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1.
Environ Sci Technol ; 2020 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-32186173

RESUMO

A novel Fenton-like catalyst was synthesized by immobilizing nano-Fe2O3 (nFe2O3) on MIL-53(Cu). The pseudo-first order rate constant of bisphenol A degradation in nFe2O3/MIL-53(Cu)/H2O2 system reached 0.0123 min-1, while the values in MIL-53(Cu)/H2O2 and nFe2O3/H2O2 systems were only 0.0026 and 0.0040 min-1, respectively. Characterization of nFe2O3/MIL-53(Cu) reveals that the supreme catalytic activity of this material could be ascribed to iron-copper synergy, smaller size and better dispersion of nFe2O3 particles. Moreover, a method of trapping Cu(I) by neocuproine was developed, which could shield Cu(I) from interacting with iron and H2O2, thus allow the quantitative distinguish of the contribution to the enhanced catalytic activity by each of the factors. Using this method, 19% of the enhancement was determined to be contributed by synergistic effect, while 24% of the enhancement was due to smaller size and better dispersion of the nFe2O3 particles on MIL-53(Cu) support. In addition, the performance of nFe2O3/MIL-53(Cu) only dropped slightly after 5 treatment cycles, showing good potential in practical application. We believe this study sheds light on tailor-design of Fenton-like catalysts and elucidating catalytic mechanisms of supported bimetallic catalysts.

2.
Water Res ; 173: 115596, 2020 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-32062228

RESUMO

Selective reduction of nitrate to N2 is attractive but still a difficult challenge in the water treatment field. Herein, we established a flow-through electrochemical system packed with polymeric beads supported nZVI (nZVI@D201) for selective nitrate reduction. Consequently, efficient nitrate reduction in the flow mode was achieved on nZVI@D201 under electrochemical regulation with N2 selectivity of up to 95% for at least 60 h. Otherwise, nZVI was gradually exhausted after 20 h, and the product was mainly the undesired NH4+. Through a series of comparative experiments, we clarified that the enhanced nitrate reduction on nZVI under electrochemical regulation was mainly attributed to electrons (from cathode) and active hydrogen ([H]) rather than the previously speculated H2. Combining the characterizations of nZVI during nitrate reduction by X-ray diffraction and X-ray photoelectron spectrometry, we found that nitrate reduction under electrochemical regulation was mediated by nZVI along with the resultant Fe0@FexOy-Fe(II) structure and was sustained by electrons (from cathode) and [H] via the in situ reduction of Fe(III) back to Fe(II). Meanwhile, the undesirable product NH4+ was efficiently oxidized to N2 by the active chlorine generated on the anode. This study not only clarifies the mechanism of enhanced nitrate reduction on nZVI via electrochemical regulation but also advances the technological coupling of nZVI reduction with electrochemistry.

3.
Inorg Chem ; 59(3): 1736-1745, 2020 Feb 03.
Artigo em Inglês | MEDLINE | ID: mdl-31927961

RESUMO

With fossil energy resources increasingly drying up and gradually causing serious environmental impacts, pursuing a tandem and green synthetic route for a complex and high-value-added compound by using low-cost raw materials has attracted considerable attention. In this regard, the selective and efficient conversion of light olefins with CO2 into high-value-added organic cyclic carbonates (OCCs) is of great significance owing to their high atom economy and absence of the isolation of intermediates. To fulfill this expectation, a multifunctional catalytic system with controllable spatial arrangement of varied catalytic sites and stable texture, in particular, within a single catalyst, is generally needed. Here, by using a stepwise electrostatic interaction strategy, imidazolium-based ILs and Au nanoparticles (NPs) were stepwise immobilized into a sulfonic group grafted MOF to construct a multifunctional single catalyst with a highly ordered arrangement of catalytic sites. The Au NPs and imidazolium cation are separately responsible for the selective epoxidation and cycloaddition reaction. The mesoporous cage within the MOF enriches the substrate molecules and provides a confined catalytic room for the tandem catalysis. More importantly, the highly ordered arrangement of the varied active sites and strong electrostatic attraction interaction result in the intimate contact and effective mass transfer between the catalytic sites, which allow for the highly efficient (>74% yield) and stable (repeatedly usage for at least 8 times) catalytic transformation. The stepwise electrostatic interaction strategy herein provides an absolutely new approach in fabricating the controllable multifunctional catalysts, especially for tandem catalysis.

4.
Water Res ; 168: 115211, 2020 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-31669780

RESUMO

It has been long desired but challenging to forward the advanced treatment of wastewater from empirical trials towards scientific design due to the lack of molecular insight into the pollutants of concern. Herein, we first established a systematic methodology to identify the ligands of Ni(II)-complexes in an electroless nickel (EN) plating effluent. The presence of N-containing groups in the ligands of most Ni(II)-complexes was verified by time-aligned ICP-MS and ESI-HRMS, implying the suitability of autocatalytic ozonation for efficient decomplexation. Thereby, a combined process was proposed on the basis of ozonation to achieve over 83% decomplexation of Ni(II) (initially at 0.36 mg/L), followed by selective Ni(II) sequestration for resource recovery. Combinational LC-MS systems revealed the ozonation-induced fragmentation or elimination of most Ni(II)-complexes as well as the structural change of the residual complexed molecules. The released free Ni(II) was further sequestrated by a nanocomposite of hydrated Zr(IV) oxide confined in a polymeric cation exchanger (nHZO@PCE). The fixed-bed working capacity of nHZO@PCE (∼550 BV) for the ozonated EN plating effluent was over 18 times that of the cation exchanger host (∼30 BV) at the breakthrough point of 0.10 mg Ni/L. More attractively, five adsorption-regeneration cycles demonstrated the great potential of the hybrid adsorbent for sustainable utilization. This study is believed to shed new light on how to design rational processes for advanced treatment of real wastewater based on molecular identification.


Assuntos
Nanocompostos , Poluentes Químicos da Água , Adsorção , Níquel , Águas Residuárias
5.
Chemosphere ; 240: 124940, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31574446

RESUMO

Charged ultrafiltration (UF) membranes can repel electrically charged molecules that are smaller than the size of the membrane pores and display high rejection of solutes, high flux, and low operation pressures compared to uncharged UF, nanofiltration (NF) and reverse osmosis (RO). Here, a charged UF membrane composite (PANI/PVDF) was prepared and regulated via electrochemically reversible control in portions of amine/imine functional groups of PANI. As a result, the permeability and rejection ratios of CR2- on charged PANI/PVDF, with PVDF as a control, increased from 19.6 to a maximum of 183.3 L m-2 h-1 bar-1 and from 3.4% to 74%, which expands the trade-off confine benefited from surface potential change from -12.21 mV to -25.26 mV, furtherly, the rejection ratio of CR2- on PANI/PVDF reached up to 93% via the electrochemical regulation. Finally, a fixed-charge model was built that well describes the steric and electric repulsion effects on membrane performance and the important roles of the electrochemically controllable surface charge. Moreover, the contour map of rejection ratios containing the ratio of molecular size vs the average pore size of the membrane (r/R = 0.2-1.0) and the zeta potential (-10 to -60 mV) were taken into account, which can be used to visually understand the rejection performance of membranes. This model is also appropriate for varying molecular sizes and for molecules with different charges. Our work opens a new horizon for the design of electrochemically controllable charged membranes to remove charged compounds.


Assuntos
Corantes/análise , Técnicas Eletroquímicas/métodos , Ultrafiltração/métodos , Purificação da Água/métodos , Eletricidade , Membranas Artificiais , Propriedades de Superfície
6.
Nat Commun ; 10(1): 5677, 2019 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-31831806

RESUMO

An important goal of the Zika virus (ZIKV) vaccine is to prevent a congenital syndrome in fetuses of pregnant women, but studies directly evaluating maternal vaccination for ZIKV are lacking. Here we report maternal vaccination using a live-attenuated ZIKV vaccine (3'UTR-∆10-LAV) in a pregnant mouse model. Maternal immunization with 3'UTR-∆10-LAV does not cause any adverse effects on pregnancy, fetal development, or offspring behavior. One maternal immunization fully protects dams against ZIKV infection and in utero transmission. Although neutralizing antibody alone is sufficient to prevent in utero transmission, a higher neutralizing titer is required to protect pregnant mice against in utero transmission than that required to protect non-pregnant mice against viral infection. The immunized dams transfer maternal antibodies to pups, which protect neonates against ZIKV infection. Notably, pregnancy weakens maternal T cell response to 3'UTR-∆10-LAV vaccination. Our results suggest that, besides vaccinating non-pregnant individuals, 3'UTR-∆10-LAV may also be considered for maternal vaccination.


Assuntos
Imunidade , Transmissão Vertical de Doença Infecciosa/prevenção & controle , Vacinação , Vacinas Virais/imunologia , Infecção por Zika virus/prevenção & controle , Zika virus/imunologia , Animais , Anticorpos Neutralizantes/imunologia , Anticorpos Antivirais/imunologia , Modelos Animais de Doenças , Feminino , Masculino , Camundongos , Gravidez , Linfócitos T/imunologia , Vacinas Atenuadas/efeitos adversos , Vacinas Atenuadas/imunologia , Vacinas Atenuadas/uso terapêutico , Vacinas Virais/efeitos adversos , Vacinas Virais/uso terapêutico , Zika virus/genética , Infecção por Zika virus/virologia
7.
NPJ Vaccines ; 4: 48, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31815005

RESUMO

Live attenuated vaccines (LAVs) are one of the most important strategies to control flavivirus diseases. The flavivirus nonstructural (NS) 4B proteins are a critical component of both the virus replication complex and evasion of host innate immunity. Here we have used site-directed mutagenesis of residues in the highly conserved N-terminal and central hydrophobic regions of Zika virus (ZIKV) NS4B protein to identify candidate attenuating mutations. Three single-site mutants were generated, of which the NS4B-C100S mutant was more attenuated than the other two mutants (NS4B-C100A and NS4B-P36A) in two immunocompromised mouse models of fatal ZIKV disease. The ZIKV NS4B-C100S mutant triggered stronger type 1 interferons and interleukin-6 production, and higher ZIKV-specific CD4+ and CD8+ T-cell responses, but induced similar titers of neutralization antibodies compared with the parent wild-type ZIKV strain and a previously reported candidate ZIKV LAV with a 10-nucleotide deletion in 3'-UTR (ZIKV-3'UTR-Δ10). Vaccination with ZIKV NS4B-C100S protected mice from subsequent WT ZIKV challenge. Furthermore, either passive immunization with ZIKV NS4B-C100S immune sera or active immunization with ZIKV NS4B-C100S followed by the depletion of T cells affords full protection from lethal WT ZIKV challenge. In summary, our results suggest that the ZIKV NS4B-C100S mutant may serve as a candidate ZIKV LAV due to its attenuated phenotype and high immunogenicity.

8.
Psychol Res Behav Manag ; 12: 825-837, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31572030

RESUMO

Background: For companies, employee creativity is vital to gaining competitive business advantages. Research regarding creativity has focused on contextual factors such as feedback, but results of studies on the relationship between feedback and creativity are inconsistent; further, only a handful of studies have been carried out from the perspective of coworkers. In this study, we aimed to analyze the association between the coworker feedback environment and creativity, to test the mediating role of feedback monitoring in this relationship and to test the moderating role of self-motivation among employees in China. Methods: A coworker feedback environment survey, a coworker feedback monitoring questionnaire, a self-motivation scale and a creativity scale were used. The staff submitted 264 questionnaires, of which 235 (74.6%) were completed by the participants. Among the respondents in the sample, 132 (56.2%) were men, and 103 (43.8%) were women. The mean age is 30 and age range from 24-49. Mplus 7.11 software was used to perform descriptive analysis, Spearman's correlation analysis, mediating analysis and moderation analysis. Results: Coworker feedback environment was positively associated with creativity (ß=0.60, p<0.01) after controlling for the demographic variable. Coworker feedback monitoring partially mediated the relationship between coworker feedback environment and creativity (χ2/df=2.5, RMSEA=0.05; CFI=0.93; GFI=0.93). When self-assessment motivation is lower, the positive relationship between coworker feedback monitoring and creativity becomes stronger (ß=0.19); the same relationship becomes weaker (ß=0.01) when self-assessment motivation is higher. Conclusion: It was suggested that a coworker feedback environment could improve employee creativity by promoting coworker feedback monitoring; creativity could be improved especially among employees who have lower self-assessment motivation.

9.
Front Plant Sci ; 10: 1203, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31632429

RESUMO

Nitrogen (N) supply could improve the grain yield of maize, which is of great importance to provide calories and nutrients in the diets of both humans and animals. Field experiments were conducted in 2009 and 2010 to investigate dynamic zinc (Zn) accumulation and the pre-silking and post-silking Zn uptake and their contributions to grain Zn accumulation of maize with different N supply under field conditions. Results showed that only 1.2% to 39.4% of grain Zn accumulation derived from pre-silking Zn uptake, with Zn remobilization being negatively affected by increasing N supply. However, post-silking Zn uptake (0.8-2.3 mg plant-1) and its substantial contribution to grain Zn accumulation (60.6%-98.8%) were progressively enhanced with the increasing N supply. Furthermore, grain Zn concentration was positively associated with grain N concentration (r = 0.752***), post-silking N uptake (r = 0.695***), and post-silking Zn uptake (r = 738***). A significant positive relationship was also found between post-silking uptake of N and Zn (r = 0.775***). These results suggest that N nutrition is a critical factor for shoot Zn uptake and its allocation to maize grain. Dry weight, and N and Zn concentration of grain and straw were significantly enhanced with the increasing N from "no N" to "optimal N" supply (150 kg N ha-1 in 2009 and 105 kg N ha-1 in 2010), but further increasing N supply (250 kg N ha-1) generally resulted in a non-significant increase in both cropping seasons. During the grain development, N supply also generally tended to improve grain N and Zn concentrations, but decrease phosphorus (P) concentration and the molar ratio of P to Zn compared with null N application. These results suggest that grain Zn accumulation mainly originates from post-silking Zn uptake. Applying N at optimal rates ensures better shoot Zn nutrition and contributes to post-silking Zn uptake, maintaining higher grain Zn availability by decreasing the molar ratio of P to Zn, and resulting in benefits to human nutrition.

10.
PLoS Pathog ; 15(9): e1007996, 2019 09.
Artigo em Inglês | MEDLINE | ID: mdl-31536610

RESUMO

The ability of DENV2 to display different morphologies (hence different antigenic properties) complicates vaccine and therapeutics development. Previous studies showed most strains of laboratory adapted DENV2 particles changed from smooth to "bumpy" surfaced morphology when the temperature is switched from 29°C at 37°C. Here we identified five envelope (E) protein residues different between two alternative passage history DENV2 NGC strains exhibiting smooth or bumpy surface morphologies. Several mutations performed on the smooth DENV2 infectious clone destabilized the surface, as observed by cryoEM. Molecular dynamics simulations demonstrated how chemically subtle substitution at various positions destabilized dimeric interactions between E proteins. In contrast, three out of four DENV2 clinical isolates showed a smooth surface morphology at 37°C, and only at high fever temperature (40°C) did they become "bumpy". These results imply vaccines should contain particles representing both morphologies. For prophylactic and therapeutic treatments, this study also informs on which types of antibodies should be used at different stages of an infection, i.e., those that bind to monomeric E proteins on the bumpy surface or across multiple E proteins on the smooth surfaced virus.


Assuntos
Vírus da Dengue/classificação , Vírus da Dengue/genética , Sequência de Aminoácidos , Substituição de Aminoácidos , Animais , Antígenos Virais/química , Antígenos Virais/genética , Linhagem Celular , Microscopia Crioeletrônica , Vírus da Dengue/ultraestrutura , Humanos , Modelos Moleculares , Simulação de Dinâmica Molecular , Mutação , Domínios e Motivos de Interação entre Proteínas , Homologia de Sequência de Aminoácidos , Sorogrupo , Temperatura Ambiente , Proteínas do Envelope Viral/química , Proteínas do Envelope Viral/genética , Proteínas do Envelope Viral/imunologia
11.
J Colloid Interface Sci ; 557: 207-215, 2019 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-31521970

RESUMO

The development of a suitable catalytic system in the single catalyst has always been the pursuit for synthetic chemists in order to perform the traditional stepwise reactions in one-pot mode. In this work, an ultra-stable bifunctional catalyst of Pd@MIL-101-SO3H was successfully constructed and applied in the one-pot oxidation-acetalization reaction whose products have been widely utilized as fuel additives, perfumes, pharmaceuticals and polymer chemistry. The excellent catalytic performance (>99% yields), on the one hand, can be ascribed to the synergistic effects of Pd NPs with both Lewis and Bronsted acid encapsulated within a sulfonated MIL-101(Cr). On the other hand, the exceptionally high capacity of water adsorption in MIL-101(Cr) could promote the equilibrium movement via interrupting the reversible process. More importantly, Pd@MIL-101-SO3H is recyclable and can be reused for at least 8 times without sacrificing its catalytic activities. As far as we know, this is the first time that a water adsorption enhanced equilibrium movement of reversible reaction by porous catalyst to achieve high yields has been realized in Pd@MIL-101-SO3H, which may provide an absolutely new and efficient strategy especially for designing reaction-oriented catalysts.

12.
Antiviral Res ; 171: 104596, 2019 11.
Artigo em Inglês | MEDLINE | ID: mdl-31493417

RESUMO

Zika virus (ZIKV) has drawn global attention as the etiologic agent of Zika Congenital Syndrome in babies born to infected pregnant women. To prevent future ZIKV outbreaks and protect persons at risk for severe disease, we developed two live-attenuated vaccine (LAV) candidates containing 10- or 20-nucleotide deletions in the 3'UTR of the viral genome (Δ10 and Δ20). After a single-dose immunization, both Δ10 and Δ20 LAVs protected mice and non-human primates against ZIKV infection. Here, we characterized the stability, safety, and efficacy of the LAVs after continuously culturing them on manufacture Vero cells for ten rounds. Whole genome sequencing showed that passage 10 (P10) LAVs retained the engineered Δ10 and Δ20 deletions; one to four additional mutations emerged at different regions of the genome. In A129 mice, the P10 LAVs exhibited viremia higher than the un-passaged LAVs, but lower than wild-type ZIKV; unlike wild-type ZIKV-infected mice, none of the P10 LAV-infected mice developed disease or death, demonstrating that the P10 LAVs remained attenuated. Mice immunized with a single dose of the P10 LAVs developed robust neutralizing antibody titers (1/1,000 to 1/10,000) and were protected against epidemic ZIKV challenge. The P10 LAVs did not exhibit increased neurovirulence. Intracranial inoculation of one-day-old CD1 pups with 103 focus-forming units of the P10 Δ10 and Δ20 LAVs resulted in 100% and ≥80% survival, respectively. Furthermore, the P10 LAVs remained incompetent in infecting Aedes aegypti mosquitoes after intrathoracic microinjection. Our results support the phenotypic stability and further development of these promising LAVs for ZIKV.

13.
Theranostics ; 9(18): 5166-5182, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31410208

RESUMO

Background and Aim: We have previously shown that high-mobility group box 1 (HMGB1) is an independent biomarker for shortened survival of prostate cancer (PCa) patients. However, the specific role of HMGB1 in tumor development and progression remains largely unknown. In this study, we investigated the molecular mechanisms of HMGB1 in PCa tumorigenesis. Methods: Gain-of-function and loss-of-function experiments were used to determine the biological functions of HMGB1 both in vitro and in vivo. Bioinformatic analysis, immunoprecipitation, and immunofluorescence assays were applied to discern and examine the relationship between HMGB1 and its potential targets. Specimens from 64 patients with PCa were analyzed for the expression of HMGB1 and its relationship with Brahma-related gene 1 (BRG1) was examined by immunohistochemistry. Results: The results demonstrated that ectopic expression of HMGB1 facilitated growth and metastasis of PCa by enhancing Akt signaling pathway and promoting epithelial-mesenchymal transition (EMT), while silencing of HMGB1 showed the opposite effects. Mechanistically, HMGB1 exerted these functions through its interaction with BRG1 which may augment BRG1 function and activate the Akt signaling pathway thereby promoting EMT. Importantly, both HMGB1 and BRG1 expression was markedly increased in human PCa tissues. Conclusions: Taken together, these findings indicate that upregulation of HMGB1 promotes PCa development via activation of Akt and accelerates metastasis through regulating BRG1-mediated EMT. HMGB1 could be used as a novel potential target for the treatment of PCa.

14.
Stem Cell Res Ther ; 10(1): 208, 2019 07 16.
Artigo em Inglês | MEDLINE | ID: mdl-31311594

RESUMO

BACKGROUND: Stem cell therapy has revealed a promising future for treating erectile dysfunction (ED), but the fate and curative mechanism of intracavernosal transplanted stem cells are under further exploration. This study aimed to demonstrate the effects of myocardin gene modification on improving erectile function and prolonging the retention of implanted adipose-derived stem cells (ASCs) using in vivo small animal imaging. METHODS: ASCs were isolated, cultured, and identified by flow cytometry and osteogenic and adipogenic induction. The effects of gene modification on cell proliferation, apoptosis, and contraction were determined by CCK-8, EdU, flow cytometry, and collagen gel lattice contraction assays as well as confocal microscopy. A total of 20 normal and 60 diabetes mellitus ED to (DMED) Sprague-Dawley rats were recruited to the 7 day and 21 day groups. Each group contained subgroups of 10 rats each: the negative control (NC), DMED + ASCs plus Ad-Luc-Myocardin, DMED + ASCs plus Ad-Luc, and DMED + phosphate buffer solution (PBS) groups. Erectile function was evaluated with the intracavernosal pressure/mean arterial pressure (△ICP/MAP) ratio. In vivo small animal imaging and an EdU cell tracking strategy were introduced to detect the transplanted ASCs, and IHC and WB were performed to assess smooth muscle cell protein levels. RESULTS: The ASCs expressed high CD29 and CD90 and scant CD45, while the multi-induction potential was verified by oil red O and alizarin red staining. Gene transfection of myocardin had no significant influence on ASC apoptosis but inhibited cell proliferation and promoted cell contraction. Myocardin combined with ASCs enhanced the therapeutic potential of ASCs for improving the △ICP/MAP ratio as well as α-SMA and calponin expression. In vivo imaging confirmed that ASCs resided within the cavernous body in 21 days, while only a few red EdU dots were detected. CONCLUSIONS: Myocardin induced ASC differentiation towards smooth muscle-like cells and enhanced the therapeutic potential of ASCs for ameliorating ED in STZ-induced diabetic rats. Notably, in vivo small animal tracking was an effective strategy for monitoring the implanted stem cells, and this strategy might have advantages over traditional EdU assays.

15.
Am J Transl Res ; 11(6): 3645-3650, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31312375

RESUMO

Healing of damaged tissue results in scar development, which can be difficult to manage. The present study was performed to determine the effects of inhibition of the microRNA (miR), miR-9, on the proliferation of fibroblasts in human hyperplastic scar (HS) formation. Samples of HS tissue and normal tissue were isolated from 20 patients, and the fibroblasts were transfected with small-interfering RNA (siRNA) for transforming growth factor beta 1 (TGF-ß1), miR-9 mimic, and miR-9 inhibition. TGF-ß1 protein and mRNA expression were examined in the fibroblasts and HS tissue samples by Western blotting and RT-PCR, respectively. Moreover, the effects of miR-9 inhibitor and mimic on cell proliferation and apoptosis were also examined in the HS tissue. Protein and mRNA expression levels of TGF-ß1 were increased in the HS tissue compared to adjacent normal tissues. The levels of TGF-ß1 mRNA and protein expression were reduced in siRNA-transfected cells. The miR-9 and TGF-ß1 mRNA expression levels were reduced in the miR-9 inhibitor treatment group compared to both the negative control (NC) and control groups. Reduced levels of miR-9 and TGF-ß1 mRNA expression were observed in the miR-9 inhibitor treatment group compared to the NC and control groups. Moreover, miR-9 inhibitor increased the percentage of apoptotic cells and decreased cell proliferation compared to the NC and control groups. In conclusion, this study showed that miR-9 plays an important role in the proliferation of fibroblasts by regulating TGF-ß1 expression in HS tissue.

16.
Water Res ; 161: 78-88, 2019 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-31181449

RESUMO

Phosphonate is an important phosphorous species in the effluent of wastewater treatment plant (WWTP), contributing to eutrophication and interfering with phosphate removal in WWTP. It is particularly difficult to determine phosphonates in samples of complex solution chemistry, resulting in very limited information on their presence in environmental matrices. Herein, we proposed a sensitive method based on liquid chromatography tandem mass spectrometry (LC-MS/MS) to determine six quantitatively most important phosphonates even at the ng/L level, i.e., 2-phosphonobutane-1,2,4-tricarboxylic acid, 1-hydroxyethane 1,1-diphosphonic acid, nitrilotris(methylene phosphonic acid), ethylenediamine tetra(methylene phosphonic acid), hexamethylenediamine tetra(methylene phosphonic acid) and diethylenetriamine penta(methylene phosphonic acid). Trimethylsilyldiazomethane (TMSCHN2) derivatization of the target phosphonates is pre-requisite since it could greatly increase the sensitivity up to 2-3 orders of magnitude over direct analysis of the virgin ones. The sample pretreatment methods (including ion exchange and solid phase extraction(SPE)), the derivatization procedures, and the LC-MS/MS conditions were systematically optimized. The limits of quantitation for the six phosphonates in the background of tap water ranged from 1.4 µg/L to 57 µg/L for direct analysis, and from 5.0 ng/L to 200 ng/L for SPE enabled pre-concentration analysis, respectively. The reliability of the proposed method was successfully validated by analysis of authentic water samples collected from one river and three WWTPs (0.088-7200 µg/L phosphonates) with satisfactory recoveries (72-126%). To the best of knowledge, this is the first report on quantification of phosphonates in environmental samples in China.


Assuntos
Organofosfonatos , Poluentes Químicos da Água , China , Cromatografia Líquida , Metilação , Reprodutibilidade dos Testes , Extração em Fase Sólida , Espectrometria de Massas em Tandem , Águas Residuárias
17.
Sci Total Environ ; 675: 62-72, 2019 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-31026644

RESUMO

A new composite catalyst, i.e., Fe doped g-C3N4/graphite (Fe-CN/G), was successfully constructed to activate peroxymonosulfate (PMS) for efficient phenolic compounds (i.e., p-chlorophenol, 4-CP) degradation in the pH range of 3-10. The optimized Fe-CN/G, i.e., Fe3.75-CN/G5.0, was fabricated at the dosage of 3.75 mmol FeCl3·6H2O, 5.0 g dicyandiamide, and 5.0 mmol glucose. Fe complexed in the nitrogen pots of Fe3.75-CN/G5.0 was demonstrated to be the primary active site for PMS activation, and the introduction of graphite favored the exposure of more accessible active sites in Fe3.75-CN/G5.0, suggesting a synergistic effect between the Fe and graphite of Fe3.75-CN/G5.0 on 4-CP degradation. Multiple experiments confirmed that sulfate radical (SO4-), hydroxyl radical (HO), singlet oxygen (1O2) and superoxide radical (O2-) exerted negligible contribution on 4-CP degradation. The in-situ Fe K-edge X-ray absorption near-edge structure (XANEX) analysis revealed a redox cycle of Fe in PMS/Fe3.75-CN/G5.0, suggesting the formation of high-valent iron-oxo species (FeIVO) was responsible for 4-CP degradation. In addition, PMS/Fe3.75-CN/G5.0 exhibited acceptable degradation of 4-CP in the presence of coexisting anions and natural organic matters (NOM). We believe this study provides new insights into the design and development of Fe-based heterogeneous catalysts for PMS-based wastewater treatment.

19.
Water Res ; 157: 472-482, 2019 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-30981978

RESUMO

As one of the key economic modes in China, chemical industry park (CIP) has made great contribution to the Chinese rapid economic growth. Concomitantly, how to effectively and safely dispose of the CIP wastewater (CIPWW) has been an unavoidable issue. Molecular transformation of dissolved organic matter (DOM) in CIPWW treatment is essential to optimize the employed process and to provide solid basis for risk evaluation of the discharged effluent as well. In this study, electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS) was used to characterize the molecular transformation of DOM during full-scale treatment of integrated chemical wastewater in a centralized wastewater treatment plant (CWWTP), where the combined process follows hydrolysis/acidification (HA)-flocculation/precipitation (FP)-A2/O-membrane bioreactor (MBR)-ultrafiltration (UF)-reverse osmosis (RO). Compared to municipal wastewater, DOM in CIPWW exhibited higher unsaturation degree, lower molecular weight, and higher toxicity. In FP unit, DOM of C<24 and higher nominal oxidation state of carbon (NOSC) values was preferentially removed. The HA and anaerobic units are capable of significantly degrading DOM, resulting in great changes in molecular composition of DOM. However, the anoxic, oxic, and MBR units only lead to a slight change of the molecular formulae. The terminal units of UF and RO can remove most DOM, with the concentration of dissolved organic carbon (DOC) declining by 19.2% and 94.6% respectively. The correlation between spectral indexes and acute toxicity with the molecular formulae of DOM suggested that polyphenols and highly unsaturated phenols were positively correlated with the specific UV absorbance at 254 nm (SUVA254). In addition, both compounds (0.32 < O/C < 0.63) as well as the aliphatic ones (0.22 < O/C < 0.56) presented positive correlation with acute toxicity. Further, the pairwise correlation analysis illustrated that SUVA254, O/Cwa, double bond equivalence (DBEwa), and NOSCwa were positively correlated with each other, whereas the acute toxicity was positively correlated with humification index (HIX), O/Cwa, and DBEwa.


Assuntos
Ultrafiltração , Águas Residuárias , China , Filtração , Espectrometria de Massas
20.
Emerg Microbes Infect ; 8(1): 585-602, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-30958095

RESUMO

Zika virus (ZIKV) can cause devastating congenital Zika syndromes in pregnant women and Guillain-Barre syndrome in adults. Understanding the molecular mechanism of ZIKV replication is essential for antiviral and vaccine development. Here we report the structural and functional characterization of ZIKV NS2A protein. Biochemical structural probing suggests that ZIKV NS2A has a single segment that traverses the ER membrane and six segments that peripherally associate with the ER membrane. Functional analysis has defined distinct NS2A residues essential for viral RNA synthesis or virion assembly. Only the virion assembly-defective mutants, but not the RNA synthesis-defective mutants, could be rescued through trans complementation with a wide-type NS2A protein. These results suggest that the NS2A molecules in virion assembly complex could be recruited in trans, whereas the NS2A molecules in viral replication complex must be recruited in cis. Together with previous results, we propose a flavivirus assembly model where NS2A plays a central role in modulating viral structural and nonstructural proteins as well as genomic RNA during virion assembly.


Assuntos
Proteínas não Estruturais Virais/metabolismo , Infecção por Zika virus/virologia , Zika virus/fisiologia , Linhagem Celular , Retículo Endoplasmático/metabolismo , Retículo Endoplasmático/virologia , Humanos , Proteínas não Estruturais Virais/genética , Montagem de Vírus , Replicação Viral , Zika virus/genética
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