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1.
Small ; : e2406377, 2024 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-39370574

RESUMO

The production of bacterial toxins and excessive accumulation of reactive oxygen species (ROS) can induce localized oxidative stress, triggering an exaggerated immune response that impedes wound healing and culminates in chronic wounds. To address this issue, a microneedle (MN) system loaded with copper-manganese oxide (CMO) is developed to modulate the hyperimmune response in wounds. CMO@MN exhibits excellent antimicrobial and anti-inflammatory properties by effectively killing bacteria, scavenging ROS, and modulating macrophage polarization through their multiple enzymatic activities and photothermal properties. RNA sequencing revealed that CMO@MN improved the therapeutic effect on the infected skin of mice by balancing the ratio of M1/M2 macrophages and promoting cell migration and angiogenesis through the regulation of relevant pathways. Overall, this CMO@MN patch skillfully balances the complex issues between the immune response and wound healing and has potential applications in the treatment of other serious bacterial infections.

2.
Br J Haematol ; 2024 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-39367620

RESUMO

Due to the limited real-world research on the application of avatrombopag (AVA) for immune thrombocytopenia (ITP) in China, we evaluated the effectiveness and safety of AVA in clinical practice. We included 121 adult ITP patients treated with AVA across three medical centres. Based on the reasons for choosing AVA, these patients were divided into eltrombopag (ELT)/hetrombopag (HET) intolerance group (IG), and ELT/HET unresponsive group (UG). Compared with UG, more patients in IG had a history of liver disease and received fewer treatments before AVA. Amongst all patients, 83% had platelet response (≥30 × 109/L) after AVA and 62% achieved complete response (≥100 × 109/L, CR). Sixty-two percent in IG and 56% in UG were able to discontinue more than one concomitant ITP medication. A total of 17 patients underwent multiple switches of thrombopoietin receptor agonists (TPO-RAs), resulting in an 88% platelet response rate. Sixty-three patients discontinued AVA, 27% were due to unaffordability. AVA was well tolerated in most patients. In the ITP population, AVA proved effective and safe, particularly in patients intolerant or unresponsive to ELT/HET. Patients benefited from TPO-RAs switches, particularly those undergoing multiple switches. However, many patients struggled with the long-term financial burden of AVA.

3.
J Hazard Mater ; 480: 136130, 2024 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-39405718

RESUMO

Wastewater acts as a significant sink and source of per- and polyfluoroalkyl substances (PFAS). This study investigated the occurrence, removal and mass flow of 48 emerging and legacy PFAS in 8 domestic and general industrial wastewater treatment plants (WWTPs) throughout entire treatment processes. In wastewater and sludge, 24 and 26 PFAS were detected, with concentrations of 246-27,100 ng/L and 91.6-214 ng/g, respectively. Predominant substances included 2H,2H-perfluorooctanoic acid (6:2 FTCA), 2H,2H-perfluorododecanoic acid (10:2 FTCA), and perfluorooctanoic acid (PFOA). Novel alternatives such as hexafluoropropylene oxide dimer acid (GenX) were not detected. Removal efficiency of total PFAS was 1-46 % in domestic WWTPs but negative in industrial WWTPs, with one industrial WWTP showing a 27-fold increase due to 6:2 FTCA generation. Median removal efficiency revealed that 9 out of 13 major PFAS decreased after treatment, while 4 increased. PFAS with -CH2- group showed weaker sludge sorption compared to those with perfluorinated carbon chains. Mass flow analysis revealed wastewater is the major fate rather than sludge for emerging PFAS. Increased mass flows of fluorotelomer carboxylic acids (FTCAs) and perfluorobutanesulfonic acid (PFBS) were observed at biochemical treatment and disinfection. The ecological risk assessment using a relative risk ranking model identified higher risks from PFBS, polyfluoroalkyl phosphate mono-esters, and FTCAs. Emerging PFAS pose challenges in removal and greater hazards to ecosystems, necessitating careful evaluation and restriction to address their risk.

4.
Bull Environ Contam Toxicol ; 113(4): 51, 2024 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-39394363

RESUMO

Both ibuprofen (IBP) and chlorophene (CP) are frequently detected contaminants in surface aqueous environment. Dissolved organic matter (DOM) is an important component in water with high photo-reactivity, playing an important role in the transformation processes of various organic pollutants. This study systematically studied the influence of DOM on the photochemical transformation of IBP and CP by using humic acid as model DOM. In addition, the effect of inorganic salts on this process is also considered due to the high salt content in the ocean. Further quenching experiments and reactive oxygen species (ROSs) detection were also conducted to explore the reactive species acting on the IBP and CP transformation. Based on the products analysis and theoretical calculation, we proposed the IBP and CP transformation mechanism. Overall, this study provides some new insights into the transformation of organic pollutants in natural surface water, which is significant for assessing the fate of pollutants.


Assuntos
Substâncias Húmicas , Ibuprofeno , Poluentes Químicos da Água , Ibuprofeno/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Substâncias Húmicas/análise , Processos Fotoquímicos , Diclorofeno/química , Espécies Reativas de Oxigênio/química
5.
Cell Signal ; 124: 111399, 2024 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-39251054

RESUMO

BACKGROUND: Osteoarthritis (OA) is a prevalent ailment characterized by the gradual degradation of joints, resulting in discomfort and restricted movement. The recently proposed mechanism of ferroptosis is intricately associated with the initiation and progression of OA. Our study found that the long non-coding RNA HOXA11-AS reduces ferroptosis by increasing the expression of SLC3A2 through the transcription factor POU2F2. MATERIALS AND METHODS: HOXA11-AS was identified through lncRNA microarray analysis, and its impact on chondrocytes and extracellular matrix was assessed using real-time quantitative PCR, western blotting, and CCK8 assays. Subsequently, overexpression of HOXA11-AS in the knee joints of mice confirmed its protective efficacy on chondrocyte phenotype in the OA model. The involvement of HOXA11-AS in regulating ferroptosis via SLC3A2 was further validated through RNA sequencing analysis of mouse cartilage and the assessment of malondialdehyde levels and glutathione peroxidase activity. Finally, a combination of RNA sequencing, pull-down assays, mass spectrometry (MS), and chromatin immunoprecipitation (ChIP) techniques was employed to identify POU2F2 as the crucial transcription factor responsible for repressing the expression of SLC3A2, which can be effectively inhibited by HOXA11-AS. RESULTS: Our study demonstrated that HOXA11-AS effectively enhanced the metabolic homeostasis of chondrocytes, and alleviated the progression of OA in vitro and in vivo experiments. Furthermore, HOXA11-AS was found to enhance SLC3A2 expression, a key regulator of ferroptosis, by interacting with the transcriptional repressor POU2F2. CONCLUSIONS: HOXA11-AS promotes SLC3A2 expression and inhibits chondrocyte ferroptosis, by binding to the transcriptional repressor POU2F2, offering a promising and innovative therapeutic approach for OA.

6.
Phytomedicine ; 135: 156048, 2024 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-39326132

RESUMO

BACKGROUND: Ulcerative colitis (UC) is a type of inflammatory bowel disease primarily affecting the colon and rectum. The clinical symptoms of UC include persistent diarrhea, abdominal pain, and rectal bleeding, with chronic inflammation often limited to the mucosal layer of the colon. Macrophages play a significant role in the pathogenesis of UC in response to the presence of gut microbiota. Puerarin is an active compound derived from the root of pueraria lobata, a traditional Chinese herbal medicine, and exhibits potent anti-inflammatory properties in various diseases and disease models including UC-like colitis in mice. However, how the molecule achieves its therapeutic effect in colitis by re-polarizing macrophages remains poorly understood. PURPOSE: Utilizing in vivo and in vitro experimental methods along with multi-omics analysis, we aimed to elucidate the potential mechanism by which puerarin targets macrophages to treat colitis. METHODS: The inflammation induced by DSS was assessed both locally in the gut and systemically, and the anti-inflammatory effect of puerarin was evaluated using molecular and histological assays such as H&E staining, qPCR, ELISA, Western blot, and immunofluorescence. Intestinal permeability parameters were measured by in vivo imaging, immunofluorescence, Western blot, qPCR, and PAS staining. The central role of macrophages in colitis was investigated through macrophage depletion/infusion using cytological methods. The direct effects of puerarin on the macrophages were examined by CCK8, flow cytometry, and qPCR in vitro. Additionally, 16S rRNA sequencing and metabolomics analysis of gut contents were conducted. Identification of key pathogenic flora was facilitated by a trans-omic approach and validated both in vitro and in vivo. RESULTS: Puerarin exerted a direct and robust suppression of M1-like polarization of macrophages in vitro, which was sufficient to confer therapeutic benefits in terms of colonic lesions and systemic inflammation in DSS mice. Puerarin also reduced the abundance of Akkermansia muciniphila in the gut, which was significantly upregulated in DSS mice in our experimental context. Further study demonstrated that puerarin effectively suppressed M1-like macrophage activation induced by Akkermansia muciniphila secreted protein Amuc_2172, thereby altering the pathology in the DSS model. CONCLUSION: Our data suggest that the pathogenesis of DSS colitis is mediated by host cellular responses to toxic foreign molecules and the gut microbiota, and targeting specific cell populations, such as macrophages, with puerarin holds potential therapeutic value.

7.
Water Res ; 265: 122277, 2024 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-39167974

RESUMO

Perfluorinated alkylated substances (PFAS), as a category of persistent organic pollutants, have garnered extensive concern due to their resilience against environmental degradation. Herein, we developed an amine-functionalized sphalerite (ZnS) with adjustable surface amine functional groups and Zn defects (ZnS-X%[N]) by in situ coprecipitation and simple hydrothermal method in the presence of cetyltrimethylammonium bromide (CTAB). This material demonstrated efficient PFAS adsorption and subsequent photo-induced degradation under UV irradiation. The characterization results by TEM, BET, FTIR, XPS and EPR revealed that CTAB primarily influences ZnS by modulating surface amine functionalities, zinc defect density, and enhancing its photoreductive capacity. Adsorption and kinetic degradation experiments further showed that a medium CTAB concentration in ZnS-40%[N] achieves highest PFAS adsorption capacity (Cmax: 0.201 mol kg-1), and the corresponding decomposition rate was the fastest (kde: 1.53; kdf: 1.19). This efficacy is attributed to the ZnS-40%[N]'s ideal adsorptive sites and surface shallow defects. Moreover, theoretical simulation also supports the above experimental inference. Overall, ZnS-X%[N] exhibits a synergistic effect on PFAS adsorption and degradation, showcasing its potential for environmental adaptability and practical application.


Assuntos
Caprilatos , Fluorocarbonos , Raios Ultravioleta , Poluentes Químicos da Água , Adsorção , Fluorocarbonos/química , Caprilatos/química , Poluentes Químicos da Água/química , Aminas/química , Compostos de Zinco/química , Cinética
8.
Orthop Surg ; 2024 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-39107882

RESUMO

OBJECTIVE: Posterior condylar offset (PCO) and anterior condylar offset (ACO) exert an influence on the sagittal alignment in total knee arthroplasty (TKA). However, there is no common consensus that the variation range of posterior condylar offset (PCO) is associated with patient-reported outcome measures (PROMs) and the optimum variation range of PCO. This study aims to investigate the correlation between PCO and the PROMs of primary TKA for osteoarthritis (OA) and find out the optimal variation range of the PCO. METHODS: In this study, we performed a radiographic analysis of 106 patients (112 knees) with primary TKA. Patients were divided into two cohorts (A and B) according to the Western Ontario and McMaster Universities Osteoarthritis index (WOMAC). Correlations between the sagittal parameter and WOMAC were investigated using univariate and multivariate analysis. The receiver operating characteristic (ROC) curve was used to establish the cut-off value for the optimal variation range. We then further investigated how different variation range affects the WOMAC subscale score and forgotten-joint-score-12 (FJS-12). RESULTS: Univariate analysis revealed a correlation between the variation range of PCO (p < 0.01), ACO (p < 0.01) and PROMs. Multivariate analysis showed that only PCO was associated with PROMs. In the ROC graph, the cut-off value of the variation range of PCO is 2.85 mm (AUC = 0.66, Youden index = 0.26). The WOMAC functional ability score of the group outside the PCO variation range of 2.85 mm significantly increased compared to the group within the range. CONCLUSION: In this study, PCO variation was significantly associated with clinical outcomes in TKA and the optimal PCO variation range was within 2.85 mm. Maintaining the PCO variation within 2.85 mm could enhance functional recovery and patient satisfaction.

11.
Nat Commun ; 15(1): 6102, 2024 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-39030211

RESUMO

Visible-light photocatalysis has evolved as a powerful technique to enable controllable radical reactions. Exploring unique photocatalytic mode for obtaining new chemoselectivity and product diversity is of great significance. Herein, we present a photo-induced chemoselective 1,2-diheteroarylation of unactivated alkenes utilizing halopyridines and quinolines. The ring-fused azaarenes serve as not only substrate, but also potential precursors for halogen-atom abstraction for pyridyl radical generation in this photocatalysis. As a complement to metal catalysis, this photo-induced radical process with mild and redox neutral conditions assembles two different heteroaryl groups into alkenes regioselectively and contribute to broad substrates scope. The obtained products containing aza-arene units permit various further diversifications, demonstrating the synthetic utility of this protocol. We anticipate that this protocol will trigger the further advancement of photo-induced alkyl/aryl halides activation.

12.
Exp Cell Res ; 439(2): 114111, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38823471

RESUMO

Skeletal muscle ischemia-reperfusion (IR) injury poses significant challenges due to its local and systemic complications. Traditional studies relying on two-dimensional (2D) cell culture or animal models often fall short of faithfully replicating the human in vivo environment, thereby impeding the translational process from animal research to clinical applications. Three-dimensional (3D) constructs, such as skeletal muscle spheroids with enhanced cell-cell interactions from human pluripotent stem cells (hPSCs) offer a promising alternative by partially mimicking human physiological cellular environment in vivo processes. This study aims to establish an innovative in vitro model, human skeletal muscle spheroids based on sphere differentiation from hPSCs, to investigate human skeletal muscle developmental processes and IR mechanisms within a controlled laboratory setting. By eticulously recapitulating embryonic myogenesis through paraxial mesodermal differentiation of neuro-mesodermal progenitors, we successfully established 3D skeletal muscle spheroids that mirror the dynamic colonization observed during human skeletal muscle development. Co-culturing human skeletal muscle spheroids with spinal cord spheroids facilitated the formation of neuromuscular junctions, providing functional relevance to skeletal muscle spheroids. Furthermore, through oxygen-glucose deprivation/re-oxygenation treatment, 3D skeletal muscle spheroids provide insights into the molecular events and pathogenesis of IR injury. The findings presented in this study significantly contribute to our understanding of skeletal muscle development and offer a robust platform for in vitro studies on skeletal muscle IR injury, holding potential applications in drug testing, therapeutic development, and personalized medicine within the realm of skeletal muscle-related pathologies.


Assuntos
Diferenciação Celular , Músculo Esquelético , Células-Tronco Pluripotentes , Traumatismo por Reperfusão , Esferoides Celulares , Humanos , Traumatismo por Reperfusão/patologia , Traumatismo por Reperfusão/metabolismo , Músculo Esquelético/citologia , Células-Tronco Pluripotentes/citologia , Células-Tronco Pluripotentes/metabolismo , Esferoides Celulares/citologia , Desenvolvimento Muscular , Técnicas de Cocultura/métodos , Células Cultivadas , Técnicas de Cultura de Células/métodos
13.
J Am Chem Soc ; 146(22): 15479-15487, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38780095

RESUMO

The development of efficient and low-cost catalysts is essential for photocatalysis; however, the intrinsically low photocatalytic efficiency as well as the difficulty in using and recycling photocatalysts in powder morphology greatly limit their practical performance. Herein, we describe quasi-homogeneous photocatalysis to overcome these two limitations by constructing ultrastiff, hierarchically porous, and photoactive aerogels of conjugated microporous polymers (CMPs). The CMP aerogels exhibit low density but high stiffness beyond 105 m2 s-2, outperforming most low-density materials. Extraordinary stiffness ensures their use as robust scaffolds for scaled photocatalysis and recycling without damage at the macroscopic level. A challenging but desirable reaction for direct deaminative borylation is demonstrated using CMP aerogel-based quasi-homogeneous photocatalysis with gram-scale productivity and record-high efficiency under ambient conditions. Combined terahertz and transient absorption spectroscopic studies unveil the generation of high-mobility free carriers and long-lived excitonic species in the CMP aerogels, underlying the observed superior catalytic performance.

14.
J Colloid Interface Sci ; 670: 323-336, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38763028

RESUMO

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.

15.
Case Rep Infect Dis ; 2024: 7219952, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38737750

RESUMO

Over 200 different serogroups of Vibrio cholerae based on O-polysaccharide specificity have been described worldwide, including the two most important serogroups, O1 and O139. Non-O1/non-O139 V. cholerae serogroups generally do not produce the cholera-causing toxin but do sporadically cause gastroenteritis and extra-intestinal infections. Recently, however, bloodstream infections caused by non-O1/non-O139 V. cholerae are being increasingly reported, and these infections are associated with high mortality in immunocompromised hosts. We describe a case of non-O1/non-O139 V. cholerae bacteremia in a patient with autoimmune pancreatitis and stenosis of the intra- and extrahepatic bile ducts. The clinical manifestations of bacteremia were fever and mild digestive symptoms. The blood cultures showed V. cholerae, which was identified as a non-O1, non-O139 serogroup by slide agglutination tests and PCR. The bloodstream infection of the patient was likely caused by the consumption of contaminated seafood at a banquet. The patient recovered after the administration of a third-generation cephalosporin. Non-O1/non-O139 V. cholerae infection presents with or without gastrointestinal manifestations; close attention should be paid to the possibility of disseminated non-O1/non-O139 V. cholerae infection in high-risk patients.

16.
J Am Chem Soc ; 2024 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-38728652

RESUMO

Porous organic polymers (POPs) with inherent porosity, tunable pore environment, and semiconductive property are ideally suitable for application in various advanced semiconductor-related devices. However, owing to the lack of processability, POPs are usually prepared in powder forms, which limits their application in advanced devices. Herein, we demonstrate an example of information storage application of POPs with film form prepared by an electrochemical method. The growth process of the electropolymerized films in accordance with the Volmer-Weber model was proposed by observation of atomic force microscopy. Given the mechanism of the electron transfer system, we verified and mainly emphasized the importance of porosity and interfacial properties of porous polymer films for memristor. As expected, the as-fabricated memristors exhibit good performance on low turn-on voltage (0.65 ± 0.10 V), reliable data storage, and high on/off current ratio (104). This work offers inspiration for applying POPs in the form of electropolymerized films in various advanced semiconductor-related devices.

17.
Nat Commun ; 15(1): 2898, 2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38575596

RESUMO

Selective molecular recognition is an important alternative to the energy-intensive industrial separation process. Porous coordination polymers (PCPs) offer designing platforms for gas separation because they possess precise controllability over structures at the molecular level. However, PCPs-based gas separations are dominantly achieved using strong adsorptive sites for thermodynamic recognition or pore-aperture control for size sieving, which suffer from insufficient selectivity or sluggish kinetics. Developing PCPs that work at high temperatures and feature both high uptake capacity and selectivity is urgently required but remains challenging. Herein, we report diffusion-rate sieving of propylene/propane (C3H6/C3H8) at 300 K by constructing a PCP material whose global and local dynamics cooperatively govern the adsorption process via the mechanisms of the gate opening for C3H6 and the diffusion regulation for C3H8, respectively, yielding substantial differences in both uptake capacity and adsorption kinetics. Dynamic separation of an equimolar C3H6/C3H8 mixture reveals outstanding sieving performance with a C3H6 purity of 99.7% and a separation factor of 318.

18.
J Hazard Mater ; 470: 134213, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38613958

RESUMO

Manganese oxides (MnO2) are commonly prevalent in groundwater, sediment and soil. In this study, we found that oxalate (H2C2O4) dissolved MnO2, leading to the formation of Mn(II)/(III), CO2(aq) and reactive oxygen species (·CO2-/O2·-/H2O2/·OH). Notably, CO2(aq) played a crucial role in ·OH formation, contributing to the degradation of atrazine (ATZ). To elucidate underneath mechanisms, a series of reactions with different gas-liquid ratios (GLR) were conducted. At the GLR of 0.3, 3.76, and + ∞ 79.4 %, 5.32 %, and 5.28 % of ATZ were eliminated, in which the cumulative ·OH concentration was 39.6 µM, 8.11 µM, and 7.39 µM and the cumulative CO2(aq) concentration was 11.2 mM, 4.7 mM, and 2.8 mM, respectively. The proposed reaction pathway was that CO2(aq) participated in the formation of a ternary complex [C2O4-Mn(II)-HCO4·3 H2O]-, which converted to a transition state (TS) as [C2O4-Mn(II)-CO3-OH·3 H2O]-, then decomposed to a complex radical [C2O4-Mn(II)-CO3·3 H2O]·- and ·OH after electron transfer within TS. It was novel to discover the role of CO2(aq) for ·OH yielding during MnO2 dissolution by H2C2O4. This finding helps revealing the overlooked processes that CO2(aq) influenced the fate of ATZ or other organic compounds in environment and providing us ideas for new technique development in contaminant remediation. ENVIRONMENTAL IMPLICATION: Manganese oxides and oxalate are common in soil, sediment and water. Their interactions could induce the formation of Mn(II)/(III), CO2(aq) and ·CO2-/O2·-/H2O2. This study found that atrazine could be effectively removed due to ·OH radicals under condition of high CO2(aq) concentration. The concentrations of Mn (0.0002-8.34 mg·L-1) and CO2(aq) (15-40 mg·L-1) were high in groundwater, and the surface water or rainfall seeps into groundwater and bring organic acids, which might promote the ·OH formation. The results might explain the missing steps of herbicides transformation in these environments and be helpful in developing new techniques in remediation in future.

19.
Sci Total Environ ; 927: 172468, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38615762

RESUMO

Aqueous trivalent manganese [Mn(III)], an important reactive intermediate, is ubiquitous in natural surface water containing humic acid (HA). However, the effect of low-molecular-weight organic acids (LMWOAs) on the formation, stability and reactivity of Mn(III) intermediate is still unknown. In this study, six LMWOAs, including oxalic acid (Oxa), salicylic acid (Sal), catechol (Cat), caffeic acid (Caf), gallic acid (Gal) and ethylene diamine tetraacetic acid (EDTA), were selected to investigate the effects of LMWOAs on the degradation of BPA induced by in situ formed Mn(III)-L in the HA/Mn(II) system under light irradiation. The chromophoric constituents of HA could absorb light radiation and generate superoxide radical to promote the oxidation of Mn(II) to form Mn(III), which was further involved in transformation of BPA. Our results implied that different LMWOAs did significantly impact on Mn(III) production and its degradation of BPA due to their different functional group. EDTA, Oxa and Sal extensively increased the Mn(III) concentration from 50 to 100 µM compared to the system without LMWOAs, following the order of EDTA > Oxa > Sal, and also enhanced the degradation of BPA with the similar patterns. In contrast, Cat, Caf and Gal had an inhibitory effect on the formation of Mn(III), which is likely because they consumed the superoxide radicals generated from irradiated HA, resulting in the inhibition of Mn(II) oxidation and further BPA removal. The product identification and theoretical calculation indicated that a single electron transfer process occurred between Mn(III)-L and BPA, forming BPA radicals and subsequent self-coupling products. Our results demonstrated that the LMWOAs with different structures could alter the cycling process of Mn via complexation and redox reactions, which would provide new implications for the removal of organic pollutants in surface water.

20.
Angew Chem Int Ed Engl ; 63(19): e202402440, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38426574

RESUMO

Perfluoroalkyl substances (PFASs) are persistent and toxic to human health. It is demanding for high-efficient and green technologies to remove PFASs from water. In this study, a novel PFAS treatment technology was developed, utilizing polytetrafluoroethylene (PTFE) particles (1-5 µm) as the catalyst and a low frequency ultrasound (US, 40 kHz, 0.3 W/cm2) for activation. Remarkably, this system can induce near-complete defluorination for different structured PFASs. The underlying mechanism relies on contact electrification between PTFE and water, which induces cumulative electrons on PTFE surface, and creates a high surface voltage (tens of volts). Such high surface voltage can generate abundant reactive oxygen species (ROS, i.e., O2⋅-, HO⋅, etc.) and a strong interfacial electrostatic field (IEF of 109~1010 V/m). Consequently, the strong IEF significantly activates PFAS molecules and reduces the energy barrier of O2⋅- nucleophilic reaction. Simultaneously, the co-existence of surface electrons (PTFE*(e-)) and HO⋅ enables synergetic reduction and oxidation of PFAS and its intermediates, leading to enhanced and thorough defluorination. The US/PTFE method shows compelling advantages of low energy consumption, zero chemical input, and few harmful intermediates. It offers a new and promising solution for effectively treating the PFAS-contaminated drinking water.

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