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1.
Nat Nanotechnol ; 19(5): 638-645, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38649747

RESUMO

Perovskite quantum dots (QDs) are promising for various photonic applications due to their high colour purity, tunable optoelectronic properties and excellent solution processability. Surface features impact their optoelectronic properties, and surface defects remain a major obstacle to progress. Here we develop a strategy utilizing diisooctylphosphinic acid-mediated synthesis combined with hydriodic acid-etching-driven nanosurface reconstruction to stabilize CsPbI3 QDs. Diisooctylphosphinic acid strongly adsorbs to the QDs and increases the formation energy of halide vacancies, enabling nanosurface reconstruction. The QD film with nanosurface reconstruction shows enhanced phase stability, improved photoluminescence endurance under thermal stress and electric field conditions, and a higher activation energy for ion migration. Consequently, we demonstrate perovskite light-emitting diodes (LEDs) that feature an electroluminescence peak at 644 nm. These LEDs achieve an external quantum efficiency of 28.5% and an operational half-lifetime surpassing 30 h at an initial luminance of 100 cd m-2, marking a tenfold improvement over previously published studies. The integration of these high-performance LEDs with specifically designed thin-film transistor circuits enables the demonstration of solution-processed active-matrix perovskite displays that show a peak external quantum efficiency of 23.6% at a display brightness of 300 cd m-2. This work showcases nanosurface reconstruction as a pivotal pathway towards high-performance QD-based optoelectronic devices.

2.
Molecules ; 29(6)2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38542883

RESUMO

Due to the unique properties of room temperature ionic liquids (RTILs), most researchers' interest in RTIL-based electrolytes in electric double-layer capacitors (EDLCs) stems from molecular simulations, which are different from experimental scientific research fields. The knowledge of RTIL-based electrolytes in EDLCs began with a supposition obtained from the results of molecular simulations of molten salts. Furthermore, experiments and simulations were promoted and developed rapidly on this topic. In some instances, the achievements of molecular simulations are ahead of even those obtained from experiments in quantity and quality. Molecular simulations offer more information on the impacts of overscreening, quasicrowding, crowding, and underscreening for RTIL-based electrolytes than experimental studies, which can be helpful in understanding the mechanisms of EDLCs. With the advancement of experimental technology, these effects have been verified by experiments. The simulation prediction of the capacitance curve was in good agreement with the experiment for pure RTILs. For complex systems, such as RTIL-solvent mixtures and RTIL mixture systems, both molecular simulations and experiments have reported that the change in capacitance curves is not monotonous with RTIL concentrations. In addition, there are some phenomena that are difficult to explain in experiments and can be well explained through molecular simulations. Finally, experiments and molecular simulations have maintained synchronous developments in recent years, and this paper discusses their relationship and reflects on their application.

3.
Mol Ther Nucleic Acids ; 35(1): 102125, 2024 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-38356866

RESUMO

Hepatocellular carcinoma (HCC) is a common malignancy with poor prognosis. In recent years, immune checkpoint inhibitors (ICIs) have enabled breakthroughs in the clinical treatment of patients with HCC, but the overall response rate to ICIs in HCC patients is still low, and no validated biomarker is available to guide clinical decision making. Here, we demonstrated that the long non-coding RNA Lnc-CCNH-8 is highly expressed in HCC and correlates with poor prognosis. Functionally, elevated Lnc-CCNH-8 inactivated co-cultured T cells in vitro and compromised antitumor immunity in an immunocompetent mouse model. Mechanistically, up-regulated Lnc-CCNH-8 can sponge microRNA (miR)-217 to regulate the expression of PD-L1. In addition, Lnc-CCNH-8 can also stabilize PD-L1 through miR-3173/PKP3 axis. Furthermore, mice bearing tumors with high Lnc-CCNH-8 expression had significant therapeutic sensitivity to anti-PD-L1 monoclonal antibody treatment. More important, HCC patients with high levels of plasma exosomal Lnc-CCNH-8 had a better therapeutic response to ICIs. Taken together, our results reveal the function of Lnc-CCNH-8 in inducing immune escape from CD8+ T-cell-mediated killing by up-regulating PD-L1 in a miR-217/miR-3173-dependent manner, which also reveals a novel mechanism of PD-L1 regulation in HCC, and exosomal Lnc-CCNH-8 can serve as a predictive marker for immunotherapy response in HCC.

4.
Ann Hum Genet ; 88(4): 287-299, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38196279

RESUMO

BACKGROUND: Toll-like receptors (TLRs) are a family of transmembrane receptors that play key roles in identifying invading pathogens and activating innate immunity. TLR1 has been reported to be associated with the risk of gastric cancer (GC) but that was based on only a simple statistical analysis. METHODS: We genotyped the TLR1 in 526 GC patients to investigate the association between the variation and gastric cancer survival by the multiplex polymerase chain reaction and sequencing method. The rs4833095 variation (chr4:38798089 [GRCh38. p14], T > C) in the TLR1 gene was genotyped in 526 patients who underwent GC resection. The associations between genotype, survival, and recurrence were investigated. The potential role of TLR1 in stomach cancer was investigated using clinical data from formalin-fixed, paraffin-embedded tissue samples. RESULTS: Patients with the T/C and C/C genotypes of rs4833095 had a lower risk of recurrence than those with the T/T genotype. Recurrence-free periods were substantially longer in patients with the T/C or C/C genotypes (22.6 and 22.3 months, respectively) than in those with the T/T genotype (20.7 months). Patients with the T/C or C/C genotype, low expression levels of VEGF1, high expression levels of ERBB2 and ERCC1, the absence of cancer nodules, a tumor size of less than 5 cm, and poor differentiation had a considerably reduced risk of recurrence. CONCLUSIONS: TLR1 rs4833095 was correlated with the postresection prognosis of patients with gastric cancer, suggesting that TLR1 may have a role in the onset or progression of gastric cancer.


Assuntos
Adenocarcinoma , Recidiva Local de Neoplasia , Polimorfismo de Nucleotídeo Único , Neoplasias Gástricas , Receptor 1 Toll-Like , Humanos , Neoplasias Gástricas/genética , Neoplasias Gástricas/patologia , Masculino , Feminino , Pessoa de Meia-Idade , Receptor 1 Toll-Like/genética , Recidiva Local de Neoplasia/genética , Adenocarcinoma/genética , Adenocarcinoma/patologia , Idoso , Genótipo , Predisposição Genética para Doença , Adulto , Prognóstico
5.
J Environ Manage ; 352: 120094, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38237335

RESUMO

Soil texture is one of the most important indicators of soil physical properties, which has traditionally been measured through laborious procedures. Approaches utilizing visible near-infrared spectroscopy, with their advantages in efficiency, eco-friendliness and non-destruction, are emerging as potent alternatives. Nevertheless, these approaches often suffer from limitations in classification accuracy, and the substantial impact of spectral preprocessing, model integration, and sample matrix effect is commonly disregarded. Here a novel 11-class soil texture classification strategy that address this challenge by combining Multiplicative Scatter Correction (MSC) with Residual Network (ResNet) models was presented, resulting in exceptional classification accuracy. Utilizing the LUCAS dataset, collected by the Land Use and Cover Area frame Statistical Survey project, we thoroughly evaluated eight spectral preprocessing methods. Our findings underscored the superior performance of MSC in reducing spatial complexity within spectral data, showcasing its crucial role in enhancing model precision. Through comparisons of three 1D CNN models and two ResNet models integrated with MSC, we established the superior performance of the MSC-incorporated ResNet model, achieving an overall accuracy of 98.97 % and five soil textures even reached 100.00 %. The ResNet model demonstrated a marked superiority in classifying datasets with similar features, as observed by the confusion matrix analysis. Moreover, we investigated the potential benefit of pre-categorization based on land cover type of the soil samples in enhancing the accuracy of soil texture classification models, achieving overall classification accuracies exceeding 99.39 % for woodland, grassland, and farmland with the 2-layer ResNet model. The proposed work provides a pioneering and efficient strategy for rapid and precise soil texture identification via visible near-infrared spectroscopy, demonstrating unparalleled accuracy compared to existing methods, thus significantly enhancing the practical application prospects in soil, agricultural and environmental science.


Assuntos
Solo , Espectroscopia de Luz Próxima ao Infravermelho , Solo/química , Espectroscopia de Luz Próxima ao Infravermelho/métodos , Redes Neurais de Computação , Agricultura , Luz
6.
Front Hum Neurosci ; 17: 1298845, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38077186

RESUMO

Introduction: This study delves into the intricacies of emotional contagion and its impact on performance within dyadic interactions. Specifically, it focuses on the context of stereotype-based stress (SBS) during collaborative problem-solving tasks among female pairs. Through an exploration of emotional contagion, this study seeks to unveil its underlying mechanisms and effects. Methods: Leveraging EEG-based hyperscanning technology, we introduced an innovative approach known as the functional graph contrastive learning (fGCL), which extracts subject-invariant representations of neural activity patterns from feedback trials. These representations are further subjected to analysis using the dynamic graph classification (DGC) model, aimed at dissecting the process of emotional contagion along three independent temporal stages. Results: The results underscore the substantial role of emotional contagion in shaping the trajectories of participants' performance during collaborative tasks in the presence of SBS conditions. Discussion: Overall, our research contributes invaluable insights into the neural underpinnings of emotional contagion, thereby enriching our comprehension of the complexities underlying social interactions and emotional dynamics.

7.
ACS Nano ; 17(22): 22722-22732, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37955634

RESUMO

Aqueous Zn metal batteries are considered promising energy storage devices due to their high energy density and low cost. Unfortunately, such great potential is at present obscured by two clouds called dendrite growth and parasitic reactions. Herein, trace amounts of sodium cyclamate (CYC-Na) are introduced as an electrolyte additive, and accordingly, an atomic-pinning-induced interfacial solvation mechanism is proposed to summarize the effect of trace addition. Specifically, coadsorption of -NH- and -SO3 groups overcomes the ring-flipping effect and pins the CYC anion near the Zn anode surface in parallel, which significantly modifies the Zn2+ solvation sheath at the interface. This process homogenizes the surface Zn2+ flux and reduces the H2O and SO42- content on the surface, thus eliminating byproducts and leveling Zn deposition. Cells with trace CYC-Na cycle stably for 3650 h and still cycle for 330 h at high depths of discharge of 56.9%. This work dispels the clouds for efficient trace additives for AZMBs.

8.
Anal Chem ; 95(45): 16531-16538, 2023 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-37747740

RESUMO

Various vacuum ultraviolet (VUV) lamps are simple and convenient VUV light sources for mass spectrometry and other research fields. However, the strong absorption of high-energy photons by window materials limits the application of an extreme ultraviolet (EUV) light. In this study, a novel high-flux EUV light source is developed using a microchannel plate (MCP) window to transmit 73.6 nm (16.9 eV) EUV light generated via the radio frequency (RF) inductive discharge of neon. The MCP used is a 0.5 mm thick glass plate with a regular array of microtubes (12 µm i.d.). The photon fluxes of the EUV light source with the MCP window (12 mm i.d.) and an aperture (1.8 mm i.d.) are ∼1.31 × 1014 and ∼9.80 × 1012 photons s-1, respectively, while their corresponding leakage flow rates of the discharge gas are 0.062 and 0.046 cm3 atom s-1, according to the contrast experiments. The transmission efficiency of the MCP to the EUV light is 30.2%, with a 1.2% deviation. An EUV photoionization time-of-flight mass spectrometer (EUV-PI-TOFMS) is built to validate the practicality of the MCP-windowed EUV light source further. The detection sensitivities in 30 s measurements for methyl chloride (CH3Cl), methylene chloride (CH2Cl2), trichloromethane (CHCl3), and carbon tetrachloride (CCl4) in synthetic air are 4366, 4120, 5854, and 4095 counts ppbv-1, respectively. The corresponding 3σ limits of detection (LODs) are 42, 34, 24, and 15 pptv. This study develops a new feasible method for efficiently utilizing high-energy EUV light, with many application prospects in scientific research.

9.
Anal Methods ; 15(3): 368-376, 2023 01 19.
Artigo em Inglês | MEDLINE | ID: mdl-36597774

RESUMO

Photoionization mass spectrometry (PI-MS) has become a versatile tool in the real-time analysis of volatile organic compounds (VOCs) from the atmosphere or exhaled breath. However, some key species, e.g., acetonitrile, are hard to measure due to their higher ionization energies than photon energy. In this study, the direct and sensitive detection of gaseous acetonitrile based on a photoinduced associative ionization (PAI) reaction was investigated with a laboratory-built PAI time-of-flight mass spectrometer (PAI-TOFMS). By doping CH2Cl2 in the photoionization ion source, the mass signal of acetonitrile that cannot be effectively obtained by photoionization appeared with an extremely high intensity through the PAI reaction between acetonitrile, CH2Cl2, and residual H2O in the system. Though the moisture in the sample gas has an evident impact on the detection efficiency of acetonitrile, with a relative signal intensity decreasing from 100% under dry conditions to 60% at saturated relative humidity, excellent detection sensitivity was still obtained for gaseous acetonitrile in different matrixes. The sensitivity calibration experiment showed that the detection sensitivities of acetonitrile in N2 buffer gas, exhaled gas, and outdoor air were 682.4 ± 5.2, 17.0 ± 0.7, and 23.9 ± 0.2 counts pptv-1, respectively, with an analysis time of 10 s. The corresponding 3σ LODs reached 0.22, 8.82, and 6.28 pptv, which are equivalent to 0.40, 16.0, and 11.4 ng m-3. The performance of the PAI-TOFMS was first demonstrated by analyzing exhaled acetonitrile from healthy non-smokers and smokers and continuous monitoring of acetonitrile in outdoor air. In summary, this study provides a new and highly sensitive method for the real-time detection of acetonitrile through mass spectrometry.


Assuntos
Expiração , Compostos Orgânicos Voláteis , Espectrometria de Massas/métodos , Compostos Orgânicos Voláteis/análise , Fenômenos Químicos , Gases
10.
Chemosphere ; 308(Pt 1): 136300, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36064007

RESUMO

A novel gravity sedimentation - forward osmosis (G-FO) hybrid reactor was built up for separating and concentrating the biomass from the algal-rich water (microalgal dewatering). The extracellular organic matter (EOM) from Chlorella vulgaris (C. vulgaris) was divided into dissolved EOM (dEOM) and bound EOM (bEOM). Water flux, flux recovery rate and moisture content (MC) were investigated. Through sedimentation rate, zeta potential and hydrophilicity/hydrophobicity to analyze the experimental results. Scanning electronic microscopy (SEM) was used to observe the different morphologies of accumulated algae cells and EOM on the surface of the membrane. The results showed that cell + bEOM solution had the fastest sedimentation rate and fewest negative charge, so the pollutants accumulated more easily on the membrane surface, resulting in the highest flux decline. Its algal cake layer was the densest from the view of SEM. Cell + bEOM + dEOM solution had the lowest flux decline and the cake layer was the loosest. Cell + bEOM solution had the most severe irreversible fouling and the lowest flux recovery rate (FRR). The membrane fouling of cell solution was lower than that of cell + bEOM + dEOM solution, and the FRR of cell solution was almost 100%. According to the nonionic macro-porous resin fraction results of EOM, cell + bEOM + dEOM solution contained more hydrophilic components, resulting in the lowest MC. On the contrary, cell + bEOM solution showed the highest MC, which contained more hydrophobic components. Effects of bEOM and dEOM on microalgae dewatering performance of a novel gravity sedimentation - forward osmosis (G-FO) hybrid system were investigated, which provided a theoretical basis for large-scale application of FO technology for microalgae dewatering.


Assuntos
Chlorella vulgaris , Poluentes Ambientais , Microalgas , Purificação da Água , Membranas Artificiais , Osmose , Tecnologia , Água , Purificação da Água/métodos
11.
Talanta ; 247: 123558, 2022 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-35605514

RESUMO

Single-photon ionization mass spectrometry (SPI-MS) is an attractive analytical technique for the online detection of volatile organic compounds; however, the low photon flux of the vacuum ultraviolet (VUV) lamp commonly used in the SPI ion source and the corresponding low detection sensitivity remain a constraint to its wide field applications. In this study, a new VUV lamp-based SPI ion source was developed. By increasing the discharging volume and optimizing the configuration of the lens and ionizer, the photon flux of the VUV lamp and the sensitivity of the ion source were significantly improved. The VUV lamp output was 2.8 × 1015 photons s-1, which was focused into the small ionization zone, and the ion intensity of gaseous benzene under SPI achieved 1.7 × 104 counts per second per pptv (cps pptv-1). This ion source can also function in photoinduced associative ionization (PAI) mode by introducing gaseous CH2Cl2 to initiate an associative ionization reaction. Because of the high efficiency of the ion source, the amount of doped CH2Cl2 needed for PAI was greatly reduced (∼2.5% of that used in previous experiments). PAI exhibited an outstanding protonation effect on monosulfur ethers (CnH2n+1S). The signal intensities of the protonated molecular ions (MH+) were 46-128 times higher than those of the molecular ions (M+) produced by SPI. Since monosulfur ethers generally have lower SPI cross-sections than polysulfur ethers (CnH2n+1S2 or CnH2n+1S3), the PAI and SPI modes were selected for the online measurement of a series of mono- and polysulfur ethers, respectively. The obtained detection sensitivity of the mono- and polysulfur ethers reached 476.5 ± 1.72-2835.1 ± 99.5 and 47.9 ± 0.4-105.1 ± 2.3 counts pptv-1, respectively, in 10 s of sampling time. The corresponding 3σ limits of detection (LODs) were 0.12-0.71 and 0.06-0.14 pptv, respectively. This study provides advances in the development of a high-flux VUV lamp and a highly efficient SPI/PAI ion source, as well as an ultrasensitive analytical method for detecting sulfur ethers.


Assuntos
Sulfetos , Compostos Orgânicos Voláteis , Éteres , Espectrometria de Massas/métodos , Vácuo , Compostos Orgânicos Voláteis/análise
12.
Talanta ; 239: 123120, 2022 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-34864537

RESUMO

Pulmonary fibrosis (PF) is a common but fatal disease that threatens human health worldwide. Developing effective diagnostic methods is of great importance for the early detection of PF in patients. In this study, bleomycin (BLM) was used in mice to mimic idiopathic pulmonary fibrosis (IPF). The exhaled breath of BLM-induced PF, PF plus DDAH1 overexpression, and healthy control mice were analyzed in real-time using a newly developed associative ionization time-of-flight mass spectrometry method (AI-TOFMS), which is uniquely sensitive, especially to oxygenated volatile organic compounds (VOCs). Multivariate data analyses and discriminant modeling analyses revealed that four exhaled compounds, i.e., acrolein, ethanol, nitric oxide, and ammonia, had a strong correlation with PF symptoms. An Orthogonal Partial Least Square Discriminant Analysis (OPLS-DA) score plot showed an excellent separation between these three groups. The area under the receiver operating characteristic (ROC) curve for these four compounds distinguished PF mice from healthy controls at 0.989. In addition, the degrees of acute inflammation and fibrosis were assessed with Hematoxylin and Eosin (H&E) staining and Masson's Trichrome staining. Finally, combined with pathological characteristics and mRNA expression levels, the formation of the above-mentioned volatile compounds was explored. The obtained experimental results indicated that these four breath compounds, acrolein, ethanol, nitric oxide, and ammonia, were potential exhaled biomarkers for pulmonary fibrosis.


Assuntos
Bleomicina , Fibrose Pulmonar Idiopática , Animais , Biomarcadores , Testes Respiratórios , Expiração , Humanos , Fibrose Pulmonar Idiopática/induzido quimicamente , Fibrose Pulmonar Idiopática/diagnóstico , Espectrometria de Massas , Camundongos
13.
Talanta ; 235: 122788, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34517646

RESUMO

A thermal desorption associative ionization time-of-flight mass spectrometer was developed for ultrasensitive detection of semi-volatile chemical warfare agents (CWAs). The excited-state CH2Cl2-induced associative ionization method presented a soft ionization characterization and an excellent sensitivity towards CWAs. The detection sensitivities of the investigated nine CWA-related substances were 2.56 × 105-5.01 × 106 counts ng-1 in a detection cycle (30 s or 100 s). The corresponding 3σ limits of detection (LODs) were 0.08-3.90 pg. Compared with the best-documented LODs via the dielectric barrier discharge ionization (DBDI) and secondary electrospray ionization (SESI), the obtained LODs of the investigated compounds were improved by 2-76 times. Additionally, the measured sensitivity of 2-Chloroethyl ethyl, a proxy for mustard gas, is 550 counts pptv-1, which exceeds the DBDI and SESI's corresponding values (4.4 counts pptv-1 and 6.5 counts pptv-1) nearly by two orders of magnitude. A field application simulation was conducted by putting a strip of PTFE film contaminated with the CWA-related agent into the thermal desorption unit. The simulation showed that the sensitivities of the instrument via swipe surveying could achieve 2.19 × 105 to 5.23 × 106 counts ng-1. The experimental results demonstrate that the excited-state CH2Cl2-induced associative ionization is an ultrasensitive ionization method for CWAs and reveal a prospect for improving the detection of CWA species future.


Assuntos
Substâncias para a Guerra Química , Gás de Mostarda , Substâncias para a Guerra Química/análise , Limite de Detecção , Espectrometria de Massas , Gás de Mostarda/análise , Espectrometria de Massas por Ionização por Electrospray
14.
RSC Adv ; 11(62): 38949-38955, 2021 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-35492489

RESUMO

5-period ZnO/Zn0.9Mg0.1O multiple quantum wells (MQWs) were employed as active layers to fabricate the p-GaN/MQWs/n-ZnO diode by molecular beam epitaxy. It exhibited an efficient UV emission around 370 nm at room temperature. Calculated band structures and carrier distributions showed that electrons were restricted to overflow to the p-type layer, and carriers were confined in the high-quality MQWs well layer.

15.
J Colloid Interface Sci ; 579: 205-211, 2020 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-32592987

RESUMO

Novel two-dimensional silicon-based material siloxene has been synthesized handily by a one-step method, which utilizes the characteristics of the topological exfoliation to simplify the process of synthesis and modification. It is worth mentioning that for the first time amino-modified derivative has been investigated. Amino modification can promote the oxidation of siloxene, enlarge the bandgap and extend the carrier lifetime of siloxene. The application of siloxene before and after modification in water-splitting has been investigated. In addition, the superiority of the resultant two-dimensional materials was concisely elaborated, which revealed that owing to more effective photogenerated carriers' separation in amino modification siloxene, hydrogen production could be greatly promoted.

16.
Oncol Lett ; 19(5): 3389-3399, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32269611

RESUMO

The potential for non-invasive lung cancer (LC) diagnosis based on molecular, cellular and volatile biomarkers has been attracting increasing attention, with the development of advanced techniques and methodologies. It is standard practice to tailor the treatments of LC for certain specific genetic alterations, including the epidermal growth factor receptor, anaplastic lymphoma kinase and BRAF genes. Despite these advances, little is known about the internal mechanisms of different types of biomarkers and the involvement of their related biochemical pathways during the development of LC. The development of faster and more effective techniques is essential for the identification of different biomarkers. The present review summarizes some of the latest methods used for detecting molecular, cellular and volatile biomarkers in LC and their potential use in clinical diagnosis and targeted therapy.

17.
J Biomed Sci ; 27(1): 37, 2020 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-32093695

RESUMO

BACKGROUND: Aerobically-grown bacteria can be challenged by hydrogen peroxide stress from endogenous aerobic metabolism and exogenously generated reactive oxygen species. Catalase (Kat), alkyl hydroperoxidase (Ahp), and glutathione peroxidase (Gpx) systems are major adaptive responses to H2O2 stress in bacteria. Stenotrophomonas maltophilia is a ubiquitous Gram-negative bacterium equipped with four Kats (KatA1, KatA2, KatMn, and KatE), one Ahp (AhpCF), and three Gpxs (Gpx1, Gpx2, and Gpx3). Here, we systematically investigated how the eight H2O2 scavenging genes differentially contribute to the low-micromolar levels of H2O2 generated from aerobic metabolism and high-millimolar levels of H2O2 from exogenous sources. METHODS: Gene expression was assessed and quantified by reverse transcription-PCR (RT-PCR) and real time quantitative PCR (qRT-PCR), respectively. The contribution of these enzymes to H2O2 stress was assessed using mutant construction and functional investigation. RESULTS: Of the eight genes, katA2, ahpCF, and gpx3 were intrinsically expressed in response to low-micromolar levels of H2O2 from aerobic metabolism, and the expression of katA2 and ahpCF was regulated by OxyR. AhpCF and KatA2 were responsible for alleviating aerobic growth-mediated low concentration H2O2 stress and AhpCF played a critical role for stationary-phase cells. KatA2 was upregulated to compensate for AhpCF in the case of ahpCF inactivation. After exposure to millimolar levels of H2O2, katA2 and ahpCF were upregulated in an OxyR-dependent manner. KatA2 was the critical enzyme for dealing with high concentration H2O2. Loss-of-function of KatA2 increased bacterial susceptibility to high concentration H2O2. CONCLUSIONS: AhpCF and KatA2 are key enzymes protecting S. maltophilia from hydrogen peroxide stress.


Assuntos
Proteínas de Bactérias/genética , Peróxido de Hidrogênio/metabolismo , Estresse Oxidativo/genética , Espécies Reativas de Oxigênio/metabolismo , Stenotrophomonas maltophilia/genética , Proteínas de Bactérias/metabolismo , Stenotrophomonas maltophilia/metabolismo
18.
Environ Geochem Health ; 42(3): 809-818, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30993498

RESUMO

Seasonal algal bloom, a water supply issue worldwide, can be efficiently solved by membrane technology. However, membranes typically suffer from serious fouling, which hinders the wide application of this technology. In this study, the feasibility of adding Ca2+ to control membrane fouling in coagulation-membrane treatment of algal-rich water was investigated. According to the results obtained, the normalized membrane flux decreased by a lower extent upon increasing the concentration of Ca2+ from 0 to 10 mmol/L. Simultaneously, the floc particle size increased significantly with the concentration of Ca2+, which leads to a lower hydraulic resistance. The coagulation performance is also enhanced with the concentration of Ca2+, inducing a slight osmotic pressure-induced resistance. The formation of Ca2+ coagulation flocs resulted in a looser, thin, and permeable cake layer on the membrane surface. This cake layer rejected organic pollutants and could be easily removed by physical and chemical cleaning treatments, as revealed by scanning electron microscopy images. The hydraulic irreversible membrane resistance was significantly reduced upon addition of Ca2+. All these findings suggest that the addition of Ca2+ may provide a simple-operation, cost-effective, and environmentally friendly technology for controlling membrane fouling during coagulation-membrane process for algal-rich water treatment.


Assuntos
Cálcio/química , Eutrofização , Ultrafiltração/instrumentação , Purificação da Água/instrumentação , Purificação da Água/métodos , Membranas Artificiais , Microcystis/química , Microscopia Eletrônica de Varredura , Pressão Osmótica , Tamanho da Partícula , Ultrafiltração/métodos , Poluentes Químicos da Água/química
19.
Anal Chem ; 91(9): 5605-5612, 2019 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-30841695

RESUMO

Excited-state CH2Cl2-induced associative ionization (AI) is a newly developed ionization method that is very effective for oxygenated organics. However, this method is not widely known. In this study, an unprecedented ionization efficiency and ultrafast reaction rate of AI toward nitro compounds were observed. The ionization efficiencies of o-nitrotoluene (o-NT), m-nitrotoluene (m-NT), and nitrobenzene (NB) were as high as (28 ± 3)%, (27 ± 2)%, and (13 ± 1)%, respectively (∼1-3 ions for every 10 molecules). The measured reaction rate coefficients of these nitroaromatics were (0.5-1.3) × 10-7 molecule-1 cm3 s-1 (∼300 K). These unusual rate coefficients indicated strong long-range interactions between the two neutral reactants, which was regarded as a key factor leading to the ultrahigh ionization efficiency. The detection sensitivities of the nitroaromatics, (1.01-2.16) × 104 counts pptv-1 in 10 s acquisition time, were obtained by an AI time-of-flight mass spectrometer (AI-TOFMS). These experimental results not only provide new insight into the AI reaction but also reveal an excellent ionization method that can improve the detection sensitivity of nitroaromatics to an unprecedented degree.

20.
Environ Pollut ; 245: 20-28, 2019 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-30408761

RESUMO

Despite extensive effort to characterize xylene-isomer-derived secondary organic aerosols (SOAs) over the past decade, differences in SOA composition among xylene isomers, and their relative contributions to SOA formation remain poorly understood. Herein, we reinvestigated the photooxidation of o-, m-, and p-xylene under two limiting NO conditions. Dicarbonyls, TBM (the acronym of C3-trione, 2,3-butanedione, and 3-methyl-2-oxiranecarbaldehyde with the same [M+H]+m/z value of 87), and highly oxidized species (HOS), based on the m/z 61 fragment, were determined to be the predominant SOA components arising from xylene photooxidation; however, their relative contributions to SOA formation appear to depend on the xylene substitution pattern. In the initial stages of the reaction, dicarbonyls present in the SOA from m- and p-xylene, and TBM in the SOA from o-xylene, were the main contributors to new particle formation (NPF). Based on their significant levels of formation, HOS and TBM were characterized to be critical components that enhance SOA growth. High NO levels were noted to inhibit the formation of C3-trione and 2,3-butanedione in the SOA from m- and o-xylene, whereas the formation of 3-methyl-2-oxiranecarbaldehyde during p-xylene photooxidation was significantly promoted. These results reveal that the substitution pattern of the xylene isomer is a significant factor that determines these differences. In addition, decreases in the levels of dicarbonyls and TBM during NPF and the formation of HOS in the presence of high levels of NO may be important factors that lead to lower SOA yields compared to those obtained under low-NO conditions. This work contributes to a better understanding of the formation mechanism of xylene-derived SOAs.


Assuntos
Aerossóis/química , Processos Fotoquímicos , Xilenos/química , Poluentes Atmosféricos/análise , Oxirredução
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