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1.
Environ Sci Pollut Res Int ; 31(11): 17156-17163, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38334926

RESUMO

Phosphonates have received a widespread attention in wastewater treatment due to their potential threat to the water environment. Advanced oxidation processes (AOPs) are feasible methods to degrade phosphonates, and most of the coexisting substances in water show a negative factor during their oxidation. However, the effect of bromide (Br-) on the degradation of phosphonates in peroxymonosulfate (PMS) activation is still unclear. Herein, using 1-hydroxyethane 1,1-diphosphonic acid (HEDP) as a target phosphonate, Br- could remarkably enhance the degradation of HEDP in PMS activation compared to the PMS alone. Under the condition of pH = 7.0, the optimal degradation efficiency of HEDP is 84.8% in the PMS/Br- process after 30-min reaction, whereas no significant oxidation is obtained in the PMS/I- and PMS/Cl- processes. Multiple experiments (i.e., electron paramagnetic resonance (EPR), radical quenching experiments and chemical probs) confirm that free bromine, SO4•- and HO• paly a minor role in HEDP removal, and bromine radical species make a dominant responsible for HEDP oxidation. Additionally, NO3-, SO42-, Cl-, and HCO3- have a little effect on the degradation of HEDP, but the HEDP removal is greatly inhibited in the presence of humic acid (HA). However, the degradation efficiency of HEDP using PMS/Br- process in river and sewage is a much higher than UV/persulfate (PDS) and UV/H2O2 processes. This study provides a new sight into the effect of Br- on the degradation phosphonates in PMS activation process.


Assuntos
Organofosfonatos , Poluentes Químicos da Água , Peróxido de Hidrogênio/química , Brometos , Bromo , Ácido Etidrônico , Poluentes Químicos da Água/análise , Peróxidos/química , Oxirredução , Água
2.
Cancer Med ; 13(3): e6736, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38204220

RESUMO

BACKGROUND: The mechanism of decreased T cells infiltrating tumor tissues in hepatocellular carcinoma is poorly understood. METHODS: Cells were separated from the single-cell RNA-sequence dataset of hepatocellular carcinoma patients (GSE149614) for cell-cell communication. Flow cytometry, EDU staining, H3-Ser28 staining, confocal immunofluorescence staining, western blotting and naked microsubcutaneous tumors were performed for the mechanism of NGF-NGFR promoting proliferation. RESULTS: The present study has revealed that during the process of T-cell infiltration from adjacent tissues to tumor tissues, an inefficiency in NGF-NGFR communication occurs in the tumor tissues. Importantly, NGF secreted by tumor cells interacts with NGFR present on the membranes of the infiltrated T cells, thereby promoting the proliferation through the activation of mitotic spindle signals. Mechanistically, the mediation of mitotic spindle signal activation promoting proliferation is executed by HDAC1-mediated inhibition of unclear trans-localization of PREX1. Furthermore, PD-1 mAb acts synergistically with the NGF-NGFR communication to suppress tumor progression in both mouse models and HCC patients. Additionally, NGF-NGFR communication was positively correlates with the PD-1/PDL-1 expression. However, expressions of NGF and NGFR are low in tumor tissues, which is responsible for the invasive clinicopathological features and the disappointing prognosis in HCC patients. CONCLUSION: Inefficiency in NGF-NGFR communication impairs PD-1 mAb immunotherapy and could thus be utilized as a novel therapeutic target in the treatment of HCC patients in clinical practice.


Assuntos
Carcinoma Hepatocelular , Neoplasias Hepáticas , Animais , Camundongos , Humanos , Carcinoma Hepatocelular/terapia , Receptor de Morte Celular Programada 1 , Neoplasias Hepáticas/terapia , Linfócitos T , Imunoterapia , Fatores de Troca do Nucleotídeo Guanina , Proteínas do Tecido Nervoso , Receptores de Fator de Crescimento Neural
3.
Environ Sci Technol ; 57(5): 1907-1918, 2023 02 07.
Artigo em Inglês | MEDLINE | ID: mdl-36695577

RESUMO

Organophosphate esters (OPEs) discharged from wastewater treatment plants (WWTPs) have attracted increasing concerns because of their potential risks to aquatic ecosystems. The identification of the structures of OPEs is a prerequisite for subsequent assessment of their environmental impacts, which could hardly be accomplished using traditional target analytical methods. In this study, we describe the use of suspect and nontarget screening techniques for identification of organophosphate triesters and diesters (tri-OPEs and di-OPEs) in the influent and effluent samples acquired from 25 municipal WWTPs across China. There are totally 33 different OPE molecules identified, 11 of which are detected in wastewater for the first time and 4 are new to the public. In all tested samples, di-OPEs account for a significant portion (53% on average) of the total OPEs (ng/L-µg/L). More importantly, most of the OPEs could not be eliminated after treatment in these WWTPs, while some of the di-OPEs even accumulate. The research priority of OPEs in the effluent based on ecological risk was also analyzed, and the results reflected a previously unrecognized exposure risk of emerging OPEs for aquatic living organisms. These findings present a holistic understanding of the environmental relevance of OPEs in WWTPs on a country scale, which will hopefully provide guidance for the upgrade of treatment protocols in WWTPs and even for the modification of governmental regulations in the future.


Assuntos
Retardadores de Chama , Purificação da Água , Ecossistema , Retardadores de Chama/análise , Ésteres , China , Organofosfatos , Monitoramento Ambiental
4.
Sci Total Environ ; 811: 152328, 2022 Mar 10.
Artigo em Inglês | MEDLINE | ID: mdl-34915012

RESUMO

Ozonation and ultraviolet-based advanced oxidation processes (UV-AOPs) play important roles in advanced treatment of municipal wastewater for water reuse. Bromide is widely present in wastewater at different concentration levels (ranging from µg/L to mg/L). However, the effect of bromide on molecular transformation of dissolved effluent organic matter (dEfOM) in real wastewater during ozonation and UV-AOPs treatments still remains unclear. Herein, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was utilized to characterize the overall molecular transformation of dEfOM and the formation of unknown halogenated byproducts (X-BPs) in ozonation, UV/H2O2, UV/persulfate (UV/PS), and UV/chlorine (UV/Cl) processes in the presence of additional bromide. Compared with the same oxidation processes without additional bromide, the degree of dEfOM oxygenation had some extent decrement with the effect of bromide. A slightly increment of the number of unknown brominated byproducts (Br-BPs) was observed during ozonation, UV/H2O2, and UV/PS treatments in the presence of additional bromide, and the largest increment of these compounds was found in UV/Cl process. A total of 82 chlorinated byproducts (Cl-BPs) and 183 Br-BPs were detected in all oxidation processes with the effect of bromide, and the number of Br-BPs was significantly higher than that of Cl-BPs. Based on mass difference analysis, 69 pairs of possible precursors/Br-BPs were identified. In addition, the additional bromide did not remarkably increase the concentrations of trihalomethanes (THMs) and haloacetic acids (HAAs) in ozonation, UV/H2O2, and UV/PS treatments, while the production of THMs and HAAs significantly decreased by 68.06% and 54.55%, respectively, during UV/Cl treatment. The calculated cytotoxicity increased to some extent for each treatment, especially for UV/Cl treatment, and the compound with largest contribution to cytotoxicity was monobromoacetic acid. This study provides new insights into the formation and transformation of X-BPs during advanced treatment of real wastewater with the effect of bromide.


Assuntos
Ozônio , Poluentes Químicos da Água , Purificação da Água , Brometos , Cloro , Desinfecção , Peróxido de Hidrogênio , Raios Ultravioleta , Poluentes Químicos da Água/análise
5.
Huan Jing Ke Xue ; 42(8): 3847-3857, 2021 Aug 08.
Artigo em Chinês | MEDLINE | ID: mdl-34309271

RESUMO

As an emerging advanced oxidation technology, UV/chlorine treatment is capable of effectively oxidizing various organic pollutants. Till now, the transformation of dissolved effluent organic matter (dEfOM) in real wastewater during UV/chlorine treatment remains unclear. In this study, ultraviolet and fluorescence spectroscopy were combined with Fourier transform ion cyclotron resonance mass spectrometry to probe the transformation of dEfOM in two municipal secondary effluents during UV/chlorine treatment. Meanwhile, the newly formed chlorinated byproducts (Cl-BPs) are particularly concerned. Generally, aromatic compounds and fluorescent components could be readily removed after UV/chlorine treatment, and most of the dEfOM underwent transformation rather than mineralization. Protein-like components, which accounted for the largest proportion of fluorescent components, were subject to a preferential reaction. UV/chlorine treatment could result in the degradation of CHOS compounds and the formation of CHO compounds. During this process, unsaturated and reduced compounds of large molecules were preferentially removed, whereas saturated and oxidized compounds with low molecular weight were produced. Moreover, the concentrations of trihalomethanes and haloacetic acids increased substantially after UV/chlorine treatment. In total, 255 and 133 Cl-BPs were detected in the respective effluents after UV/chlorine treatment. In addition, 12 and 43 possible precursor-Cl-BPs pairs were identified, respectively, based on electrophilic substitution and addition reactions by means of mass difference analysis. This study is expected to provide fundamental information for practical application of the UV/chlorine treatment process.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Cloro/análise , Desinfecção , Trialometanos , Raios Ultravioleta , Águas Residuárias , Poluentes Químicos da Água/análise
6.
Oral Oncol ; 119: 105363, 2021 08.
Artigo em Inglês | MEDLINE | ID: mdl-34182278

RESUMO

OBJECTIVE: To provide information about hospitalization costs and length of stay (LOS) for inpatients undergoing oral cancer (OC) surgery, and to investigate the association of hospitalization costs and LOS with demographics, tumor subsite, surgery-related and hospital characteristics. METHODS: Data extracted from Chinese National Health Statistics Network Reporting System database in Hunan, China during 2017-2019 were analyzed using quantile regression models. RESULTS: A total of 6,420 OC patients undergoing surgery were identified. After controlling potential compounding variables, the median hospitalization cost was significantly higher in male than in female patientsby $515.70 at the median (p < 0.001). Patients aged over 60 hadsignificantly less costs by $294.85 at the meanthan did those below 60, while no differenceof LOS existed across age. OC patients with neck dissection had significantly higher costs by $1,983.33 at the median than those without (P < 0.001). Regional flaps were the most economical, with lower costs than free flaps by $3,084 (P < 0.001) and the pectoralis major myocutaneous flap (PMMF) by $549.45 (P < 0.001) at the median. CONCLUSION: Male is a significant driver of hospitalization costs and LOS for OC, and age over 60 is associated with lower costs, but not with LOS. Mouth primary site is associated with the highest costs and LOS, while lip primary site the lowest. Absence of neck dissection in early-stage OC can significantly reduce costs and LOS, but its oncological validity needs more evidence. Regional flaps are less expensive than free flaps and the PMMF for oral reconstruction, and are recommended in select patients.


Assuntos
Hospitalização/economia , Tempo de Internação , Neoplasias Bucais , Idoso , China , Feminino , Retalhos de Tecido Biológico , Custos de Cuidados de Saúde , Humanos , Masculino , Pessoa de Meia-Idade , Neoplasias Bucais/cirurgia , Estudos Retrospectivos
7.
Water Res ; 199: 117158, 2021 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-33975087

RESUMO

Ultraviolet-based advanced oxidation processes (UV-AOPs) are very promising in advanced treatment of municipal secondary effluents. However, the transformation of dissolved effluent organic matter (dEfOM) in advanced treatment of real wastewater, particularly at molecular level, remains unclear. In this study, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with multiple statistical analysis were performed to better understand the transformation of dEfOM in UV/H2O2, UV/persulfate (UV/PS), and UV/chlorine treatments. An obvious increase in oxygen content of dEfOM was observed after every UV-AOPs treatment, and the detailed oxygenation processes were further uncovered by mass difference analysis based on 24 types of typical reactions. Generally, UV/H2O2 process was subjected to the most oxygenation reactions with the typical tri-hydroxylation one (+3O), whereas di-hydroxylation reaction (+H2O2) was dominant in UV/PS and UV/chlorine processes. Additionally, the three UV-AOPs shared the majority of precursors, and more proportions of unique products were identified for each process. The precursors with lower H/C and higher aromaticity were readily degraded by UV/chlorine over UV/H2O2 and UV/PS, with the products featuring lower molecular weight. Moreover, dEfOM of high aromaticity tended to produce chlorinated byproducts through addition reactions in chlorination and UV/chlorine processes. Among these UV-AOPs, the highest reduction of both acute toxicity and specific UV absorbance at 254 nm (SUVA254) was observed for UV/chlorine, implying the potential for UV/chlorine process in advanced treatment of wastewater. In addition, acute toxicity was highly correlated with SUVA254 and CHOS compounds. This study is believed to help better understand the different fates of dEfOM in real wastewater during UV-AOPs treatment.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Cloro , Peróxido de Hidrogênio , Espectrometria de Massas , Oxirredução , Raios Ultravioleta , Poluentes Químicos da Água/análise
8.
Water Res ; 188: 116484, 2021 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-33045637

RESUMO

Ozonation is a well-recognized process in advanced treatment of municipal secondary effluent for water reclamation. However, the transformation of dissolved effluent organic matter (dEfOM) during ozonation of real effluents, particularly at molecular level, has been scarcely reported. In this study, we performed ozonation treatments on real secondary effluents from two municipal wastewater treatment plants, and used Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) and various spectroscopic techniques to probe the transformation of dEfOM at four ozone dosage levels (0.28, 0.61, 0.89, and 1.21 mg O3/mg DOC). Most of the precursors were unsaturated and reduced compounds (positive double bond equivalent minus oxygen per carbon ((DBE-O)/C) and negative nominal oxidation state of carbon (NOSC)), whereas the products were mainly the saturated and oxidized ones (negative (DBE-O)/C and positive NOSC). As the ozone dosage increased, the relative abundance of O8-19 species gradually increased in the ozonated samples, whereas an opposite trend was observed for O5-7S1 species. Further, we employed 18 types of reactions to represent the ozonation process, and found that the oxygenation reaction (+3O) possessed the largest number of possible precursor-product pairs, and CHON compounds possessed the highest reactivity. Besides the dominant oxygenation reactions, decyclopropyl (-C3H4) was relatively common reaction for CHON compounds, while it was oxidative desulfonation (-SH2) for CHOS ones. In addition, the transformation of precursors to products accompanied with the drop of (DBE-O)/C, and the increase of NOSC and the O/C ratio. The precursors with aromaticity and fluorescence were mainly correlated with the compounds featuring higher (DBE-O)/C and lower NOSC values. This study is believed to help better understand and improve the application of ozonation process in advanced treatment of real wastewater.


Assuntos
Ozônio , Poluentes Químicos da Água , Purificação da Água , Espectrometria de Massas , Águas Residuárias/análise , Poluentes Químicos da Água/análise
9.
Oral Dis ; 27(6): 1366-1375, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32492239

RESUMO

OBJECTIVE: To explore the correlations between the habit of betel quid and areca nut (BQ-AN) chewing and the prognosis of oral cancer (OC). METHODS: We performed a systematic review and meta-analysis to clarify this issue. Data searches were performed using PubMed, Web of Science, Epistemonikos, and Embase databases through November 2019. The primary outcome was the difference in the prognosis of OC between BQ-AN chewers and non-chewers, measured in terms of 5-year overall survival (OS) and 5-year disease-specific survival (DSS) log (HR) reported in articles. The pooled HR with 95% CI of 5-year OS and 5-year DSS was calculated using a fixed-effects model. RESULTS: Ten articles with eleven OS or DSS survival studies (one of the articles contained two studies), which were published between 2003 and 2017, were eligible for inclusion in the present study. All the 11 studies were observational studies, among which 10 were retrospective and 1 was prospective. One study measured both OS and DSS. Eight studies, with a total of 2,761 patients, used 5-year OS as the primary endpoint and four studies, with a total of 2,551 patients, used 5-year DSS. Overall, the pooled HR evaluating BQ-AN chewers was 1.26 (95% CI: 1.09-1.46) for 5-year OS and 1.40 (95% CI: 1.15-1.70) for 5-year DSS, compared with non-chewers. There was a significant association between BQ-AN chewing and OC survival. CONCLUSIONS: Betel quid and areca nut chewing is significantly associated with poor prognosis in patients with OC.


Assuntos
Areca , Neoplasias Bucais , Areca/efeitos adversos , Humanos , Mastigação , Neoplasias Bucais/etiologia , Nozes , Prognóstico , Estudos Prospectivos , Estudos Retrospectivos
10.
Water Res ; 190: 116761, 2021 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-33360615

RESUMO

Anaerobic digestion of organic waste and wastewater represents an attractive sustainable bio-technology to produce methane as an alternative to fossil energy. In response to improvement of methane production via enhancing methanogenesis, current strategies of the addition of external biological/non-biological materials have to confront either the loss of materials, high cost and/or possible destruction of the microbial community. Here, we report the first case of using immobilized fungi Aspergillus sydowii 8L-9-F02 to optimize the microbial community, achieving remarkable improvement of the methane production in both batch test (1.5 times) and continuous flow operation (1.13-1.31 times). The crucial role of fungi is associated with the stimulation of enrichment of Methanosaeta and Methanobacterium for methanogenesis from 28.2 to 67.4% as well as the improved activity of enzyme F420. Moreover, fungi also increase the content of extracellular polymeric substances, facilitating the formation of bio-aggregates. This work provides a new pathway to enhance methanogenesis during anaerobic digestion of wastewater by using fungi as bio-enhancer.


Assuntos
Metano , Purificação da Água , Anaerobiose , Aspergillus , Reatores Biológicos , Fungos , Esgotos , Águas Residuárias
11.
Water Res ; 184: 116173, 2020 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-32712507

RESUMO

Phosphonates discharged from wastewater treatment plants (WWTPs) have attracted increasing concerns because of their potential impact on eutrophication and potential risks to aquatic ecosystems. However, very few studies are available on their occurrence and transformation in WWTPs, partly due to the lack of sensitive methods for phosphonate analysis in complex matrices. Herein, based on our recent progress in phosphonate analysis, the occurrence and transformation of phosphonates along the full-scale wastewater treatment processes of two textile dyeing WWTPs were revealed. A set of typical phosphonates, including six phosphonate chelators (PCs) and four potential degradation products of PCs (DP-PCs) were quantified in different units and the final dewatered sludge. Three PCs (2-phosphonobutane-1,2,4-tricarboxylic acid (PBTC), 1-hydroxyethane 1,1-diphosphonic acid (HEDP) and nitrilotris(methylene phosphonic acid) (NTMP)) at upmost mg/L and a considerable amount of four DP-PCs (9.12-608 µg/L) were detected in the influents of both WWTPs. In the subsequent treatment, NTMP could be removed more efficiently than PBTC and HEDP, especially in the coagulation unit, and the dissolved phosphonates were eliminated more readily than other dissolved organic phosphorus fractions. Of particular note, the toxicologically critical DP-PC (i.e., aminomethylphosphonic acid) was produced during the coagulation and biological treatment units. The final precipitation unit seemed essential to ensure satisfactory removal of PCs and DP-PCs. In addition, a significant accumulation of phosphonates in dewatered sludge (up to 7.81 g/kg) and the widespread occurrence of harmful DP-PCs also reminded us to pay more concerns on their potential risks during further sludge disposal in future.


Assuntos
Organofosfonatos , Poluentes Químicos da Água , Ecossistema , Esgotos , Têxteis , Eliminação de Resíduos Líquidos , Águas Residuárias , Poluentes Químicos da Água/análise
12.
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
13.
J Enzyme Inhib Med Chem ; 34(1): 203-217, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30835140

RESUMO

A series of quinazoline derivatives with benzylidene hydrazine carboxamide were designed and synthesised as EGFR inhibitors. Most compounds exhibited exceptional anti-proliferative activity against A549, HepG2, MCF-7 and H1975 cells. Furthermore, six compounds demonstrated excellent inhibition activity against EGFRWT with the IC50 value both less than 2 nM. Among the six compounds, 44 exhibited the strongest activity (0.4 nM) and potently inhibited EGFRL858R/T790M (0.1 µM). Excitingly, the most potent compound 14 showed excellent enzyme inhibitory activity with 6.3 nM and 8.4 nM for both EGFRWT and EGFRT790M/L858R. The result of AO single staining and Annexin V/PI staining showed that the compound 14 and 44 could induce remarkable apoptosis of A549 cells. The compound 14 arrested the cell cycle at the S phase and compound 44 arrested the cell cycle at the G0 phase in A549 cells. These preliminary results demonstrate that compound 14 and 44 may be promising lead compound-targeting EGFR.


Assuntos
Antineoplásicos/farmacologia , Carcinoma Pulmonar de Células não Pequenas/tratamento farmacológico , Desenho de Fármacos , Neoplasias Pulmonares/tratamento farmacológico , Inibidores de Proteínas Quinases/farmacologia , Quinazolinas/farmacologia , Antineoplásicos/síntese química , Antineoplásicos/química , Apoptose/efeitos dos fármacos , Carcinoma Pulmonar de Células não Pequenas/metabolismo , Carcinoma Pulmonar de Células não Pequenas/patologia , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Relação Dose-Resposta a Droga , Resistencia a Medicamentos Antineoplásicos/efeitos dos fármacos , Ensaios de Seleção de Medicamentos Antitumorais , Receptores ErbB/antagonistas & inibidores , Receptores ErbB/metabolismo , Gefitinibe/química , Gefitinibe/farmacologia , Humanos , Neoplasias Pulmonares/metabolismo , Neoplasias Pulmonares/patologia , Simulação de Acoplamento Molecular , Estrutura Molecular , Inibidores de Proteínas Quinases/síntese química , Inibidores de Proteínas Quinases/química , Quinazolinas/síntese química , Quinazolinas/química , Relação Estrutura-Atividade
14.
Water Res ; 135: 322-330, 2018 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-29486382

RESUMO

Recent research on contaminant removal by zerovalent iron (ZVI) has evolved from investigating simple model systems to systems that encompass increased dimensions of complexity. Sulfidation and aerobic conditions are two of the most broadly relevant complications. Combining these two, this study investigated the dynamic interactions between sulfidated microscale ZVI and dissolved O2, for removal of Cr(VI), a model contaminant for metals and metalloids. The results show that the coupling of sulfidation and oxygenation significantly improves Cr removal, which is attributed to enhanced Fe(II) production that resulted from accelerated corrosion of Fe(0). The Cr(VI) removal rate increased with increasing O2 saturation from 0% to 100% but showed a bimodal dependence on the S/Fe ratio. At the optimal S/Fe ratio, the ZVI exhibits a highly porous surface morphology, which, according to prior literature on sulfur induced corrosion, promotes corrosion. In addition, a novel time series correlation was developed between aqueous Fe(II) and Cr(VI) based on data collected in the presence and absence of 1,10-phenanthroline, to probe for changes of reductants during the reaction time course. The analysis indicated that Fe(0) was responsible for the initial small amount of Cr(VI) removal, which then transitioned to a phase controlled by surface Fe(II). The slopes of the time series correlations during the latter phase of the reaction vary with experimental conditions but are mostly much higher than the theoretical stoichiometric ratio between Cr(VI) and Fe(II) (i.e., 0.33), indicating that Fe(II) regeneration contributes significantly to Cr removal.


Assuntos
Cromatos/isolamento & purificação , Ferro/química , Oxigênio/química , Poluentes Químicos da Água/isolamento & purificação , Cromatos/química , Cromo/química , Cromo/isolamento & purificação , Análise de Séries Temporais Interrompida , Fenantrolinas/química , Sulfetos/química , Água/química , Poluentes Químicos da Água/química
15.
J Hazard Mater ; 343: 364-375, 2018 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-29017120

RESUMO

The co-precipitation method was used to synthesize a hybrid with MgAl-layered double hydroxide loaded graphene (RGO-LDH). CuMoO4 was then introduced onto the surface of RGO-LDH to prepare a hybrid with CuMoO4 modified RGO-LDH (RGO-LDH/CuMoO4). The composition, structure and morphology of RGO-LDH/CuMoO4 were characterized by X-ray diffraction, Laser raman spectroscopy and Transmission electron microscope-energy-dispersive X-ray spectroscopy. It was found that the hybrid of RGO-LDH/CuMoO4 had been successfully prepared. The effects of flame retardancy and smoke suppression of epoxy resin were studied with added RGO-LDH/CuMoO4. Results showed that the PHRR and THR of the EP composite with RGO-LDH/CuMoO4 added were decreased dramatically. The char yield, LOI and UL-94 vertical burning rating of the EP composite were increased, with improved flame ratardancy. In addition, the SPR, TSP, and Ds,max of the EP composite were decreased drastically with added RGO-LDH/CuMoO4. Its improved flame retardancy and smoke suppression performance were due mainly to the physical barrier of graphene and LDH, and the catalytic carbonization function of LDH. Meanwhile, Cu2O and MoO3 generated from RGO-LDH/CuMoO4 in the combustion process helped enhance the production of char residue and raised the compactness of the char layer.

16.
Environ Sci Technol ; 50(21): 11879-11887, 2016 11 01.
Artigo em Inglês | MEDLINE | ID: mdl-27684600

RESUMO

Applications of zerovalent iron (ZVI) for water treatment under aerobic conditions include sequestration of metals (e.g., in acid mine drainage) and decolorization of dyes (in wastewaters from textile manufacturing). The processes responsible for contaminant removal can be a complex mixture of reduction, oxidation, sorption, and coprecipitation processes, which are further complicated by the dynamics of oxygen intrusion, mixing, and oxide precipitation. To better understand such systems, the removal of an azo dye (Orange I) by micron-sized granular ZVI at neutral pH was studied in open (aerobic) stirred batch reactors, by measuring the kinetics of Orange I decolorization and changes in "geochemical" properties (DO, Fe(II), and Eh), with and without two treatments that might improve the long-term performance of this system: sulfidation by pretreatment with sulfide and magnetization by application of a weak magnetic field (WMF). The results show that the changes in solution chemistry are coupled to the dynamics of oxygen intrusion, which was modeled as analogous to dissolved oxygen sag curves. Both sulfidation and magnetization increased Orange I removal rates 2.4-71.8-fold, but there was little synergistic benefit to applying both enhancements together. Respike experiments showed that the enhancement from magnetization carries over from magnetization to sulfidation, but not the reverse.


Assuntos
Corantes , Ferro/química , Compostos Azo/química , Águas Residuárias , Purificação da Água
17.
Environ Sci Technol ; 50(3): 1483-91, 2016 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-26727297

RESUMO

Many oxyanion-forming metals (As, Sb, Se, Tc, etc.) can be removed from water by adsorption and/or redox reactions involving iron oxides, including the oxides associated with zerovalent iron (ZVI). The rate of antimonite (Sb(III) hydrolysis species) removal by ZVI was determined in open, well-mixed batch reactors as a function of experimental factors, including aging of the ZVI, addition of Fe(II), Sb dose, mixing rate, pH, initial concentrations of Sb(III), etc. However, the largest effect observed was the roughly 6-8 fold increase in Sb(III) removal rate due to the application of a weak magnetic field (WMF) during the experiments. The WMF effect on Sb removal arises from stimulated corrosion and delayed passivation of the ZVI, as evidenced by time series correlation analysis of "geochemical" properties (DO, Fetot, Eh, and pH) measured synchronously in each experiment. The removal of Sb under the conditions of this study was mainly due to oxidation of Sb(III) to Sb(V) and adsorption and coprecipitation onto the iron oxides formed from accelerated corrosion of ZVI, as evidenced by Sb K-edge XANES, EXAFS, and XPS. The degree of the WMF enhancement for Sb(III) was found to be similar to the WMF effect reported previously for Sb(V), As(III), As(V), and Se(VI).


Assuntos
Antimônio/química , Ferro/química , Poluentes Químicos da Água/química , Adsorção , Corrosão , Campos Magnéticos , Oxirredução
18.
Appl Microbiol Biotechnol ; 98(4): 1871-82, 2014 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-23949995

RESUMO

Oil reservoirs and production facilities are generally contaminated with H2S resulting from the activity of sulphidogenic prokaryotes (SRP). Sulphidogenesis plays a major role in reservoir souring and microbial influenced corrosion in oil production systems. In the present study, sulphidogenic microbial diversity and composition in saline production fluids retrieved from three blocks of corroding high temperature (79 ~ 95 °C) oil reservoirs with high sulfate concentrations were investigated by phylogenetic analyses of gene fragments of the dissimilatory sulfite reductase (dsr). Analysis of dsr gene fragments revealed the presence of several clusters of sulphidogenic prokaryotes that cover the orders Desulfovibrionales (Desulfovibrio, Desulfomicrobium thermophilum), Desulfobacterales (Desulfobacterium, Desulfosarcina, Desulfococcus, Desulfotignum, Desulfobotulus, Desulfobulbus), Syntrophobacterales (Desulfacinum, Thermodesulforhabdus, Desulforhabdus), Clostridiales (Desulfotomaculum) and Archaeoglobales (Archaeoglobus); among which sequences affiliated to members of Desulfomicrobium, Desulfotomaculum and Desulfovibrio appeared to be the most encountered genera within the three blocks. Collectively, phylogenetic and non-metric multidimensional scaling analyses indicated similar but structurally different sulphidogenic prokaryotes communities within the waters retrieved from the three Blocks. This study show the diversity and composition of sulphidogenic prokaryotes that may play a role in the souring mediated corrosion of the oilfield and also provides a fundamental basis for further investigation to control oil reservoir souring and corrosion of pipelines and topside installations.


Assuntos
Microbiologia da Água , Deltaproteobacteria/metabolismo , Sulfito de Hidrogênio Redutase/metabolismo , Petróleo , Bactérias Redutoras de Enxofre/metabolismo , Temperatura
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