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1.
Environ Sci Technol ; 58(21): 9456-9465, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38745405

RESUMO

The elimination of uranium from radioactive wastewater is crucial for the safe management and operation of environmental remediation. Here, we present a layered vanadate with high acid/base stability, [Me2NH2]V3O7, as an excellent ion exchanger capturing uranyl from highly complex aqueous solutions. The material possesses an indirect band gap, ferromagnetic characteristic and a flower-like morphology comprising parallel nanosheets. The layered structure of [Me2NH2]V3O7 is predominantly upheld by the H-bond interaction between anionic framework [V3O7]nn- and intercalated [Me2NH2]+. The [Me2NH2]+ within [Me2NH2]V3O7 can be readily exchanged with UO22+. [Me2NH2]V3O7 exhibits high exchange capacity (qm = 176.19 mg/g), fast kinetics (within 15 min), high removal efficiencies (>99%), and good selectivity against an excess of interfering ions. It also displays activity for UO22+ ion exchange over a wide pH range (2.00-7.12). More importantly, [Me2NH2]V3O7 has the capability to effectively remove low-concentration uranium, yielding a residual U concentration of 13 ppb, which falls below the EPA-defined acceptable limit of 30 ppb in typical drinking water. [Me2NH2]V3O7 can also efficiently separate UO22+ from Cs+ or Sr2+ achieving the highest separation factors (SFU/Cs of 589 and SFU/Sr of 227) to date. The BOMD and DFT calculations reveal that the driving force of ion exchange is dominated by the interaction between UO22+ and [V3O7]nn-, whereas the ion exchange rate is influenced by the mobility of UO22+ and [Me2NH2]+. Our experimental findings indicate that [Me2NH2]V3O7 can be considered as a promising uranium scavenger for environmental remediation. Additionally, the simulation results provide valuable mechanistic interpretations for ion exchange and serve as a reference for designing novel ion exchangers.


Assuntos
Urânio , Vanadatos , Urânio/química , Vanadatos/química , Troca Iônica , Poluentes Radioativos da Água/química , Cinética
2.
Langmuir ; 40(20): 10449-10459, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38717310

RESUMO

It is widely acknowledged that doping silicon can significantly enhance the friction performance of diamond-like carbon (DLC) films in a water environment. However, the mechanism of low friction caused by doped silicon is still highly controversial. Therefore, this article compares the interface interaction between DLC and Si-DLC films in a water environment through first-principles calculations of physisorption and chemisorption effects. The results indicate that water molecules are predominantly chemically adsorbed rather than physically adsorbed on the Si-DLC surface. Further study reveals that when OH-termination is formed on the Si-DLC surface, water molecules are predominantly physically adsorbed rather than chemically adsorbed on the Si-DLC hydroxylation surface. Consequently, a more stable hydration layer is formed on the surface through the hydrogen bond network formed by Si-OH groups, ultimately leading to lower friction. Moreover, molecular dynamics simulations further suggest that the lower friction coefficient of Si-DLC films in a water environment may be due to more water molecules at the friction interface and fewer interface covalent bonds. In short, the low-friction coefficient of the Si-DLC film in a water environment may be caused not only by the chemisorption of water molecules on its surface but also by the physisorption of water molecules on the Si-DLC film after surface hydroxylation.

3.
Inorg Chem ; 2024 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-38818647

RESUMO

Under xenon lamps, ZnFe2O4 (ZFO) has been shown to be effective in removing uranium through photocatalysis. However, its performance is still inadequate in low-light environments due to low photon utilization and high electron-hole complexation. Herein, S-doped hollow ZnFe2O4 microcubes (Sx-H-ZFO, x = 1, 3, 6, 9) were synthesized using the MOF precursor template method. The hollow morphology improves the utilization of visible light by refracting and reflecting the incident light multiple times within the confined domain. S doping narrows the band gap and shifts the conduction band position negatively, which enhances the separation, migration, and accumulation of photogenerated charges. Additionally, S doping increases the number of adsorption sites, ultimately promoting efficient surface reactions. Consequently, Sx-H-ZFO is capable of removing U(VI) in low-light environments. Under cloudy and rainy weather conditions, the photocatalytic rate of S3-H-ZFO was 100.31 µmol/(g·h), while under LED lamps (5000 Lux) it was 72.70 µmol/(g·h). More interestingly, a systematic mechanistic investigation has revealed that S doping replaces some of the oxygen atoms to enhance electron transfers and adsorption of O2. This process initiates the formation of hydrogen peroxide, which reacts directly with UO22+ to form solid studtite (UO2)O2·2H2O. Additionally, the promising magnetic separation capability of Sx-H-ZFO facilitates the recycling and reusability of the material. This work demonstrates the potential of ZnFe2O4 extraction uranium from nuclear wastewater.

4.
Small ; : e2401374, 2024 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-38659396

RESUMO

The removal of uranyl ions (UO2 2+) from water is challenging due to their chemical stability, low concentrations, complex water matrix, and technical limitations in extraction and separation. Herein, a novel molybdenum disulfide/graphene oxide heterojunction (MoS2/GO-H) is developed, serving as an effective electrode for capacitive deionization (CDI). By combining the inherent advantages of electroadsorption and electrocatalysis, an innovative electroadsorption-electrocatalysis system (EES) strategy is introduced. This system utilizes interface polarization at the MoS2 and GO interface, creating an additional electric field that significantly influences carrier behavior. The MoS2/GO-H electrode, with its extraordinary adsorption capacity of 805.57 mg g-1 under optimal conditions, effectively treated uranium-laden wastewater from a mine, achieving over 90% removal efficiency despite the presence of numerous competing ions at concentrations significantly higher than UO2 2+. Employing density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations, it is found that the MoS2/GO-H total charge density at the Fermi level, enhanced by interfacial polarization, surpasses that of separate MoS2 and GO, markedly boosting conductivity and electrocatalytic effectiveness.

5.
Inorg Chem ; 63(13): 5931-5944, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38490189

RESUMO

Piezoelectric-photocatalysis is distinguished by its piezoelectricity as an external force that induces deformation within the catalyst to engender a polarized electric field compared to conventional photocatalysis. Herein, the piezoelectric photocatalyst BiOBr has been expertly synthesized via a plasma process and applied for piezoelectric-photocatalysis removal of uranium(VI) for the first time. The abundant surface oxygen vacancies (OVs) could induce a dipole moment and built-in electric field, which endows BiOBr with excellent separation and transport efficiency of photogenerated charges to actuate more charges to participate in the piezoelectric-photocatalytic reduction process. Consequently, under visible light and ultrasound (150 W and 40 kHz), the removal rate constant of OVs-BiOBr-30 (0.0306 min-1) was 2.4, 30.6, and 6 times higher than those of BiOBr (0.01273 min-1), ultrasound, or photocatalysis, respectively. The piezoelectric-photocatalytic synergy is also universal for BiOX (X = Cl, Br, or I) to accelerate the reduction rate of uranium(VI). This work highlights the role of piezoelectric-photocatalysis in the treatment of uranium-containing wastewater, which is of great significance for resource conservation and environmental remediation.

6.
Inorg Chem ; 63(12): 5681-5688, 2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38484383

RESUMO

Three new POM-based compounds, with formulae [Na0.63Ag3(Htba)2.37(tba)0.63(H2O)2(PMo12O40)]·4H2O (Ag3PMo), [Ag4(Htba)4(H2O)2(PMo12O40)](NO3)·H2O (Ag4PMo), and [Ag3(Htba)2(tba)(PW12O40)0.5](NO3)0.5·13H2O (Ag3PW), were prepared with a 3-(4H-1,2,4-triazol-4-yl)benzoic acid (Htba) ligand, Keggin-type anions ([PMo12O40]3-/[PW12O40]3-), and a silver ion (Ag+). The structural features of these compounds are particularly different from the multinuclear subunits, which are [Ag3(tba)3] clusters in Ag3PMo, [Ag4(tba)3] chains in Ag4PMo, and [Ag3(tba)3]2 clusters in Ag3PW, connected by multidonor atom tba ligands and Ag+ ions. Meanwhile, in these compounds, polyanions act as polydentate ligands to link adjacent Ag-tba metal-organic units and expand their spatial dimensions. These compounds, as heterogeneous catalysts, exhibit high stability and excellent catalytic activity to construct benzimidazoles. Ag3PMo could efficiently catalyze the condensation of benzene-1,2-diamines and benzaldehydes and produce benzimidazoles in good yields. In addition, Ag3PMo could be reused up to 7 times and was suitable for gram-scale reactions.

7.
Environ Sci Pollut Res Int ; 31(14): 22073-22086, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38400975

RESUMO

Inspired by its large specific surface area, and tunable chemical and physical properties, a hollow carbon-based mater8ial derived from ZIF-8 with phosphate groups (HCM-PO4) was prepared for the elimination of U(VI). The structural and surface features of HCM and HCM-PO4 were thoroughly examined using techniques such as SEM, TEM, and XRD. The resulting carbon material, HCM-PO4, exhibits a higher BET surface area of 571.2 m2·g-1, featuring a hollow structure. The removal procedure of HCM-PO4 for U(VI) aligns with the quasi-secondary kinetic model. Furthermore, the theoretical sorption capacity of HCM-PO4 was found to be 482.30 mg·g-1 at 298.15 K. The results obtained from XPS, FT-IR, and EDS analysis of HCM-PO4 after adsorption revealed the coordination of the phosphate group for U(VI), contributing significantly to the adsorption process. In brief, the HCM-PO4 demonstrates excellent adsorptive ability, positioning it as a hopeful expectant to remove U(VI) from wastewater.


Assuntos
Carbono , Fosfatos , Adsorção , Espectroscopia de Infravermelho com Transformada de Fourier , Cinética
8.
Diabetes Metab Res Rev ; 40(2): e3766, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38351639

RESUMO

BACKGROUND: Evidence of the effects of metabolically healthy obesity (MHO) on atherosclerosis is limited; the transition effects of metabolic health and obesity phenotypes have been ignored. We examined the association between metabolic health and the transition to atherosclerosis risk across body mass index (BMI) categories in a community population. METHODS: This cross-sectional study was based on a national representative survey that included 50,885 community participants aged ≥40 years. It was conducted from 01 December 2017 to 31 December 2020, in 13 urban and 13 rural regions across Hunan China. Metabolic health was defined as meeting less than three abnormalities in blood pressure, glucose, high-density lipoprotein cholesterol, triglycerides, or waist circumference. The participants were cross-classified at baseline based on their metabolic health and obesity. In addition, the relationship between atherosclerosis and transitions in metabolic health status based on 4733 participants from baseline to the second survey after 2 years was considered. The relationship between metabolic health status and the risk of transition to Carotid atherosclerosis (CA) was assessed using logistic regression and Cox proportional hazards regression analyses. RESULTS: In this study, the mean age of the participants was 60.7 years (standard deviation [SD], 10.91), 53.0% were female, and 51.2% had CA. As compared with metabolically healthy normal weight (MHN), those with MHO phenotype (odd ratio [OR] 1.10, 95% confidence interval [CI] 1.02-1.21), metabolically unhealthy normal weight (OR 1.27, 95% CI 1.19-1.35), metabolically unhealthy overweight (OR 1.41, 95% CI 1.33-1.48), and metabolically unhealthy obese (OR 1.54, 95% CI 1.44-1.64) had higher risk for CA. However, during the follow-up of 2 years, almost 33% of the participants transitioned to a metabolically unhealthy status. As compared with stable healthy normal weight, transition from metabolically healthy to unhealthy status (hazard ratios [HR] 1.21, 95% [CI] 1.02-1.43) and stable metabolically unhealthy overweight or obesity (MUOO) (HR 1.32, 95% CI 1.17-1.48) were associated with higher risk of CA. CONCLUSIONS: In the community population, obesity remains a risk factor for CA despite metabolic health. However, the risks were highest for metabolically unhealthy status across all BMI categories. A large proportion of metabolically healthy overweight or participants with obesity converts to an unhealthy phenotype over time, which is associated with an increased risk of CA.


Assuntos
Aterosclerose , Doenças das Artérias Carótidas , Obesidade Metabolicamente Benigna , Humanos , Feminino , Pessoa de Meia-Idade , Masculino , Obesidade Metabolicamente Benigna/epidemiologia , Sobrepeso/complicações , Estudos Transversais , Obesidade/complicações , Obesidade/epidemiologia , Obesidade/metabolismo , Fatores de Risco , Índice de Massa Corporal , Nível de Saúde , Fenótipo , Doenças das Artérias Carótidas/epidemiologia , Doenças das Artérias Carótidas/etiologia , Aterosclerose/epidemiologia , Aterosclerose/etiologia
10.
Front Endocrinol (Lausanne) ; 14: 1266552, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37850101

RESUMO

Background: Several easily and inexpensively measured indicators of visceral adiposity dysfunction are currently available, but it remains unclear whether they are correlated with stroke risk in the community-dwelling population. We aimed to examine the longitudinal association of the triglyceridemic-waist phenotypes, the triglyceride glucose (TyG) index, as well as TyG-related indicators with stroke risk. Methods: In this study, we conducted a prospective cohort study in Hunan, a region located in Central China, where the prevalence of stroke is relatively high. We included a total of 20185 subjects aged ≥40 years between November 2017 and December 2018. Triglyceride glucose-body mass index (TyG-BMI) and triglyceride glucose-waist circumference (TyG-WC) were calculated as multiplying TyG index by BMI and WC, respectively. Triglyceride waist phenotypes were categorized into four phenotypes: HTGW (elevated triglyceride and enlarged WC), NTNW (normal triglyceride and normal WC); HTNW (high triglyceride and normal WC), and NTGW (normal triglyceride and enlarged WC). We constructed a multivariable Cox regression model to assess the association between these novel lipid indicators and the risk of stroke. Subgroup analysis was conducted to test the robustness of our research findings. ROC curve was used for assessing the predictive ability of different stroke risk indices. Results: After 2 years of follow- up, 135 participants experienced new stroke events. After adjusting for potential confounders, we found that participants with HTGW had higher likelihood of stroke (HR: 1.96, 95% CI: 1.21 to 3.16). However, we did not find significant associations for HTNW (HR: 1.42, 95% CI: 0.91 to 2.21) and NTGW (HR: 1.09, 95% CI 0.67 to 1.78). when compared to participants in the first TyG quartile, those in the fourth TyG quartile were associated with a 2.06-fold (95% CI: 1.22, 3.50) risk of stroke. Each 1-SD increase in TyG, TyG-BMI, and TyG-WC was associated with a higher risk of stroke, with adjusted HRs of 1.34 (95% CI: 1.11 to 1.61), 1.35 (95% CI: 1.14 to 1.59), and 1.23 (95% CI: 1.04 to 1.46), respectively. In subgroup analyses, those positive relationships appeared to be stronger among male participants with lower levels of physical activity and smoking. Conclusion: HTGW, along with higher levels of TyG and TyG-related indicators, were found to be associated with an elevated risk of stroke. HTGW and these novel lipid indicators might be reliable indicators to identify populations at elevated risk of stroke.


Assuntos
Obesidade , Acidente Vascular Cerebral , Humanos , Masculino , Estudos Prospectivos , Glucose , Acidente Vascular Cerebral/epidemiologia , Acidente Vascular Cerebral/etiologia , Triglicerídeos
11.
Langmuir ; 39(37): 13386-13398, 2023 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-37688790

RESUMO

Cuttings particles of different sizes in the drilling fluid are the leading cause of wear at the casing and drill pipe joints, and diamond-like carbon (DLC) films have excellent research potential in reducing tool wear due to their ultra-low friction coefficient and high wear resistance. In this paper, a corresponding molecular dynamics model was developed using LAMMPS to investigate the effect of silica particles of different particle sizes on the friction and wear mechanisms of Fe/DLC friction pairs at the microscale. The results show that small cuttings particles in a dry environment are more likely to cause interface wear between the casing and drill pipe joint, while in a water environment, the opposite is true. The main reason is that small particles in a dry environment have smaller contact areas and greater indentation depth, leading to greater wear at the friction interface. The movement of water molecules in the water environment will promote the composite movement of large particles, thereby exacerbating the wear of the interface. Moreover, the relevant research results at the micro-scale indicate that DLC films can effectively reduce wear, which provides theoretical support for its application in drill pipe joints.

12.
FASEB J ; 37(9): e23152, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-37603538

RESUMO

Umbilical cord-mesenchymal stem cells (UC-MSCs)-derived exosomes have been considered as an effective treatment for ischemic stroke. CircRNA BBS2 (circBBS2) was demonstrated to be down-regulated in patients with ischemic stroke. However, the role of UC-MSCs-derived exosomal circBBS2 in ischemic stroke and potential mechanisms remain unclear. Hypoxia/reperfusion (H/R)-exposed SH-SY5Y cells and middle cerebral artery occlusion (MCAO)-treated rats were served as in vitro and in vivo models of ischemic stroke. Target gene expression was detected by qRT-PCR. Cell viability was assessed by MTT assay. Ferroptosis was determined by iron, MDA, GSH, and lipid ROS levels. Protein levels were measured by Western blotting. The target relationships among circBBS2, miR-494, and SLC7A11 were validated by RNA-pull down, RIP, and dual-luciferase reporter assays. TTC and HE staining were performed to evaluate cerebral infarction volume and neuropathological changes. circBBS2 was lowly expressed and ferroptosis was triggered in MCAO rats and H/R-stimulated SH-SY5Y cells. UC-MSCs-derived exosomes enhanced cell viability and restrained ferroptosis via increasing circBBS2 expression in SH-SY5Y cells. Mechanistically, circBBS2 sponged miR-494 to enhance the SLC7A11 level. Knockdown of miR-494 or SLC7A11 reversed the effects of silencing circBBS2 or miR-494 on ferroptosis of SH-SY5Y cells, respectively. Furthermore, UC-MSCs-derived exosomes attenuated ischemic stroke in rats via delivering circBBS2 to inhibit ferroptosis. UC-MSCs-derived exosomal circBBS2 enhanced SLC7A11 expression via sponging miR-494, therefore repressing ferroptosis and relieving ischemic stroke. Our findings shed light on a novel mechanism for UC-MSCs-derived exosomes in the treatment of ischemic stroke.


Assuntos
Ferroptose , AVC Isquêmico , MicroRNAs , Neuroblastoma , Animais , Humanos , Ratos , Sistema y+ de Transporte de Aminoácidos/genética , Ferroptose/genética , Hipóxia , AVC Isquêmico/genética , MicroRNAs/genética , RNA Circular/genética
13.
J Hazard Mater ; 459: 132112, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37494797

RESUMO

Numerous efforts have been devoted to understanding the electron transfer process of uranium (UO22+) on adsorbent materials, whereas the potential oxygen vacancies (OVs) in metal oxides have long been overlooked. Once these interactions are taken into account, the emerging molecular orbital effects undoubtedly affect the adsorption process. Here, we synthesized CC/γ-MnO2 by growing MnO2 on carbon cloth (CC), followed by the creation of oxygen vacancies (OVs) through electrochemical methods to form CC/γ-MnO2-OVs. The CC/γ-MnO2-OVs shows significantly enhanced selectivity and durability for UO22+, with the maximum adsorption capacity increasing from 456.8 to 1648.1 mg/g (by a factor of 3.6). Theoretical calculations suggest that the generation of OVs leads to an increase in charge transfer and a decrease in adsorption energy between UO22+ and CC/γ-MnO2, due to the interaction between Mn 3d orbital in CC/γ-MnO2 and O 2p orbital in UO22+. The OVs in CC/γ-MnO2 provide a spatial structure for anchoring the OU=O moiety of UO22+, while the surface van der Waals forces and the formation of chemical bonds between Mn-U contribute to charge interactions. This synergistic effect allows CC/γ-MnO2-OVs to exhibit favorable selectivity, a large adsorption capacity, and rapid adsorption kinetics towards uranyl ions. This work achieves enhanced UO22+ separation by introducing OVs in CC/γ-MnO2 through a facile electrochemical strategy, highlighting the great potential for nuclear waste processing.

14.
J Hazard Mater ; 457: 131745, 2023 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-37295327

RESUMO

In order to deal with the sudden nuclear leakage event to suppress the spread of radioactive contaminants in a short period of time, it is extremely urgent needed to explore an adsorbent that could be capable of in-situ remedial actions to rapidly capture the leaked radionuclides in split second. An adsorbent was developed that MoS2 via ultrasonic to expose more surface defects afterwards functionalized by phosphoric acid resulting in more active sites being endowed on the edge S atoms of Mo-vacancy defects, while simultaneously increased the hydrophilicity and interlayer spacing. Hence, an overwhelming fast adsorption rates (adsorption equilibrium within 30 s) are presented and place the MoS2-PO4 at the top of performing sorbent materials. Moreover, the maximum capacity calculated from Langmuir model is as high as 354.61 mg·g-1, the selective adsorption capacity (SU) achieving 71.2% in the multi-ion system and with more than 91% capacity retention after 5 cycles of recycling. Finally, XPS and DFT insight into the adsorption mechanism, which can be explained as interaction of UO22+ on the surface of MoS2-PO4 by forming U-O and U-S bonds. The successful fabrication of such a material may provide a promising solution for emergency treatment of radioactive wastewater during nuclear leakage events.

15.
Inorg Chem ; 62(23): 8969-8979, 2023 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-37259837

RESUMO

Uranium-bearing wastewaters exert a great threat to the ecological environment due to its high radiotoxicity level. The designing and fabrication of novel adsorption materials can be promoted for radionuclide elimination from wastewater. In this work, results from density functional theory and Born-Oppenheimer molecular dynamics simulations are reported for the uranyl adsorption behavior on the MoS2/Mo2CTx heterostructure in the gas phase and in an aqueous environment. Uranyl ions prefer to be adsorbed at deprotonated O sites on the Mo2COH surface and S sites on the MoS2 side of the heterojunctions, resulting in the formation of bidentate configurations. In addition to coordination interaction, H-bond and van der Waals interactions can also play an important role in binding configurations. More importantly, the oxidation state U(VI) can be reduced to U(V) and then to U(IV) caused by the strong reducibility of the Mo2COH surface at room temperature, whereas the uranyl complex can move freely on the MoS2 surface. However, the coordination number of U with respect to H2O in the first hydration shell on the Mo2COH surface remains unchanged and is found to be 3, which is similar to that on the MoS2 surface. This work provides novel nanosorbents for the removal of uranyl from wastewater. The present viewpoint provides valuable mechanistic interpretations for uranyl adsorption and will give a supplement to the experimental research.

16.
Langmuir ; 39(14): 5145-5155, 2023 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-37010490

RESUMO

In this paper, the frictional behaviors of Fe-Cr alloys in the lubricating effect of oil-based lubricant are investigated through reactive molecular dynamics. It is shown that the oil-based lubricant achieves ultralow friction through hydrodynamic lubrication by linear alpha olefin (C8H16) and passivation of the friction pairs by hydrogen gas (H2) and free H atoms generated by the friction chemistry. Moreover, there is a critical value for the transition of the crystal structure of Fe-Cr alloy from body-centered cubic (Bcc) to amorphous structure (Other), leading to a dramatic change in friction. Meanwhile, a sliding interface consisting of a large number of amorphous structures is formed near the rigid layer, which keeps the friction force stable.

17.
J Hazard Mater ; 452: 131248, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-36963194

RESUMO

Effective spatial separation and utilization of photogenerated charges are critical for photocatalysis process. Herein, novel Co3O4 @TiO2 @CdS@Au double-shelled nanocage (CTCA) with spatially separated redox centers was synthesized by loading Co3O4 and Au NP cocatalysts on the inner and outer surfaces of Z-scheme heterojunction (TiO2 @CdS). The reduction rate constant of U(VI) by CTCA reached 0.218 min-1 under simulated sunlight irradiation, which was 6.6, 3.2 and 36.3 times than that of monolayer CTCA (0.033 min-1), CTC (0.068 min-1) and CT (0.006 min-1). The full-spectrum light-assisted photothermal catalytic performance can enable CTCA to remove 98.8% of U(VI) and degrade nearly 90% of five organic pollutants simultaneously. Detailed characterizations and theory calculations revealed that the photogenerated holes and electrons in CTCA flow inward and outward. More importantly, Co3O4 acts as a "nano heater" to generate the photothermal effect for further enhancing the charge transfer and accelerating the surface reaction kinetics. Meanwhile, the photogenerated electrons and superoxide radicals play a dominant role in reducing the adsorbed U(VI) to insoluble (UO2)O2·2H2O(s). This work provides valuable input toward a novel double-shelled hollow nanocage reactor with excellent photothermal catalysis ability for efficient recovery U(VI) from uranium mine wastewater to address environmental contamination issues.

18.
FASEB J ; 37(3): e22733, 2023 03.
Artigo em Inglês | MEDLINE | ID: mdl-36723877

RESUMO

Accumulating evidence suggests that human umbilical cord mesenchymal stem cell-derived exosomes (hUC-MSCs-Exos) are a promising therapeutic strategy for cerebral ischemia-reperfusion injury (CIRI). However, the underlying mechanism remains unclear. hUC-MSCs-Exos were identified by electron microscopy, NTA, and Western blotting. In the hypoxia/reoxygenation (H/R) cell model, human brain microvascular endothelial cells (HBMECs) were cocultured with hUC-MSCs-Exos. Then, cell viability, migration, apoptosis, and tube formation were measured by MTT, flow cytometry, transwell, and tube formation assays. RT-qPCR and Western blotting were used to detect the changes in RNA and protein. RNA pull-down and dual luciferase reporter assays confirmed the relationship between circDLGAP4, miR-320, and KLF5. Ischemia-reperfusion (I/R) rat model was established for in vivo experiments. hUC-MSCs-Exos increased the expression levels of circDLGAP4 and KLF5 but decreased miR-320 in H/R-treated HBMECs by transferring exosomal circDLGAP4. Knockdown of circDLGAP4 in hUC-MSCs-Exos reversed the promoting effects of hUC-MSCs-Exos on cell viability, migration, and tube formation in H/R-treated HBMECs in vitro and also abolished the protective effects of hUC-MSCs-Exos on cerebrovascular injury in I/R rats. Mechanistically, exosomal circDLGAP4 negatively regulated miR-320 in HBMECs, which directly bound to KLF5. In addition, the downregulation of miR-320 could reverse the regulatory effect of exosomal shcircDLGAL5 in H/R-treated HBMECs by upregulating KLF5. hUC-MSCs-Exos-derived circDLGAP4 reduced cerebrovascular injury by regulating miR-320/KLF5 signaling. These results provide a stem cell-based approach to treat CIRI.


Assuntos
Exossomos , Células-Tronco Mesenquimais , MicroRNAs , Traumatismo por Reperfusão , Humanos , Ratos , Animais , MicroRNAs/genética , MicroRNAs/metabolismo , Células Endoteliais/metabolismo , Traumatismo por Reperfusão/genética , Traumatismo por Reperfusão/metabolismo , Células-Tronco Mesenquimais/metabolismo , Cordão Umbilical/metabolismo , Exossomos/genética , Exossomos/metabolismo , Fatores de Transcrição Kruppel-Like/genética , Fatores de Transcrição Kruppel-Like/metabolismo
19.
Small ; 19(20): e2300003, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36807523

RESUMO

Designing highly efficient photocatalysts with rapid migration of photogenerated charges and surface reaction kinetics for the photocatalytic removal of uranium (U(VI)) from uranium mine wastewater remains a significant challenge. Inspired by natural photosynthesis, a biomimetic photocatalytic system is assembled by designing a novel hollow nanosphere MnOx @TiO2 @CdS@Au (MTCA) with loading MnOx and Au nano particles (Au NPs) cocatalysts on the inner and outer surfaces of the TiO2 @CdS. The spatially separated cocatalysts efficiently drive the photogenerated charges to migrate in opposite directions, while the Z-scheme heterogeneous shell further separates the interfacial charges. Theoretical calculation identifies multiple consecutive forward charge transfers without charge recombination within MTCA. Thus, MTCA could efficiently remove 99.61% of U(VI) after 15 min of simulated sunlight irradiation within 3 mmol L-1 NaHCO3 with 0.231 min-1 of the reduction rate constant, outperforming most previously reported photocatalysts. MTCA further significantly removes 91.83% of U(VI) from the natural uranium mining wastewater under sunlight irradiation. This study provides a novel approach to designing an ideal biomimetic photocatalyst for remediating environmental pollution.

20.
Langmuir ; 39(5): 1905-1913, 2023 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-36700881

RESUMO

Whether a graphitization mechanism can control the low-friction behavior of DLC films is still controversial. In this paper, we establish the molecular dynamics model of the DLC film with graphene (DLC-GR-DLC) by LAMMPS and study the influence of the graphitization mechanism on the friction and wear behavior of the DLC film. The friction force of the DLC-GR-DLC model in the running-in stage is significantly smaller than that of the DLC film and then gradually increases to the same size as that of the DLC film. Further analysis indicates that the graphitization mechanism could indeed reduce the shear stress of the friction interface when graphene remains intact. However, the curling and breaking of the graphene structure will lead to an increase in shear force at the friction interface.

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