aimed to measure the intraspecific difference in PSF magnitude caused by inoculating the soil from different P. pinnata source populations and growing seedlings under differing light intensity and water availability treatments, and at varying plant densities. We found negative PSFs for both populations with the inoculum soil originating from the same sites, but PSFs differed significantly with the inoculum soil from different sites. PSF strength responded differently to biotic and abiotic drivers; PSF strength was weaker in low moisture and high light treatments than in high moisture and low light treatments. Our study documents intraspecific variation in JC effects: specifically, P. pinnata have less defenses to their natively-sourced soil, but are more defensive to the soil feedbacks from soil sourced from other populations. Our results imply that drought and light intensity tended to weaken JC effects, which may result in loss of species diversity with climate change.

5.
Water Res ; 257: 121684, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38723348

RESUMEN

Natural manganese oxides could induce the intermolecular coupling reactions among small-molecule organics in aqueous environments, which is one of the fundamental processes contributing to natural humification. These processes could be simulated to design novel advanced oxidation technology for water purification. In this study, periodate (PI) was selected as the supplementary electron-acceptor for colloidal manganese oxides (Mn(IV)aq) to remove phenolic contaminants from water. By introducing polyferric sulfate (PFS) into the Mn(IV)aq/PI system and exploiting the flocculation potential of Mn(IV)aq, a post-coagulation process was triggered to eliminate soluble manganese after oxidation. Under acidic conditions, periodate exists in the H4IO6- form as an octahedral oxyacid capable of coordinating with Mn(IV)aq to form bidentate complexes or oligomers (Mn(IV)-PI*) as reactive oxidants. The Mn(IV)-PI* complex could induce cross-coupling process between phenolic contaminants, resulting in the formation of oligomerized products ranging from dimers to hexamers. These oligomerized products participate in the coagulation process and become stored within the nascent floc due to their catenulate nature and strong hydrophobicity. Through coordination between Mn(IV)aq and H4IO6-, residual periodate is firmly connected with manganese oxides in the floc after coagulation and could be simultaneously separated from the aqueous phase. This study achieves oxidizing oligomerization through a homogeneous process under mild conditions without additional energy input or heterogeneous catalyst preparation. Compared to traditional mineralization-driven oxidation techniques, the proposed novel cascade processes realize transformation, convergence, and separation of phenolic contaminants with high oxidant utilization efficiency for low-carbon purification.


Asunto(s)
Oxidación-Reducción , Purificación del Agua , Purificación del Agua/métodos , Óxidos/química , Compuestos de Manganeso/química , Contaminantes Químicos del Agua/química , Floculación
6.
J Colloid Interface Sci ; 670: 323-336, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38763028

RESUMEN

Selective removal of target organic pollutants in complex water quality of municipal sewage is extremely important for the deep treatment of water quality. Here, energetic MOF and Fe-MOF are doped in electrostatic spinning process to adjust the structure and composition of the catalysts, active oxygen species (ROSs), realizing the selective removal of organic pollutants. Non-azo and azo pollutants are selected as target pollutants. Catalysts PCFe-8 with Fe nanoclusters, EPCFe-8 with Fe-Nx, and EPC-8 without Fe doping are used to activate peroxymonosulfate (PMS) for degrading pollutants. The results show that the PCFe-8/PMS system can produce the most SO4- and exhibit superior removal of azo pollutants, whereas the degradation behavior of non-azo pollutants is more inclined to occur in the EPCFe-8/PMS system and the EPC-8/PMS system. This work provides a reference for elucidating the relationship between catalyst structure and components, types of ROSs, and selective degradation of pollutants.

7.
Water Res ; 251: 121113, 2024 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-38215539

RESUMEN

A novel treatment technique by coupling granular activated carbon (GAC) adsorption and ozone regeneration was constructed for long-lasting water decontamination. The GAC adsorption showed high performance for atrazine (ATZ) removal (99.9 %), and the ozone regeneration ensured the recyclability of GAC for water purification. The regeneration process was evaluated via several paths to assist the efficient adsorption process. Employing ozone micro-nano bubbles (O3-MNBs) for regenerating GAC showed superior performance compared to traditional ozone. Meantime, inhibiting the formation of bromate (BrO3-). ATZ adsorption process suffered from the pore-filling, hydrogen bonding effect and π-π EDA interaction. The surface phenolic hydroxyl group, carboxyl group and pyridine nitrogen benefitted the triggering of ozone to generate reactive oxygen species, and regenerate the GAC surface. The superior performance of the adsorption and regeneration process was verified via a long-term running by a pilot study. It significantly improved the removal of organic micropollutants, UV254 and permanganate index. Additionally, the intermittent O3-MNBs regeneration process resulted in efficient decontamination within the pores structure of GAC, which also effectively preserved the pore structure from destruction. For actual application, the cost of water production can be saved around 0.63 kWh m-3. This work proposed new ideas and theoretical support for economic water production.


Asunto(s)
Atrazina , Bencenosulfonatos , Ozono , Contaminantes Químicos del Agua , Purificación del Agua , Carbón Orgánico/química , Proyectos Piloto , Ozono/química , Purificación del Agua/métodos , Contaminantes Químicos del Agua/análisis , Agua , Adsorción
8.
Water Res ; 246: 120697, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37837899

RESUMEN

The selective and rapid elimination of refractory organic pollutants from surface water is significant. However, the relationship of between reactive oxygen species (ROSs) and diversified pollutants molecular structures still needs to be further clarified. Here, we utilize polydopamine (PDA)-assisted coating strategy to prepare hollow 2D carbon nanosheet (ZPL-HCNS) and 2D Co3O4 nanosheet (ZPL-Co3O4) by thermolysis of PDA coated ZIF-L (ZIF-L@PDA) precursor under different gas atmosphere, which realizes the controlled generation of radicals and non-radicals. Organic pollutants including bisphenols, sulfonamides, quinolones, tetracyclines, and azo dyes are applied to assess the catalytic performance. Results show that dyes containing azo structure are more likely to be degraded by radical process, which is due to that the energy (ΔE) requirements to break the azo bond is higher than energy released from singlet oxygen to oxygen molecule and lower than that of sulfate radical to sulfate. Frontier molecular orbital theory HOMO-LUMO and Fukui function expounded the possible selectivity mechanism. In addition, the degradation pathway and biotoxicity test are carried out. This work provides a reference to illustrate the selective degradation for ROSs and molecular structure of pollutants.


Asunto(s)
Contaminantes Ambientales , Especies Reactivas de Oxígeno , Estructura Molecular , Oxígeno Singlete , Oxidación-Reducción
9.
EBioMedicine ; 96: 104790, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37708700

RESUMEN

BACKGROUND: Severe community-acquired pneumonia (SCAP) results in high mortality as well as massive economic burden worldwide, yet limited knowledge of the bio-signatures related to prognosis has hindered the improvement of clinical outcomes. Pathogen, microbes and host are three vital elements in inflammations and infections. This study aims to discover the specific and sensitive biomarkers to predict outcomes of SCAP patients. METHODS: In this study, we applied a combined metagenomic and transcriptomic screening approach to clinical specimens gathered from 275 SCAP patients of a multicentre, prospective study. FINDINGS: We found that 30-day mortality might be independent of pathogen category or microbial diversity, while significant difference in host gene expression pattern presented between 30-day mortality group and the survival group. Twelve outcome-related clinical characteristics were identified in our study. The underlying host response was evaluated and enrichment of genes related to cell activation, immune modulation, inflammatory and metabolism were identified. Notably, omics data, clinical features and parameters were integrated to develop a model with six signatures for predicting 30-day mortality, showing an AUC of 0.953 (95% CI: 0.92-0.98). INTERPRETATION: In summary, our study linked clinical characteristics and underlying multi-omics bio-signatures to the differential outcomes of patients with SCAP. The establishment of a comprehensive predictive model will be helpful for future improvement of treatment strategies and prognosis with SCAP. FUNDING: National Natural Science Foundation of China (No. 82161138018), Shanghai Municipal Key Clinical Specialty (shslczdzk02202), Shanghai Top-Priority Clinical Key Disciplines Construction Project (2017ZZ02014), Shanghai Key Laboratory of Emergency Prevention, Diagnosis and Treatment of Respiratory Infectious Diseases (20dz2261100).

10.
J Colloid Interface Sci ; 652(Pt A): 69-81, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37591085

RESUMEN

Electrospinning MOFs nanoparticles derived porous carbon nanofibers with rational structure and design are recently as environmentally friendly and highly efficient catalytic materials for wastewater treatment. However, most of the pore-making strategies are based on precursors structural shrinkage during pyrolysis, which is a challenge to create abundant large pores and open channels. Here, a confined expansion pore-making strategy with active MOF is introduced, where energetic Zn-MOF (Zn2+/triazole) and ZIF-67 (Co2+/dimethylimidazole) are utilized as pore forming additive and precursor of active sites, respectively. The high nitrogen content gives triazole the ability to puff up and realizes N-doped during pyrolysis. Moreover, degradation mechanisms and pathways of pollutants were measured by 3D EEM, LC-MS, quenching experiments, and Fukui function. This pore-making strategy via energetic MOF local contraction and expansion provides a novel method to prepare diversiform function porous carbon materials for environmental remediation.

11.
Cell Biosci ; 13(1): 111, 2023 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-37332019

RESUMEN

BACKGROUND: The early accurate diagnoses for autoimmune encephalitis (AE) and infectious encephalitis (IE) are essential since the treatments for them are different. This study aims to discover some specific and sensitive biomarkers to distinguish AE from IE at early stage to give specific treatments for good outcomes. RESULTS: We compared the host gene expression profiles and microbial diversities of cerebrospinal fluid (CSF) from 41 patients with IE and 18 patients with AE through meta-transcriptomic sequencing. Significant differences were found in host gene expression profiles and microbial diversities in CSF between patients with AE and patients with IE. The most significantly upregulated genes in patients with IE were enriched in pathways related with immune response such as neutrophil degranulation, antigen processing and presentation and adaptive immune system. In contrast, those upregulated genes in patients with AE were mainly involved in sensory organ development such as olfactory transduction, as well as synaptic transmission and signaling. Based on the differentially expressed genes, a classifier consisting of 5 host genes showed outstanding performance with an area under the receiver operating characteristic (ROC) curve (AUC) of 0.95. CONCLUSIONS: This study provides a promising classifier and is the first to investigate transcriptomic signatures for differentiating AE from IE by using meta-transcriptomic next-generation sequencing technology.

12.
Environ Sci Pollut Res Int ; 30(30): 75156-75169, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-37217816

RESUMEN

Nano zero-valent iron (nZVI) has a great potential for arsenic removal, but it would form aggregates easily and consume largely by H+ in the strongly acidic solution. In this work, 15%CaO doped with nZVI (15%CaO-nZVI) was successfully synthesized from a simplified ball milling mixture combined with a hydrogen reduction method, which had a high adsorption capacity for As(V) removal from high-arsenic acid wastewater. More than 97% As(V) was removed by 15%CaO-nZVI under the optimum reaction conditions of pH 1.34, initial As(V) concentration 16.21 g/L, and molar ratio of Fe/As (nFe/nAs) 2.5:1. The effluent pH solution was weakly acidic 6.72, and the secondary arsenic removal treatment reduced the solid waste and improved arsenic grade in slag from the mass fraction of 20.02% to 29.07%. Multiple mechanisms including Ca2+ enhanced effect, adsorption, reduction, and co-precipitation coexisted for As(V) removal from high-arsenic acid wastewater. Doping of CaO might lead to improving cracking channels which was benefit for electronic transmission and the confusion of atomic distribution. The in situ weak alkaline environment generated on the surface of 15%CaO-nZVI would increase the content of γ-Fe2O3/Fe3O4, which was in favor for As(V) adsorption. In addition, H+ in the strongly acidic solution could accelerate corrosion of 15%CaO-nZVI and abundant fresh and reactive iron oxides continuously generated, which would provide plenty specific reactive site and fast charge transfer and ionic mobility for arsenic removal.


Asunto(s)
Arsénico , Contaminantes Químicos del Agua , Purificación del Agua , Hierro/química , Arsénico/análisis , Aguas Residuales , Contaminantes Químicos del Agua/análisis , Óxidos/química , Adsorción
13.
Sci Rep ; 13(1): 6989, 2023 04 28.
Artículo en Inglés | MEDLINE | ID: mdl-37117238

RESUMEN

Low-frequency magnetic fields exert a significant inhibitory effect on tumor growth and have been developed as a therapeutic modality. However, the effect of a low-frequency magnetic field on the interaction between cells is still poorly understood. This study aimed to preliminarily evaluate the direct effect of magnetic field ditectely on cultured cells and indirect effect mediated by cell-environment (conditioned medium). 293 T cells, Hepg2 cells, A549 cells have been cultured at 37 ± 0.18 °C in presence of an extremely low-frequency magnetic field of 20 Hz, 5-mT. The adherent tumor cells were more sensitive to magnetic field inhibition in the original environment (conditioned medium) with adherence inhibition rate for Hepg2 and A549 estimated at 18% and 30% respectively. The inhibition effect was suppressed when the suspended cells separated or clump density at a low density. The nontumor cell lines showed no inhibitory effect on exposure to a low-frequency magnetic field. The intracellular ion fluorescence (IIF) showed that the magnetic field significantly altered the membrane potential, indicating hyperpolarization of the adherent cells (ΔIIF 293 T cells: - 25%, ΔIIF Hepg2 cells: - 20% and ΔIIF A549 cells: - 13%) and depolarization of the suspended cells (ΔIIF Raji cells: + 9%). In addition, the conditioned media collected after magnetic field exposure acted on unexposed tumor cells and caused inhibition. Our findings might provide a basis for the mechanism of magnetic field interaction between cells and cell environment in the future.


Asunto(s)
Campos Electromagnéticos , Campos Magnéticos , Medios de Cultivo Condicionados/farmacología , Línea Celular
14.
Environ Sci Technol ; 57(16): 6723-6732, 2023 04 25.
Artículo en Inglés | MEDLINE | ID: mdl-37043741

RESUMEN

Identifying reactive species in advanced oxidation process (AOP) is an essential and intriguing topic that is also challenging and requires continuous efforts. In this study, we exploited a novel AOP technology involving peracetic acid (PAA) activation mediated by a MnII-nitrilotriacetic acid (NTA) complex, which outperformed iron- and cobalt-based PAA activation processes for rapidly degrading phenolic and aniline contaminants from water. The proposed MnII/NTA/PAA system exhibited non-radical oxidation features and could stoichiometrically oxidize sulfoxide probes to the corresponding sulfone products. More importantly, we traced the origin of O atoms from the sulfone products by 18O isotope-tracing experiments and found that PAA was the only oxygen-donor, which is different from the oxidation process mediated by high-valence manganese-oxo intermediates. According to the results of theoretical calculations, we proposed that NTA could tune the coordination circumstance of the MnII center to elongate the O-O bond of the complexed PAA. Additionally, the NTA-MnII-PAA* molecular cluster presented a lower energy gap than the MnII-PAA complex, indicating that the MnII-peroxy complex was more reactive in the presence of NTA. Thus, the NTA-MnII-PAA* complex exhibited a stronger oxidation potential than PAA, which could rapidly oxidize organic contaminants from water. Further, we generalized our findings to the CoII/PAA oxidation process and highlighted that the CoII-PAA* complex might be the overlooked reactive cobalt species. The significance of this work lies in discovering that sometimes the metal-peroxy complex could directly oxidize the contaminants without the further generation of high-valence metal-oxo intermediates and/or radical species through interspecies oxygen and/or electron transfer.


Asunto(s)
Complejos de Coordinación , Contaminantes Químicos del Agua , Ácido Peracético , Oxígeno , Metales , Complejos de Coordinación/química , Cobalto , Oxidación-Reducción , Agua , Peróxido de Hidrógeno
15.
Chemosphere ; 330: 138654, 2023 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-37044142

RESUMEN

Enzymes immobilized on the surface of the carriers are difficult to maintain their conformation and high activity due to the influence of the external harsh environments. A biomimetic core-shell PDA@Lac bioreactor was constructed by depositing polydopamine (PDA) on the surface of the recombinant Escherichia coli with CotA laccase gene, and releasing intracellular laccase into the PDA shell using ultrasound to break the cell wall of the bacteria. The bioreactor provided a nano-confined environment for the laccase and accelerated the mass and electron transfer in the volume-confined space, with a 2.77-fold increase in Km compared with the free laccase. Since there was no barrier of the cell wall, the crystal violet dye can enter the bioreactor to participate in the enzymatic reaction. As a result, PDA@Lac achieved excellent decolorization performance even without ABTS as an electron mediator. Moreover, the cytoplasmic solution retained in the PDA shell promoted the enzyme's tolerance to pH, temperature and harsh environments. In addition to PDA encapsulation, carbonyl and -NH2 groups of PDA were bound covalently with -NH2 and -COOH on the laccase in the PDA@Lac, resulting in an extremely high laccase loading of 817.59 mg/g. Also, the relative activity of the bioreactor maintained approximately 75% after 10 cycles of reuse. In addition, the protection of the PDA shell increased the resistance of laccase to UV irradiation. This work provides a novel method of laccase immobilization for application in wastewater treatment.


Asunto(s)
Biomimética , Lacasa , Lacasa/química , Polímeros/química , Enzimas Inmovilizadas/química , Reactores Biológicos , Colorantes
16.
Chemosphere ; 313: 137251, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36395895

RESUMEN

This study was carried out to investigate the enhanced removal of arsenite (As(III)) by potassium ferrate (K2FeO4) coupled with three Al-based coagulants, which focused innovatively on the distribution and transformation of hydrolyzed aluminum species as well as the mechanism of K2FeO4 interacted with different aluminum hydrolyzed polymers during As(III) removal. Results demonstrated that As(III) removal efficiency could be substantially elevated by K2FeO4 coupled with three Al-based coagulants treatment and the optimum As(III) removal effect was occurred at pH 6 with more than 97%. K2FeO4 showed a great effect on the distribution and transformation of aluminum hydrolyzed polymers and then coupled with a variety of aluminum species produced by the hydrolysis of aluminum coagulants for arsenic removal. During enhanced coagulation, arsenic removal by AlCl3 was main through the charge neutralization of in situ Al13 and the sweep flocculation of Al(OH)3, while PACl1 mainly depended on the charge neutralization of preformed Al13 and the bridging adsorption of Al13 aggregates, whereas PACl2 mainly relied on the sweep flocculation of Al(OH)3. This study provided a new insight into the distribution and transformation of aluminum species for the mechanism of As(III) removal by K2FeO4 coupled with different Al-based coagulants.


Asunto(s)
Arsénico , Purificación del Agua , Aluminio , Purificación del Agua/métodos , Hidróxido de Aluminio , Polímeros , Floculación
17.
Environ Sci Pollut Res Int ; 30(4): 10697-10709, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36083368

RESUMEN

It is well known the capacity of potassium ferrate (Fe(VI)) for the oxidation of pollutants or co-precipitation and adsorption of hazardous species. However, little information has been paid on the adsorption and co-precipitation contribution of the Fe(VI) resultant nanoparticles, the in situ hydrolytic ferric iron oxides. Here, the removal of arsenate (As(V)) and arsenite (As(III)) by Fe(VI) was investigated, which focused on the interaction mechanisms of Fe(VI) with arsenic, especially in the contribution of the co-precipitation and adsorption of its hydrolytic ferric iron oxides. pH and Fe(VI) played significant roles on arsenic removal; over 97.8% and 98.1% of As(V) and As(III) removal were observed when Fe(VI):As(V) and Fe(VI):As(III) were 24:1 and 16:1 at pH 4, respectively. The removal of As(V) and As(III) by in situ and ex situ formed hydrolytic ferric iron oxides was examined respectively. The results revealed that As(III) was oxidized by Fe(VI) to As(V), and then was removed though co-precipitation and adsorption by the hydrolytic ferric iron oxides with the contribution content was about 1:3. For As(V), it could be removed directly by the in situ formed particles from Fe(VI) through co-precipitation and adsorption with the contribution content was about 1:1.5. By comparison, As(III) and As(V) were mainly removed through adsorption by the 30-min hydrolytic ferric iron oxides during the ex situ process. The hydrolytic ferric iron oxides size was obviously different in the process of in situ and ex situ, possessing abundant and multiple morphological structures ferric oxides, which was conducive for the efficient removal of arsenic. This study would provide a new perspective for understanding the potential of Fe(VI) treatment on arsenic control.


Asunto(s)
Arsénico , Arsenitos , Nanopartículas , Contaminantes Químicos del Agua , Arseniatos , Arsénico/química , Hierro/química , Compuestos Férricos , Oxidación-Reducción , Óxidos/química , Adsorción , Contaminantes Químicos del Agua/química , Concentración de Iones de Hidrógeno
18.
Environ Sci Pollut Res Int ; 30(13): 38480-38499, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36577825

RESUMEN

In this study, a novel in situ iron-loaded activated carbon (AFPAC) was prepared by a FeSO4/K2FeO4 impregnation and oxidation combination two-step supported on activated carbon for enhanced removal of Cr(VI) from aqueous solutions. Cr(VI) removal efficiency greatly increased by AFPAC more than 70% than that of fresh activated carbon (AC), which is due to rich iron oxides formed in situ and the synergistic effect between iron oxides and activated carbon. Cr(VI) adsorption behaviors on AFPAC under different water quality parameters were investigated. The maximum monolayer adsorption capacities for Cr(VI) by AFPAC are as high as 26.24 mg/g, 28.65 mg/g, and 32.05 mg/g at 25 °C, 35 °C and 45 °C at pH 4, respectively. Density functional theory (DFT) results showed that the adsorption energy of K2Cr2O7 on the surface of FeOOH was - 2.52 eV, which was greater than that on the surface of bare AC, and more charge transfer occurred during the adsorption of K2Cr2O7 on the surface of FeOOH, greatly promoting the formation of Cr = O-Fe. Cr(VI) removal by AFPAC included electrostatic attraction, redox reaction, coordinate complexation, and co-precipitation. Cr(VI) adsorption process on AFPAC consisted of the three reaction steps: (1) AFPAC was fast protonation and Cr2O72- would electrostatically attract to the positively charged AFPAC surface. (2) Cr2O72- was reduced into Cr2O3 by the carbons bond to the oxygen functionalities on activated carbon and the redox reaction process of FeSO4 and K2FeO4. (3) The inner-sphere complexes were formed, and adsorbed on AFPAC by iron oxides and then co-precipitation.


Asunto(s)
Hierro , Contaminantes Químicos del Agua , Hierro/química , Carbón Orgánico/química , Contaminantes Químicos del Agua/análisis , Cromo/química , Adsorción , Compuestos Ferrosos , Óxidos
19.
Molecules ; 27(21)2022 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-36364281

RESUMEN

Natural organic matter (NOM) has always been considered the main precursor of disinfection by-products (DBPs) during the chlorine disinfection of drinking water. This research focuses on investigating the correlation between the functional group (carboxyl and carbonyl groups) content of NOM and the formation of trichloromethane (TCM) and chloral hydrate (CH). The quantitative determination of carboxyl groups, carbonyl groups, TCM, and CH were conducted during the drinking water treatment processes with different coagulant dosages and with/without pre-oxidation by KMnO4 or NaClO. The most appropriate coagulant for the removal of conventional components was polyaluminum chloride (PAC), and the dosage was 110 mg/L. Up to 43.7% and 14.5% of the carboxyl and carbonyl groups, respectively, were removed through the coagulation and sedimentation processes, which can be enhanced by increasing PAC dosage. The filtration process further increased the removal rates of these two functional groups to 59.8% and 33.5%, respectively. The formation potential of the TCM and CH decreased as the PAC dosage increased. Pre-oxidation by KMnO4 (0.8-1.0 mg/L) effectively controlled the formation of DBPs while increasing the carboxyl and carbonyl group content. Pre-oxidation by NaClO decreased the formation of TCM rather than CH, and a suitable amount (0.5-1.0 mg/L) decreased the carboxyl and carbonyl groups. It was found that there was a good linear correlation between carboxyl groups and TCM and CH. The linear fit R2 values of the carboxyl groups to TCM and CH were 0.6644 and 0.7957, respectively. The linear fit R2 values of the carbonyl groups to TCM and CH were 0.5373 and 0.7595, respectively.


Asunto(s)
Desinfectantes , Agua Potable , Contaminantes Químicos del Agua , Purificación del Agua , Trihalometanos/análisis , Hidrato de Cloral/análisis , Agua Potable/análisis , Cloro/análisis , Desinfección , Cloroformo , Contaminantes Químicos del Agua/análisis , Halogenación , Desinfectantes/análisis
20.
Front Cell Infect Microbiol ; 12: 947486, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36189364

RESUMEN

Whipple's disease is a rare chronic systemic disease that affects almost any organ system of the body caused by the intracellular bacterium Tropheryma whipplei, which is found ubiquitously in the environment. Sequencing of the T. whipplei genome has revealed that it has a reduced genome (0.93 Mbp), a characteristic shared with other intracellular bacteria. Until our research started, 19 T. whipplei strains had been sequenced from cultures originated in France, Canada, and Germany. The genome of T. whipplei bacterium has not been studied in Asia yet. Here, two metagenome-assembled genomes (MAGs) of T. whipplei from China were reconstructed through metagenomic next-generation sequencing (mNGS) and genome binning. We also provided genomic insights into the geographical role and genomic features by analyzing the whole genome. The whole-genome phylogenetic tree was constructed based on single-nucleotide polymorphism (SNP) distance calculations and then grouped by distance similarity. The phylogenetic tree shows inconsistencies with geographic origins, thus suggesting that the variations in geographical origins cannot explain the phylogenetic relationships among the 21 T. whipplei strains. The two Chinese strains were closely related to each other, and also found to be related to strains from Germany (T. whipplei TW08/27) and France (T. whipplei Bcu26 and T. whipplei Neuro1). Furthermore, the Average Nucleotide Identity (ANI) matrix also showed no association between geographic origins and genomic similarities. The pan-genome analysis revealed that T. whipplei has a closed pan-genome composed of big core-genomes and small accessory genomes, like other intracellular bacteria. By examining the genotypes of the sequenced strains, all 21 T. whipplei strains were found to be resistant to fluoroquinolones, due to the genetic mutations in genes gyrA, gyrB, parC, and parE. The 21 T. Whipplei strains shared the same virulence factors, except for the alpC gene, which existed in 7 out of the 21 T. whipplei strains. When comparing 21 entire T. whipplei pan-genomes from various nations, it was discovered that the bacterium also possessed a closed genome, which was a trait shared by intracellular pathogens.


Asunto(s)
Metagenoma , Tropheryma , Fluoroquinolonas , Genómica , Filogenia , Tropheryma/genética , Factores de Virulencia
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