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1.
Phys Med Biol ; 69(14)2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38955331

RESUMO

Objective.The trend in the medical field is towards intelligent detection-based medical diagnostic systems. However, these methods are often seen as 'black boxes' due to their lack of interpretability. This situation presents challenges in identifying reasons for misdiagnoses and improving accuracy, which leads to potential risks of misdiagnosis and delayed treatment. Therefore, how to enhance the interpretability of diagnostic models is crucial for improving patient outcomes and reducing treatment delays. So far, only limited researches exist on deep learning-based prediction of spontaneous pneumothorax, a pulmonary disease that affects lung ventilation and venous return.Approach.This study develops an integrated medical image analysis system using explainable deep learning model for image recognition and visualization to achieve an interpretable automatic diagnosis process.Main results.The system achieves an impressive 95.56% accuracy in pneumothorax classification, which emphasizes the significance of the blood vessel penetration defect in clinical judgment.Significance.This would lead to improve model trustworthiness, reduce uncertainty, and accurate diagnosis of various lung diseases, which results in better medical outcomes for patients and better utilization of medical resources. Future research can focus on implementing new deep learning models to detect and diagnose other lung diseases that can enhance the generalizability of this system.


Assuntos
Aprendizado Profundo , Processamento de Imagem Assistida por Computador , Pneumotórax , Pneumotórax/diagnóstico por imagem , Humanos , Processamento de Imagem Assistida por Computador/métodos , Tomografia Computadorizada por Raios X
2.
Ren Fail ; 46(2): 2359640, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38832483

RESUMO

Research has shown that patients undergoing hemodialysis experience seasonal variations in their serum potassium levels. There was inconsistent seasonal fluctuation in serum potassium levels among the hemodialysis population across different locations. In the form of narrative review for the first time, the article discusses the seasonal changes of serum potassium in this population and its potential reasons, this article demonstrates that it is primarily attributable to seasonal dietary potassium intake. However, existing studies have not quantified seasonal dietary potassium intake, so the results are still speculative. Furthermore, future research ought to further expound upon the clinical implications of seasonal variations in serum potassium levels among dialysis patients, as well as other influencing mechanisms such as the pathophysiological causes of these seasonal changes, particularly those pertaining to dietary, geographical, and regional factors. These findings contribute to a more thorough interpretation of laboratory results in hemodialysis patients and provide important guidance for their individualized dietary management.


Assuntos
Potássio , Diálise Renal , Estações do Ano , Humanos , Potássio/sangue , Falência Renal Crônica/terapia , Falência Renal Crônica/sangue , Potássio na Dieta/administração & dosagem
3.
Heliyon ; 10(9): e30023, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38726131

RESUMO

Primary spontaneous pneumothorax (PSP) primarily affects slim and tall young males. Exploring the etiological link between chest wall structural characteristics and PSP is crucial for advancing treatment methods. In this case-control study, chest computed tomography (CT) images from patients undergoing thoracic surgery, with or without PSP, were analyzed using Artificial Intelligence. Convolutional Neural Network (CNN) model of EfficientNetB3 and InceptionV3 were used with transfer learning on the Imagenet to compare the images of both groups. A heatmap was created on the chest CT scans to enhance interoperability, and the scale-invariant feature transform (SIFT) was adopted to further compare the image level. A total of 2,312 CT images of 26 non-PSP patients and 1,122 CT images of 26 PSP patients were selected. Chest-wall apex pit (CAP) was found in 25 PSP and three non-PSP patients (p < 0.001). The CNN achieved a testing accuracy of 93.47 % in distinguishing PSP from non-PSP based on chest wall features by identifying the existence of CAP. Heatmap analysis demonstrated CNN's precision in targeting the upper chest wall, accurately identifying CAP without undue influence from similar structures, or inappropriately expanding or minimizing the test area. SIFT results indicated a 10.55 % higher mean similarity within the groups compared to between PSP and non-PSP (p < 0.001). In conclusion, distinctive radiographic chest wall configurations were observed in PSP patients, with CAP potentially serving as an etiological factor linked to PSP. This study accentuates the potential of AI-assisted analysis in refining diagnostic approaches and treatment strategies for PSP.

4.
Environ Sci Technol ; 58(3): 1462-1472, 2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38155590

RESUMO

The 2021 WHO guidelines stress the importance of measuring ultrafine particles using particle number concentration (PNC) for health assessments. However, commonly used particle metrics such as aerodynamic diameter and number concentrations do not fully capture the diverse chemical makeup of complex particles. To address this issue, our study used high-throughput mass spectrometry to analyze the properties of cooking oil fumes (COFs) in real time and evaluate their impact on BEAS-2B cell metabolism. Results showed insignificant differences in COF number size distributions between soybean oil and olive oil (peak concentrations of 5.20 × 105/cm3), as well as between corn oil and peanut oil (peak concentrations of 4.35 × 105/cm3). Despite the similar major chemical components among the four COFs, variations in metabolic damage were observed, indicating that the relatively small amount of chemical components of COFs can also influence particle behavior within the respiratory system, thereby impacting biological responses. Additionally, interactions between accompanying gaseous COFs and particles may alter their chemical composition through various mechanisms, introducing additional chemicals and modifying existing proportions. Hence, the chemical composition and gaseous components of COFs hold equal importance to the particle number concentration (PNC) when assessing their impact on human health. The absence of these considerations in the current guidelines underscores a research gap. It is imperative to acknowledge that for a more comprehensive approach to safeguarding public health, guidelines must be regularly updated to reflect new scientific findings and robust epidemiological evidence.


Assuntos
Óleos , Material Particulado , Humanos , Material Particulado/análise , Culinária/métodos , Gases/análise , Alimentos
5.
Environ Sci Technol ; 57(51): 21593-21604, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-37955649

RESUMO

Decades of research have established the toxicity of soot particles resulting from incomplete combustion. However, the unique chemical compounds responsible for adverse health effects have remained uncertain. This study utilized mass spectrometry to analyze the chemical composition of extracted soot organics at three oxidation states, aiming to establish quantitative relationships between potentially toxic chemicals and their impact on human alveolar basal epithelial cells (A549) through metabolomics-based evaluations. Targeted analysis using MS/MS indicated that particles with a medium oxidation state contained the highest total abundance of compounds, particularly oxygen-containing polycyclic aromatic hydrocarbons (OPAHs) composed of fused benzene rings and unsaturated carbonyls, which may cause oxidative stress, characterized by the upregulation of three specific metabolites. Further investigation focused on three specific OPAH standards: 1,4-naphthoquinone, 9-fluorenone, and anthranone. Pathway analysis indicated that exposure to these compounds affected transcriptional functions, the tricarboxylic acid cycle, cell proliferation, and the oxidative stress response. Biodiesel combustion emissions had higher concentrations of PAHs, OPAHs, and nitrogen-containing PAHs (NPAHs) compared with other fuels. Quinones and 9,10-anthraquinone were identified as the dominant compounds within the OPAH category. This knowledge enhances our understanding of the compounds contributing to adverse health effects observed in epidemiological studies and highlights the role of aerosol composition in toxicity.


Assuntos
Poluentes Atmosféricos , Hidrocarbonetos Policíclicos Aromáticos , Compostos Policíclicos , Humanos , Compostos Policíclicos/análise , Fuligem/análise , Fuligem/química , Fuligem/toxicidade , Espectrometria de Massas em Tandem , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Pulmão , Oxigênio/análise , Metaboloma , Poluentes Atmosféricos/análise , Emissões de Veículos/análise
6.
Environ Sci Technol ; 57(49): 20460-20469, 2023 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-38019752

RESUMO

Biodiesel, derived from alkyl esters of vegetable oils or animal fats, has gained prominence as a greener alternative to diesel due to its reduced particle mass. However, it remains debatable whether biodiesel exposure has more severe health issues than diesel. This study performed high-resolution mass spectrometry to examine the detailed particle chemical compositions and lipidomics analysis of human lung epithelial cells treated with emissions from biodiesel and diesel fuels. Results show the presence of the peak substances of CHO compounds in biodiesel combustion that contain a phthalate ester (PAEs) structure (e.g., n-amyl isoamyl phthalate and diisobutyl phthalate). PAEs have emerged as persistent organic pollutants across various environmental media and are known to possess endocrine-disrupting properties in the environment. We further observed that biodiesel prevents triglyceride storage compared to diesel and inhibits triglycerides from becoming phospholipids, particularly with increased phosphatidylglycerols (PGs) and phosphatidylethanolamines (PEs), which potentially could lead to a higher probability of cancer metastasis.


Assuntos
Poluentes Atmosféricos , Emissões de Veículos , Animais , Humanos , Emissões de Veículos/análise , Biocombustíveis/análise , Metabolismo dos Lipídeos , Gasolina/análise , Poluentes Atmosféricos/análise
7.
Front Nutr ; 10: 1241580, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37693241

RESUMO

In this paper, we study the effect of microbial fermentation on the nutrient composition and flavor of sweet potato slurry, different strains of Aspergillus niger, Saccharomyces cerevisiae, Lactobacillus plantarum, Bacillus coagulans, Bacillus subtilis, Lactobacillus acidophilus, and Bifidobacterium brevis were employed to ferment sweet potato slurry. After 48 h of fermentation with different strains (10% inoculation amount), we compared the effects of several strains on the nutritional and functional constituents (protein, soluble dietary fiber, organic acid, soluble sugar, total polyphenol, free amino acid, and sensory characteristics). The results demonstrated that the total sugar level of sweet potato slurry fell significantly after fermentation by various strains, indicating that these strains can utilize the nutritious components of sweet potato slurry for fermentation. The slurry's total protein and phenol concentrations increased significantly, and many strains demonstrated excellent fermentation performance. The pH of the slurry dropped from 6.78 to 3.28 to 5.95 after fermentation. The fermentation broth contained 17 free amino acids, and the change in free amino acid content is closely correlated with the flavor of the sweet potato fermentation slurry. The gas chromatography-mass spectrometry results reveal that microbial fermentation can effectively increase the kinds and concentration of flavor components in sweet potato slurry, enhancing its flavor and flavor profile. The results demonstrated that Aspergillus niger fermentation of sweet potato slurry might greatly enhance protein and total phenolic content, which is crucial in enhancing nutrition. However, Bacillus coagulans fermentation can enhance the concentration of free amino acids in sweet potato slurry by 64.83%, with a significant rise in fresh and sweet amino acids. After fermentation by Bacillus coagulans, the concentration of lactic acid and volatile flavor substances also achieved its highest level, which can considerably enhance its flavor. The above results showed that Aspergillus niger and Bacillus coagulans could be the ideal strains for sweet potato slurry fermentation.

8.
ACS Appl Mater Interfaces ; 15(29): 34922-34930, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37459462

RESUMO

The graphite/lithium metal hybrid anode shows great potential for achieving high-specific-energy lithium batteries. Despite the "dead lithium" problem caused by repeated stripping and deposition of Li component based on a conversion reaction, the degradation mechanism, based on intercalation reaction, of graphite in a hybrid anode is generally ignored. In this contribution, through in situ X-ray diffraction and in situ Raman analysis, we reveal that hysteresis and the mixed-phase state of graphite during deintercalation play a critical role in hybrid battery degradation. On the other hand, we successfully mitigated graphite degradation and increased the reversible capacity of the hybrid anode by introducing an inorganic-rich solid electrolyte interface. Remarkably, the hybrid anode (30% higher specific capacity compared to graphite) exhibits an average coulombic efficiency of 99.11% and retains 96.13% of initial capacity over 120 cycles. This work sheds new light on the advancement of high-specific-energy lithium secondary batteries.

9.
Sci Total Environ ; 900: 165575, 2023 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-37499815

RESUMO

The ambient air quality of harbors area in Asia is commonly more polluted compared to other continents. The airborne pollutant is directly or indirectly related to a significant impact of traffic emissions. This study for the first time assessed the impacts on brown carbon (BrC) and volatile organic compounds (VOCs) from in-port liquid natural gas (LNG) tractor truck at harbor areas, via conducting real-time monitoring of VOCs characteristic and sampling for ambient air at a harbor (named as W harbor) in Shanghai, China, collecting emissions of in-port LNG tractor truck and miniCast in laboratory, as well as statistics of external container diesel trucks in the port for further validation. HPLC/DAD/Q-Tof MS was adopted for sample analysis. Results showed that many CHO compounds were associated with vehicle exhausts. Among of them, aliphatic CHO compounds with low degree of unsaturation were identified as fatty acids and fatty acid methyl esters extensively existing in fuel combustion emissions. And non-aliphatic CHO compounds characterized by low O/C ratios (<0.17) identified for the harbor air came from the emissions of in-port LNG power trucks with low-speed driving and idling. The ambient average non-methane total hydrocarbons (NMHC) concentration (0.59 ppm) at W harbor was much greater than that for other areas in Shanghai. The higher ratios of toluene/benzene (3.30) and m/p-xylene/ethylbenzene (3.11) observed at W harbor implied instead of external container diesel trucks, the dominating contributing of internal LNG tractor trucks to ambient VOCs cannot be neglected. This study concluded that LNG is not as clean as it was expected. The LNG-fueled vehicles can produce strong light-absorption chromophores as well as high concentration of VOCs.

10.
Nano Lett ; 23(11): 4908-4915, 2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37216428

RESUMO

The electrocatalytic conversion of polysulfides is crucial to lithium-sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo2O5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li-S batteries exhibit an impressive reversible capacity of 612 mAh g-1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li-S batteries.

11.
Environ Pollut ; 318: 120874, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36526053

RESUMO

Both brown carbon (BrC) and the non-absorbing components coated on black carbon (BC) aerosols can enhance the light absorption of BC aerosols. BrC is a complicated mixture of organic compounds and not well characterized, which hinders exploring the links between BrC and optical properties. We conducted an in-depth field study on optical properties of ambient aerosols at a monitoring site in Shanghai, China via real-time monitoring and offline analysis. Results showed that BrC caused light absorption coefficients were 3.3 ± 3.3 Mm-1, 2.2 ± 5.0 Mm-1, 1.2 ± 1.2 Mm-1 at λ = 370, 470 and 520 nm, respectively, accounting for 11%, 10%, 6% of the total aerosol absorption for the corresponding wavelengths. A larger proportion of long-chain aliphatic organosulfates (OSs, CnH2n+2O4S, (CH2)nO5S, (CH2)nO6S) with double bond equivalent (DBE) values of 0 or 1 accounted for 5-20% of the light absorption (λ = 365 nm) for soluble brown carbon (BrC), which were dominating for the days with less N-containing aromatic compounds appearing. Furthermore, the structure of CnH2n+2O4S, (CH2)nO5S, (CH2)nO6S were explored using target MS/MS of HPLC-Q-ToF-MS: (CH2)nO5S series, the most abundant family of OSs, were constructed by functionalizing a saturated hydrocarbon with one sulfate and one carbonyl group. CnH2n+2O4S series were oxidized with only one sulfate group in the aliphatic chain R. (CH2)nO6S series were proposed as aliphatic OSs with one ester group. We speculated aliphatic OSs were formed via acid catalyzed perhydrolysis of hydroperoxides derived from long-chain alkanes releasing from diesel fueled vehicles, followed by the reaction with sulfate anion radicals. Therefore, relevant technologies should be further explored to reduce the impacts from vehicle emissions.


Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , China , Carbono/análise , Espectrometria de Massas em Tandem , Monitoramento Ambiental/métodos , Aerossóis/análise , Sulfatos , Ésteres , Material Particulado/análise
12.
J Environ Sci (China) ; 127: 389-398, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36522070

RESUMO

Aldehyde and ketone compounds are ubiquitous in the air and prone to adverse effects on human health. Cooking emission is one of the major indoor sources. Aiming to evaluate health risks associated with inhalation exposure to aldehyde and ketone compounds, 13 carbonyl compounds (CCs) released from heating 5 edible oils, 3 seasonings, and 2 dishes were investigated in a kitchen laboratory. For the scenarios of heating five types of oil, aldehydes accounted for 61.1%-78.0% of the total emission, mainly acetaldehyde, acrolein and hexanal. Comparatively, heating oil with added seasonings released greater concentrations of aldehyde and ketone compounds. The concentration enhancement of larger molecular aldehydes was significantly greater. The emission factors of aldehyde and ketone compounds for cooking the dish of chili fried meat were much greater compared to that of tomato fried eggs. Therefore, food materials also had a great impact on the aldehyde and ketone emissions. Acetone and acetaldehyde were the most abundant CCs in the kitchen. Acrolein concentrations ranged from 235.18 to 498.71 µg/m3, which was about 100 times greater compared to the guidelines provided by Office of Environmental Health Hazard Assessment (OEHHA). The acetaldehyde inhalation for adults was 856.83-1515.55 µg and 56.23-192.79 µg from exposure to chili fried meat and tomato fried eggs, respectively. This exceeds the reference value of 90 µg/day provided by OEHHA. The findings of this study provided scientific evidences for the roles of cooking emissions on indoor air quality and human health.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Adulto , Humanos , Poluentes Atmosféricos/análise , Cetonas , Acroleína , Culinária , Poluição do Ar em Ambientes Fechados/análise , Aldeídos/análise , Acetaldeído , Monitoramento Ambiental
13.
ACS Nano ; 16(12): 20891-20901, 2022 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-36378080

RESUMO

For developing the reversible lithium metal anode, constructing an ideal solid electrolyte interphase (SEI) by regulating the Li+ solvation structure is a powerful way to overcome the major obstacles of lithium dendrite and limited Coulombic efficiency (CE). Herein, spherical mesoporous molecular sieve MCM-41 nanoparticles are coated on a commercial PP separator and used to regulate the Li+ solvation structure for lithium metal batteries (LMBs). The regulated solvation structure exhibits an agminated state with more contact ion pairs (CIPs) and ionic aggregates (AGGs), which successfully construct a homogeneous inorganic-rich SEI in the lithium anode. Meanwhile, the regulated solvation structure weakens the interaction between the solvents and Li+, resulting in low Li+ desolvation energy and uniform Li deposition. Thus, a high CE (∼96.76%), dendrite-free Li anode, and stable Li plating/stripping cycling for approximately 1000 h are achieved in the regulated carbonate-based electrolyte without any additives. Therefore, regulating the Li+ solvation structure in the electrolyte by employing a mesoporous material is a forceful way to construct an ideal SEI and harness lithium metal.

14.
Sci Total Environ ; 853: 158385, 2022 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-36055512

RESUMO

Cooking oil fume (COF) is an important source of indoor and outdoor air pollutants. COF generates a large number of organic compounds through volatilization and thermal oxidation, mainly including acids, alcohols, aldehydes and polycyclic aromatic hydrocarbons (PAHs), which can contribute 10 %-35 % to airborne organic particles in urban areas. COF not only affects human health owning to their small sizes, but also may absorb incident light due to the presence of brown carbon (BrC) chromophores in organic components. Therefore, we investigated size distributions and light absorption properties of particles produced from heating four types of edible oil. Results showed over 75 % of COF particles belonged to ultrafine particles (UFPs) and capable of absorbing light. The particle number size distributions for heating all edible oils were bimodal lognormal distribution, and the two mode diameters were within 27.9-32.2 nm and 187.7-299.6 nm. Both real-time monitoring and offline analyzing results show the average absorption coefficients of particles generated from heating soybean oil were much greater compare to those of heating other three edible oils. The mean AAE370/520 for heating soybean oil, olive oil, corn oil and peanut oil were 1.877, 1.669, 1.745 and 1.288, respectively, indicating the presence of BrC chromophores. A large proportion of BrC identified by HPLC-DAD-Q-TOF-MS only contain carbon, hydrogen and oxygen, which are CnH2nO2, CnH2n-2O2, CnH2n-4O2 and CnH2n-6O2 (9

Assuntos
Poluentes Atmosféricos , Hidrocarbonetos Policíclicos Aromáticos , Humanos , Material Particulado/análise , Calefação , Metanol , Óleo de Soja , Óleo de Milho , Azeite de Oliva , Óleo de Amendoim , Poluentes Atmosféricos/análise , Aerossóis/análise , Óleos , Gases , Carbono , Oxigênio , Hidrogênio , Aldeídos , Ácidos Graxos , Monitoramento Ambiental/métodos
15.
Chin Herb Med ; 14(1): 97-103, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36120128

RESUMO

Objective: The purpose of this study is to investigate the anti-diabetic effects of linarin, a flavonoid extracted from Chrysanthemi Indici Flos (CIF), and its potential mechanisms. Methods: The effects of linarin on cell viability and glucose consumption in HepG2 cells were measured. Meanwhile, monosodium glutamate (MSG) mouse model was constructed to monitor the changes of insulin tolerance, glucose tolerance, triglyceride and cholesterol. The protein expression levels of p-AMPK, p-ACC, PEPCK and p-GS were detected by Western blot. Results: Linarin could increase the relative glucose consumption of HepG2 cells, improve insulin tolerance and glucose tolerance, and decrease the levels of triglyceride and cholesterol of MSG mice. Simultaneously, the expression levels of p-AMPK and p-ACC in HepG2 cells and the liver tissue of MSG mice were increased, while the expression levels of PEPCK and p-GS were decreased after treatment with linarin. Conclusion: Insulin resistance could be ameliorated by linarin in type 2 diabetes, and its mechanism may be related to AMPK signaling pathway.

16.
Environ Technol ; : 1-9, 2022 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-35924754

RESUMO

A series of La-Ce-MnOx catalysts derived from the precipitation of acetate salt and ammonium carbonate were calcined at different temperatures and applied for the catalytic oxidation of soot from diesel exhausts. The structure states of the as-prepared catalysts and catalytic behaviour for soot oxidation were studied by many characterization techniques such as XRD, XANES, N2 adsorption-desorption, TPR, O2-TPD, XPS and TGA. XANES results display most Mn species are Mn4+ when the samples are calcined at 500 and 600°C. However, for MCLa-700 and MCLa-800 catalysts, the predominance valence is 3+ ions. The MCLa-500 and MCLa-600 catalysts possess higher concentrations of surface active oxygen evidenced by H2-TPR and soot-TPR. Therefore, the combustion rate of soot over MCLa-600 catalyst is remarkably increased with the T10, T50 and T90 at 318°C, 360°C and 388°C under NOx atmosphere respectively.

17.
Adv Mater ; 34(26): e2202222, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35534022

RESUMO

Defective materials have been demonstrated to possess adsorptive and catalytic properties in lithium-sulfur (Li-S) batteries, which can effectively solve the problems of lithium polysulfides (LiPSs) shuttle and sluggish conversion kinetics during charging and discharging of Li-S batteries. However, there is still a lack of research on the quantitative relationship between the defect concentration and the adsorptive-catalytic performance of the electrode. In this work, perovskites Sr0.9 Ti1- x Mnx O3- δ (STMnx ) (x = 0.1-0.3) with different oxygen-vacancy concentrations are quantitatively regulated as research models. Through a series of tests of the adsorptive property and electrochemical performance, a quantitative relationship between oxygen-vacancy concentration and adsorptive-catalytic properties is established. Furthermore, the catalytic mechanism of oxygen vacancies in Li-S batteries is investigated using density functional theory calculations and in situ experiments. The increased oxygen vacancies can effectively increase the binding energy between perovskite and LiPSs, reduce the energy barrier of LiPSs decomposition reaction, and promote LiPSs conversion reaction kinetics. Therefore, the perovskite STMn0.3  with high oxygen-vacancy concentrations exhibits excellent LiPSs adsorptive and catalytic properties, realizing high-efficiency Li-S batteries. This work is helpful to realize the application of the quantitative regulation strategy of defect engineering in Li-S batteries.

18.
Sci Total Environ ; 838(Pt 3): 156189, 2022 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-35618117

RESUMO

The molecular characteristics of organic aerosols (OAs) in heavily polluted areas affected by coal combustion (CC) were investigated. In terms of relative abundance, the total nitrogen-containing organic compounds (NOC) accounted for about 61%-68% of all molecules detected in methanol-soluble organic carbon (MSOC) by LC - Q-TOF - MS. More than 85% of the CHON- formulas are nitro-aromatic compounds, which are generally considered to be secondary organic compounds, as evidenced by the lower degree of overlap of these substances in the atmospheric samples and CC samples. Some polycyclic aromatic compounds with 4 N and 1-2O and very low H/C and O/C ratio produced by CC are unstable and easily react to form compounds with higher degrees of saturation. Almost all of the CHON+ homologues detected in the CC samples were also found in the atmospheric samples, indicating that the large amount of CHON+ compounds produced by CC are stable during atmospheric processes. The CHN+ compounds produced by CC contain a certain amount of highly unsaturated compounds, among which 1 N-containing polycyclic aromatic hydrocarbons (1 N-PAHs) is stable in atmosphere and can serve as markers of CC.


Assuntos
Poluentes Atmosféricos , Hidrocarbonetos Policíclicos Aromáticos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Carvão Mineral , Monitoramento Ambiental , Nitrogênio , Compostos de Nitrogênio , Compostos Orgânicos/análise , Hidrocarbonetos Policíclicos Aromáticos/análise
19.
ACS Appl Mater Interfaces ; 13(29): 34282-34291, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34282880

RESUMO

Reversible solid oxide cells (RSOCs) present a conceivable potential for addressing energy storage and conversion issues through realizing efficient cycles between fuels and electricity based on the reversible operation of the fuel cell (FC) mode and electrolysis cell (EC) mode. Reliable electrode materials with high electrochemical catalytic activity and sufficient durability are imperatively desired to stretch the talents of RSOCs. Herein, oxygen vacancy engineering is successfully implemented on the Fe-based layered perovskite by introducing Zr4+, which is demonstrated to greatly improve the pristine intrinsic performance, and a novel efficient and durable oxygen electrode material is synthesized. The substitution of Zr at the Fe site of PrBaFe2O5+δ (PBF) enables enlarging the lattice free volume and generating more oxygen vacancies. Simultaneously, the target material delivers more rapid oxygen surface exchange coefficients and bulk diffusion coefficients. The performance of both the FC mode and EC mode is greatly enhanced, exhibiting an FC peak power density (PPD) of 1.26 W cm-2 and an electrolysis current density of 2.21 A cm-2 of single button cells at 700 °C, respectively. The reversible operation is carried out for 70 h under representative conditions, that is, in air and 50% H2O + 50% H2 fuel. Eventually, the optimized material (PBFZr), mixed with Gd0.1Ce0.9O2, is applied as the composite oxygen electrode for the reversible tubular cell and presents excellent performance, achieving 4W and 5.8 A at 750 °C and the corresponding PPDs of 140 and 200 mW cm-2 at 700 and 750 °C, respectively. The enhanced performance verifies that PBFZr is a promising oxygen electrode material for the tubular RSOCs.

20.
Environ Sci Technol ; 54(23): 14889-14898, 2020 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-32790286

RESUMO

Light absorption enhancement (Eabs) of black carbon (BC) is a key factor in global climate models and is impacted by brown carbon (BrC) and the lensing effect of coatings. We conducted an in-depth field study on Eabs for ambient aerosols at a monitoring point in Shanghai, China, by real-time aerosol optical property monitoring and high-performance liquid chromatography/diode array detector/quadrupole-time-of-flight mass spectrometry (HPLC/DAD/Q-ToF-MS) analysis. The results showed Eabs at λ = 530 nm caused by the lensing effect was about 1.39 ± 027, accounting for 18.84% of the total light absorption. In this study, BrC is classified as soluble BrC (soluble in both water and methanol) or insoluble BrC (insoluble in both water and methanol). Soluble BrC accounted for 13.68 ± 11.15% of the total aerosol light absorption. For the first time, we concluded that insoluble BrC can contribute more than 60 and 97% of total aerosol and BrC light absorption in port cities, respectively. The molecular analysis of soluble BrC identified N-containing aromatic compounds (4-nitrophenol, 4-nitrocatechol, methyl nitrophenol, methyl nitrocatechols, and nitro-1-naphthol) commonly observed in biomass burning emissions or biomass burning-impacted atmospheres. A series of components (C16H26O3S, C17H28O3S, C18H30O3S, and C19H32O3S) were determined to be emissions from nearby cargo ships filled with heavy fuel oil (HFO), which further confirmed that insoluble BrC emitted from cargo ships could be the largest contributor to Eabs. This study confirms the global significance of evaluating HFO used in port cities in climate models. The control measures of cargo ship emission should be considered for the related environmental and health issues in port cities.


Assuntos
Poluentes Atmosféricos , Carbono , Aerossóis/análise , Poluentes Atmosféricos/análise , Carbono/análise , China , Cidades , Monitoramento Ambiental , Metanol , Água
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