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1.
Nature ; 613(7945): 667-675, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36697864

RESUMO

Continuous imaging of cardiac functions is highly desirable for the assessment of long-term cardiovascular health, detection of acute cardiac dysfunction and clinical management of critically ill or surgical patients1-4. However, conventional non-invasive approaches to image the cardiac function cannot provide continuous measurements owing to device bulkiness5-11, and existing wearable cardiac devices can only capture signals on the skin12-16. Here we report a wearable ultrasonic device for continuous, real-time and direct cardiac function assessment. We introduce innovations in device design and material fabrication that improve the mechanical coupling between the device and human skin, allowing the left ventricle to be examined from different views during motion. We also develop a deep learning model that automatically extracts the left ventricular volume from the continuous image recording, yielding waveforms of key cardiac performance indices such as stroke volume, cardiac output and ejection fraction. This technology enables dynamic wearable monitoring of cardiac performance with substantially improved accuracy in various environments.


Assuntos
Ecocardiografia , Desenho de Equipamento , Coração , Dispositivos Eletrônicos Vestíveis , Humanos , Débito Cardíaco , Ecocardiografia/instrumentação , Ecocardiografia/normas , Coração/diagnóstico por imagem , Ventrículos do Coração/diagnóstico por imagem , Volume Sistólico , Dispositivos Eletrônicos Vestíveis/normas , Pele
2.
Antimicrob Agents Chemother ; 68(5): e0115923, 2024 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-38506549

RESUMO

Vancomycin heteroresistance is prone to missed detection and poses a risk of clinical treatment failure. We encountered one clinical Enterococcus faecium strain, SRR12, that carried a complete vanM gene cluster but was determined as susceptible to vancomycin using the broth microdilution method. However, distinct subcolonies appeared within the clear zone of inhibition in the E-test assay, one of which, named SRR12-v1, showed high-level resistance to vancomycin. SRR12 was confirmed as heteroresistant to vancomycin using population analysis profiling and displayed "revive" growth curves with a lengthy lag phase of over 13 hours when exposed to 2-32 mg/L vancomycin. The resistant subcolony SRR12-v1 was found to carry an identical vanM gene cluster to that of SRR12 but a significantly increased vanM copy number in the genome. Long-read whole genome sequencing revealed that a one-copy vanM gene cluster was located on a pELF1-like linear plasmid in SRR12. In comparison, tandem amplification of the vanM gene cluster jointed with IS1216E was seated on a linear plasmid in the genome of SRR12-v1. These amplifications of the vanM gene cluster were demonstrated as unstable and would decrease accompanied by fitness reversion after serial passaging for 50 generations under increasing vancomycin pressure or without antibiotic pressure but were relatively stable under constant vancomycin pressure. Further, vanM resistance in resistant variants was verified to be carried by conjugative plasmids with variable sizes using conjugation assays and S1-pulsed field gel electrophoresis blotting, suggesting the instability/flexibility of vanM cluster amplification in the genome and an increased risk of vanM resistance dissemination.


Assuntos
Antibacterianos , Enterococcus faecium , Testes de Sensibilidade Microbiana , Família Multigênica , Plasmídeos , Resistência a Vancomicina , Vancomicina , Enterococcus faecium/genética , Enterococcus faecium/efeitos dos fármacos , Plasmídeos/genética , Vancomicina/farmacologia , Resistência a Vancomicina/genética , Antibacterianos/farmacologia , Proteínas de Bactérias/genética , Humanos , Sequenciamento Completo do Genoma
3.
Langmuir ; 40(18): 9579-9591, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38657205

RESUMO

Herein, a fiber-supported iron-based ionic liquid as a type of fibrous catalyst has been developed for the synthesis of bioactive 3,4-dihydropyrimidin-2-(1H)-ones (DHPMs) via three-component Biginelli reactions in a cleaner manner. The described fibrous catalyst was obtained from the commercially available polyetheretherketone (PEEK) fiber by postfunctionalization processes and was characterized and analyzed in detail by means of diversified technologies. Furthermore, the fiber-supported iron-based ionic liquids could mediate the classical three-component Biginelli reactions to proceed smoothly to gain a variety of substituted DHPMs with yields of up to 99%. The superior catalytic activities of the fibrous catalyst were ascribed to the quasi-homogeneous medium by ionic liquids generated in the surface layer of the PEEK fiber, which could afford an appropriate reaction zone and could further be available for the aggregation of substrates to facilitate the three-component reaction. Notably, the fibrous catalyst is available for recycling over 10 runs just by a pair of tweezers, and the operational procedure was capable of enlarging the catalytic system to the gram-scale without any performance degradation, which provided a cleaner manner to take advantage of the iron-based catalyst in organic synthesis with potential industrialization prospects.

4.
Angew Chem Int Ed Engl ; : e202401743, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38837598

RESUMO

Alkali metal borohydrides present a rich source of energy dense materials of boron and hydrogen, however their potential in propellants has been hitherto untapped. Potassium borohydride is a promising fuel with high gravimetric energy density and relatively low sensitivity to air and moisture. Problems arise due to the dehydrogenation of the borohydride on heating with minimal energy release. Common methods to extract both boron and hydrogen by means of borane species involve direct reaction of boron trifluoride species with alkali borohydrides. However, these methods face storage and safety issues due to rapid release of diborane on mixing the reactants. We propose a method of diborane release through controlled release of boron trifluoride by means of a tetrafluoroborate based ionic liquid. The trifluoride is released from the ionic liquid at elevated temperatures and enables safe mixture of the reactants at room temperature. It was found that the reaction between borohydride and boron trifluoride proceeds well above room temperature with potassium borohydride releasing diborane and potassium fluoride. The reaction pathway shows a primary reaction releasing diborane and potassium fluoride and a second less energy efficient step leading to the formation of potassium tetrafluoroborate. A 3d printed propellant formulation was also tested.

5.
Angew Chem Int Ed Engl ; 61(1): e202112511, 2022 Jan 03.
Artigo em Inglês | MEDLINE | ID: mdl-34709699

RESUMO

We demonstrate a new material by intercalating Mo3 S13 2- into Mg/Al layered double hydroxide (abbr. Mo3 S13 -LDH), exhibiting excellent capture capability for toxic Hg2+ and noble metal silver (Ag). The as-prepared Mo3 S13 -LDH displays ultra-high selectivity of Ag+ , Hg2+ and Cu2+ in the presence of various competitive ions, with the order of Ag+ >Hg2+ >Cu2+ >Pb2+ ≥Co2+ , Ni2+ , Zn2+ , Cd2+ . For Ag+ and Hg2+ , extremely fast adsorption rates (≈90 % within 10 min, >99 % in 1 h) are observed. Much high selectivity is present for Ag+ and Cu2+ , especially for trace amounts of Ag+ (≈1 ppm), achieving a large separation factor (SFAg/Cu ) of ≈8000 at the large Cu/Ag ratio of 520. The overwhelming adsorption capacities for Ag+ (qm Ag =1073 mg g-1 ) and Hg2+ (qm Hg =594 mg g-1 ) place the Mo3 S13 -LDH at the top of performing sorbent materials. Most importantly, Mo3 S13 -LDH captures Ag+ via two paths: a) formation of Ag2 S due to Ag-S complexation and precipitation, and b) reduction of Ag+ to metallic silver (Ag0 ). The Mo3 S13 -LDH is a promising material to extract low-grade silver from copper-rich minerals and trap highly toxic Hg2+ from polluted water.

6.
Bioprocess Biosyst Eng ; 44(6): 1119-1130, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33555380

RESUMO

The anode electrode of microbial fuel cell (MFC) is the key component to determine its power generation performance because it is the habitat and electron transfer center of the electricity-producing microorganisms. Carbon-based anodes have been confirmed to improve MFC performance. Its large surface area, excellent conductivity and low cost make it very suitable for electrode materials used in MFC. However, the low biocompatibility and instability of common carbon-based materials restrict their practical application in MFC. In this work, a bimetal oxide MnFe2O4 was prepared and used to modify carbon felt anode by a simple drop coating method. The influence of the amount of MnFe2O4 material on the performance of MFC was systematically studied. The results showed that the power density of the carbon felt anode with a MnFe2O4 modified amount of 1 mg/cm2 increased by 66.9% compared with the unmodified anode. Meanwhile, the MFC cycle using MnFe2O4 modified anode was more stable. After 6 months of long-term operation, the power density reached 3836 mW/m2. The anode modified by MnFe2O4 has capacitance characteristics, good biocompatibility and fast electron transmission rate, which significantly improves the power generation performance of MFC. In addition, the use of a simple drop coating method to prepare electrodes can reduce the difficulty of electrode fabrication and the cost of MFC, laying a certain foundation for the industrialization of MFC.


Assuntos
Fontes de Energia Bioelétrica , Carbono/química , Compostos Férricos/química , Compostos de Manganês/química , Eletrodos
7.
J Am Chem Soc ; 142(3): 1574-1583, 2020 01 22.
Artigo em Inglês | MEDLINE | ID: mdl-31855420

RESUMO

The new material Polypyrrole-Mo3S13 (abbr. Mo3S13-Ppy) is a new material prepared by ion-exchange between Ppy-NO3 and (NH4)2Mo3S13. The Mo3S13-Ppy was designed to exhibit strong selectivity for Ag+ and highly toxic Hg2+ in mixtures with other ions. It displays an apparent selectivity ranking of Hg2+ > Ag+ ≥ Co2+, Ni2+, Cu2+, Zn2+, Cd2+, and Pb2+. The strong affinity of Mo3S13-Ppy for Ag+ and Hg2+ was confirmed with extremely high distribution coefficients (Kd) (∼107 mL/g) and remarkable removal efficiencies (>99.99%), resulting in <1 ppb concentrations of these ions. Furthermore, Mo3S13-Ppy achieved excellent separation selectivity for Ag+ from Cu2+ (even at a high Cu2+/Ag+ ratio, the molar ratio of 867 and mass ratio of 500) because of the special structure of Mo3S132- and its component Mo4+ and (S2)2-. This is promising for the direct extraction of low-grade silver from copper-rich minerals. The maximum Ag uptake capacity of 408 mg/g is redox-based and surprisingly involves the deposition of large, millimeter sized, metallic silver (Ag0) crystals on the surface of Mo3S13-Ppy.

8.
Nanotechnology ; 31(3): 035403, 2020 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-31557753

RESUMO

The development of low-cost electrocatalysts with high performance is important to provide sustainable hydrogen energy. In this work, via one-step sulfuration of [Formula: see text] intercalated NiFe-layered double hydroxide (abbr. NiFe-MoO4-LDH), hierarchical microspheres are assembled by intersecting nanoplates (15-30 nm in thickness) which are then decorated with MoS2 and (NiFe)S x nanoparticles (∼25 nm in size). The NiFe-MoO4-LDH is synthesized beforehand by a one-pot hydrothermal reaction. Under sulfuration at 300 °C, 400 °C and 600 °C, the NiFe-MoO4-LDH transforms into multi-metal sulfides of NiFeMoS-T (T is applied temperature). During sulfuration, the confinement effect of LDH limits the growth of metal sulfides, causing formation of nanoparticles of MoS2 and (NiFe)S x to expose more catalytic active sites. In an alkaline medium, NiFeMoS-400 depicts superior performance for hydrogen evolution reaction (HER), giving an overpotential of 210 mV at 10 mA cm-2. A Tafel slope of 88 mV dec-1 indicates a mixed Volmer-Heyrovsky rate-determining step. The electrode also maintains long-term electrochemical durability during 15 h electrolysis at 25 mA cm-2. The NiFe-MoO4-LDH precursor owns three metal elements (Ni, Fe and Mo), which ensure the formation of polymetallic sulfides, and maximum utilization of the LDH layer and interlayer metals contributes to the optimal electrocatalytic activity. The NiFeMoS nanoassembly is a potential low-cost and high-efficiency electrocatalyst.

9.
Phys Chem Chem Phys ; 22(39): 22746-22757, 2020 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-33020777

RESUMO

Herein, a new type of lanthanide coordination polymer film made up of europium (Eu(iii)) and poly(N-methacryloylglycine) (Eu(iii)-PMAG) was prepared on an ITO electrode surface driven by the coordination between N-methacryloylglycine (MAG) and Eu(iii) through a single-step polymerization process. The fluorescence signal of Eu(iii)-PMAG films at 617 nm originating from Eu(iii) could be well retained in the buffer solution but was regulated by the concentration of Cu(ii) and the complexing agent EDTA. The switching of fluorescence by Cu(ii) was attributed to the inhibition of the "antenna effect" between Eu(iii) and the MAG ligand in the films. The coexistence of reduced ß-nicotinamide adenine dinucleotide (NADH) in the solution can apparently quench the fluorescence of Eu(iii)-PMAG films through the internal filtration effect of UV absorbance overlapping the excitation wavelength, but itself exhibiting a fluorescence emission at 468 nm. In addition, the electrocatalytic oxidation of NADH with the help of the ferrocenedicarboxylic acid (FcDA) probe demonstrated a cyclic voltammetry (CV) signal at 0.45 V (vs. SCE). Based on various reversible stimulus-responsive behaviours, a 4-input/10-output logic network was built using Cu(ii), EDTA, NADH and FcDA as inputs and the signals of fluorescence from Eu(iii)-PMAG (617 nm) and NADH (468 nm), the CV response from FcDA and the UV-vis absorbance from the Cu(ii)-EDTA complex as outputs. Meanwhile, 6 different functional logic devices were constructed based on the same versatile platform, including a 2-to-1 encoder, a 1-to-2 decoder, a 1-to-2 demultiplexer, a parity checker, a transfer gate and a reprogrammable 3-input/2-output keypad lock. Combined with the new type of lanthanide coordination polymer film, NADH played central roles in designing sophisticated computing systems with its fluorescence, UV and electrocatalytic properties. This work might provide a novel avenue to develop intelligent multi-analyte sensing and information processing at the molecular level based on one single platform.

10.
Emerg Infect Dis ; 25(1): 157-160, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30561317

RESUMO

We identified 2 methicillin-resistant Staphylococcus aureus strains of sequence type 398 from surgical site infections in China. Genetic analysis and clinical data from these strains suggested that they were human-related but sporadic. Hemolysis analysis and mouse-skin infection models indicated a high virulence potential for these strains.


Assuntos
Farmacorresistência Bacteriana/genética , Staphylococcus aureus Resistente à Meticilina/genética , Infecções Estafilocócicas/microbiologia , Infecção da Ferida Cirúrgica/microbiologia , Virulência/genética , Adulto , Animais , Antibacterianos/farmacologia , Técnicas de Tipagem Bacteriana , China , Feminino , Humanos , Masculino , Meticilina/farmacologia , Staphylococcus aureus Resistente à Meticilina/patogenicidade , Camundongos , Camundongos Endogâmicos BALB C , Camundongos Nus , Pessoa de Meia-Idade , Tipagem de Sequências Multilocus , Adulto Jovem
11.
Inorg Chem ; 58(8): 4979-4988, 2019 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-30933488

RESUMO

Tunable luminescence (quenching or blue shift) of HNA/OS-LRH composites (HNA is 3-hydroxy-2-naphthoic acid; OS is the anionic surfactant of 1-octanesulfonic acid sodium; LRHs are layered rare-earth hydroxides, R = Tb3+, Y3+) in the solid state and delaminated state is reported, which is utilized as an effective fluorescent probe for detecting metal ions. HNA/OS species are intercalated into LRH layers to generate composites of HNA xOS1- x-LTbH ( x = 0.10, 0.15, 0.20 , 0.25) and HNA yOS1- y-LYH ( y = 0.05, 0.10, 0.15, 0.20, 0.25, 0.30). In the solid state, LYH composites exhibit green emissions (from 493 to 504 nm) with a large blue shift in comparison to the 542 nm emission of free HNA- anions, while in the delaminated state in formamide (FM), the composites display blue emission (480 nm) relative to the green emission (512 nm) of an HNA soltuion in FM. However, LTbH composites display coquenched luminescence in both the solid state and delaminated state. Also, HNA0.25OS0.75-1:1-LYH, HNA0.25OS0.75-1:2-LYH, and HNA0.05OS0.95-1:1-LYH (1:1 and 1:2 are HNA:NaOH molar ratios) show significantly elongated fluorescence lifetimes of 15.35, 14.37, and 12.72 ns, respectively, in comparison with free HNA-Na (6.44 ns), and their quantum yields of 23.40%, 21.97%, and 22.31%, respectively, are much larger than that of free HNA-Na (4.86%). The LTbH composite (HNA0.25OS0.75-1:1-LTbH) has also a relatively higher quantum yield of 12.46%. The HNA0.25OS0.75-1:1-LYH colloid exhibits excellent recognition selectivity for Al3+ over other metal ions (Mg2+, Co2+, Ni2+, Cu2+, Zn2+, Pb2+, Cd2+, and Hg2+) with distinct fluorescence sensitization. It shows an intense change in its fluorescence emission when it is bound to Al3+ ions, giving a lower detection limit of 6.32 × 10-6 M. This is novel research on the fluorescence chemosensing of LRH composites.

12.
Phys Chem Chem Phys ; 21(44): 24572-24583, 2019 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-31663551

RESUMO

In this work, poly(N,N'-dimethylaminoethylmethacrylate-co-N-isopropylacrylamide) copolymer films were polymerized on the surface of Au electrodes with a facile one-step method, and Au nanoclusters (AuNCs) and tetraphenylethene (TPE) were synchronously embedded in the films, designated as P(DMA-co-NIPA)/AuNCs/TPE. Ferrocene dicarboxylic acid (FDA), an electroactive probe in solution displayed inverse pH- and SO42--sensitive on-off cyclic voltammetric (CV) behaviors at the film electrodes. The electrocatalytic oxidation of nicotinamide adenine dinucleotide (NADH) mediated by FDA in solution could substantially amplify the CV response difference between the on and off states. Moreover, the two fluorescence emission (FL) signals from the TPE constituent at 450 nm and AuNCs component at 660 nm in the films also demonstrated SO42-- and pH-sensitive behaviors. Based on the aforementioned results, a 4-input/9-output biomolecular logic circuit was constructed with pH, Na2SO4, FDA and NADH as the inputs, and the CV signals and the FL responses at 450 and 660 nm at different levels as the outputs. Additionally, some functional non-Boolean devices were elaborately designed on an identical platform, including a 1-to-2 decoder, a 2-to-1 encoder, a 1-to-2 demultiplexer and different types of keypad locks. This work combines copolymer films, bioelectrocatalysis, and fluorescence together so that more complicated biocomputing systems could be established. This work may pave a new way to develop advanced and sophisticated biocomputing logic circuits and functional devices in the future.


Assuntos
Técnicas Eletroquímicas/métodos , Nanopartículas Metálicas/química , NAD/química , Polímeros/química , Estilbenos/química , Benzoatos/química , Eletrodos , Compostos Ferrosos/química , Ouro/química , Concentração de Íons de Hidrogênio , Metalocenos , Oxirredução , Espectrometria de Fluorescência , Sulfatos/química
13.
Sensors (Basel) ; 18(10)2018 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-30297654

RESUMO

In this work, binary hydrogel films based on carboxylated multi-walled carbon nanotubes/poly(N,N-diethylacrylamide) (c-MWCNTs/PDEA) were successfully polymerized and assembled on a glassy carbon (GC) electrode surface. The electroactive drug probes matrine and sophoridine in solution showed reversible thermal-, salt-, methanol- and pH-responsive switchable cyclic voltammetric (CV) behaviors at the film electrodes. The control experiments showed that the pH-responsive property of the system could be ascribed to the drug components of the solutions, whereas the thermal-, salt- and methanol-sensitive behaviors were attributed to the PDEA constituent of the films. The CV signals particularly, of matrine and sophoridine were significantly amplified by the electrocatalysis of c-MWCNTs in the films at 1.02 V and 0.91 V, respectively. Moreover, the addition of esterase, urease, ethyl butyrate, and urea to the solution also changed the pH of the system, and produced similar CV peaks as with dilution by HCl or NaOH. Based on these experiments, a 6-input/5-output logic gate system and 2-to-1 encoder were successfully constructed. The present system may lead to the development of novel types of molecular computing systems.

14.
Sensors (Basel) ; 16(4)2016 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-27104542

RESUMO

The research on intelligent bioelectrocatalysis based on stimuli-responsive materials or interfaces is of great significance for biosensors and other bioelectronic devices. In the present work, lectin protein concanavalin A (Con A) and glycoenzyme glucose oxidase (GOD) were assembled into {Con A/GOD}n layer-by-layer (LbL) films by taking advantage of the biospecific lectin-glycoenzyme affinity between them. These film electrodes possess stimuli-responsive properties toward electroactive probes such as ferrocenedicarboxylic acid (Fc(COOH)2) by modulating the surrounding pH. The CV peak currents of Fc(COOH)2 were quite large at pH 4.0 but significantly suppressed at pH 8.0, demonstrating reversible stimuli-responsive on-off behavior. The mechanism of stimuli-responsive property of the films was explored by comparative experiments and attributed to the different electrostatic interaction between the films and the probes at different pH. This stimuli-responsive films could be used to realize active/inactive electrocatalytic oxidation of glucose by GOD in the films and mediated by Fc(COOH)2 in solution, which may establish a foundation for fabricating novel stimuli-responsive electrochemical biosensors based on bioelectrocatalysis with immobilized enzymes.


Assuntos
Técnicas Biossensoriais/métodos , Enzimas Imobilizadas/química , Glucose Oxidase/química , Glucose/isolamento & purificação , Biocatálise , Concanavalina A/química , Compostos Ferrosos/química , Glucose/química , Peroxidase do Rábano Silvestre/química , Concentração de Íons de Hidrogênio , Metalocenos , Oxirredução , Polímeros/química
15.
BMC Infect Dis ; 15: 161, 2015 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-25886859

RESUMO

BACKGROUND: Klebsiella pneumoniae has been the dominant pathogen for liver abscesses in several Asian countries. Although the prevalence of K. pneumoniae liver abscess (KLA) in mainland China is increasing recently, the clinical and microbiological characteristics of KLA in China have not been elucidated. METHODS: Clinical and microbiology characteristics of 45 consecutive patients with KLA from a tertiary teaching hospital in China between June 2008 and June 2012 were retrospectively evaluated. RESULTS: Vast majority of the strains were susceptible to main antimicrobial agents. Most of K. pneumoniae strains from pyogenic liver abscess patients belonged to K1/K2 serotype (68.9% for K1 serotype and 20% for K2 serotype). All K. pneumoniae strains were rmpA positive, and 68.9% of these strains were magA positive. Overall, 57.8% (26/45) of K. pneumoniae strains belonged to ST23. Twenty-five of 26 ST23 K. pneumoniae isolates (96.2%) from KLA patients were magA-positive and K1 serotype. Only 28.9% (13/45) of KLA isolates exhibited hypermucoviscous phenotype, which is clinically used as the characteristic of hypervirulent K. pneumoniae (hvKP). Liver abscess sizes in patients infected with hvKP were tend to be larger than those in patients infected with cKP. There was no significant association between the microbiological and clinical characteristics including serotypes, magA and rmpA genotypes, and STs with the metastatic infection and prognosis of KLA. CONCLUSIONS: Neither the serotypes, magA and rmpA genotypes, nor the STs of K. pneumoniae were associated with the metastatic infection and prognosis of KLA. However, further studies with larger sample are needed in the future.


Assuntos
Infecções por Klebsiella/microbiologia , Klebsiella pneumoniae/genética , Abscesso Hepático Piogênico/microbiologia , Adolescente , Adulto , China/epidemiologia , DNA Bacteriano/genética , Feminino , Genótipo , Humanos , Infecções por Klebsiella/epidemiologia , Klebsiella pneumoniae/classificação , Klebsiella pneumoniae/isolamento & purificação , Abscesso Hepático Piogênico/epidemiologia , Masculino , Pessoa de Meia-Idade , Prevalência , Estudos Retrospectivos , Sorogrupo , Adulto Jovem
16.
Chemosphere ; 362: 141752, 2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38508465

RESUMO

Microbial fuel cell (MFC) has attracted much attention in treating organic wastewater due to its double functions of degrading organics and generating electricity with microorganisms as biocatalysts. Unfortunately, some organics with biological toxicity such as acridine could inhibit the growth and activity of the microorganisms on the anode so that the double functions of MFC would recede. Enhancing microbial activity by using new biocompatible materials as anodes is prospective to solve problem. A novel anode was achieved by electrodepositing g-C3N4 sheets to the carbon felt (CF) modified with polyaniline-dopamine composite film, and used to treat wastewater containing acridine for the first time. After the operation of 13 d, MFC loading with the composite anode showed a degradation efficiency of 98.3% in 150 mg L-1 acridine, while that of CF-MFC was 55.8%. Moreover, MFC loading the modified anode obtained a maximum power density of 1976 ± 47 mW m-2, 140.1% higher than that of CF-MFC. Further analysis revealed that the functional microorganisms associated with acridine degradation such as Achromobacter and Alcaligenes were enriched on the g-C3N4/PANI-DA/CF anode. Moreover, the composite anode could improve the activity of microorganisms and elicit them to generate conductive nanowires, which was beneficial to transferring electrons from microbes to anode over long distances, suggesting a promising prospect application in MFC.

17.
Anal Chim Acta ; 1288: 342156, 2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38220288

RESUMO

BACKGROUND: Molecular shape selectivity, based on the size and shape parameters of the molecule, such as length and planarity, is a separation process that can be used for compounds with restricted shapes, such as isomers. The separation of geometric isomers is challenging because these compounds have similar physicochemical properties but differ slightly in molecular shape. The ability to separate and quantify these isomers is important in high performance liquid chromatography (HPLC), which is one of the most widely used techniques in separation science today, because the shape of the molecule has a strong influence on biological processes. RESULTS: We prepared symmetrical discoidal dendrimeric organomolecule gelators (GSDM) and o-phenylenediamine-derived low-molecular-weight dendrimeric organomolecule gelators (G1) and bonded them to silica surfaces. The dendritic organic compound-grafted silica (SiO2@GSDM and SiO2@G1) was used as HPLC stationary phases for the separation of shape-restricted isomers of polycyclic aromatic hydrocarbons (PAHs), carotenoids and tocopherols. The two phases exhibit a very high molecular shape selectivity compared to the commercially available alkyl phases. There are differences in molecular shape selectivity between the two stationary phases. Changes in the chemical structure of dendritic organic compounds can alter the orientation of the molecules, as well as changes in the molecular recognition ability. It was found that SiO2@GSDM has high molecular linear selectivity for PAHs at different temperatures, even at 50 °C. The planar selectivity of SiO2@GSDM was better for triphenylene and o-terphenyl benzenes compared to SiO2@G1. SIGNIFICANCE: This separation behavior may be attributed to the combined effect of weak interaction centers, which allowed the effective separation of bioactive and shape-restricted isomers through multiple interactions. Furthermore, SiO2@GSDM showed better separation of tocopherols and carotenoids, suggesting that the backbone and ordered structure of organic molecular gelators is an effective way to improve the shape selectivity of the molecules, whereas the molecular orientation of the functional groups influences the separation mechanism of the shape-restricted isomers.

18.
Environ Sci Pollut Res Int ; 31(25): 36849-36860, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38758436

RESUMO

A hydrothermal synthesis method was developed to produce high crystallinity ZSM-5 zeolite using coal gasification coarse slag (CGCS) as the raw material. Instead of the expensive NaOH(s.), Na2SiO3(s.) was utilized to activate, depolymerize, and recombine Si and Al elements in the CGCS. The mother liquor circulation technology was employed to recover and reuse raw materials and residual reagents (Na2SiO3(aq.) and TPABr), reducing waste emissions and enhancing resource utilization efficiency. The synthesized ZSM-5 had a specific surface area of 455.675 m2 g-1, pore volume of 0.284 cm3 g-1, and pore diameter of 2.496 nm. The influence of various factors on the morphology and crystallinity of ZSM-5 was investigated, resulting in the production of ZSM-5 with higher specific surface area and pore volume. Adsorption experiments showed that WU-ZSM-5 exhibited a removal efficiency of 85% for ammonia nitrogen (NH4+-N(aq.)), validating its effectiveness in coal chemical wastewater purification. The mother liquor recycling technology enabled zero-emission utilization of solid waste resources and improved the utilization rate of alkali and template to 90%. These results demonstrate the potential application of the developed method in the efficient treatment of coal chemical wastewater.


Assuntos
Carvão Mineral , Águas Residuárias , Zeolitas , Zeolitas/química , Águas Residuárias/química , Adsorção , Eliminação de Resíduos Líquidos/métodos , Purificação da Água/métodos
19.
Artigo em Inglês | MEDLINE | ID: mdl-37906218

RESUMO

The development of low-cost and high-efficiency iodine sorbents is of great significance for the control of nuclear pollution. In this work, we intercalate the tin sulfide cluster of [Sn2S6]4- to Mg/Al-type layered double hydroxides to obtain Sn2S6-LDH, which exhibits highly efficient capture performance of iodine vapor and iodine in solutions. The dispersion effect of the positively charged LDH layers contributes to the adequate exposure of [Sn2S6]4- anions, providing plentiful adsorption sites. For iodine vapor, Sn2S6-LDH showed an extremely large iodine capture capacity of 2954 mg/g with a large contribution from physisorption. For iodine in solutions, a significantly large sorption capacity of 1308 mg/g was achieved. During iodine capture, I2 molecules were reduced to I- ions (by S2- in [Sn2S6]4-), which then reacted with Sn4+ to form SnI4, where the molar amount of captured iodine is 4-fold that of Sn. Besides, the as-reduced I- combined with I2 again to generate [I3]-, which then entered the LDH interlayers to maintain electric neutrality. While reducing iodine, S2- itself in [Sn2S6]4- was oxidized to S8, which further combined with SnI4 to form a novel compound of SnI4(S8)2. The excellent iodine capture capability endows Sn2S6-LDH with a promising application in trapping radioactive iodine.

20.
J Mater Chem B ; 11(41): 9840-9866, 2023 10 25.
Artigo em Inglês | MEDLINE | ID: mdl-37822275

RESUMO

Nanozymes, nanomaterials possessing enzymatic activity, have been studied extensively by researchers. However, their complex composition, low density of active sites, and inadequate substrate selectivity have hindered the maturation and widespread acceptance of nanozymes. Single-atom nanozymes (SAzymes) with atomically dispersed active sites are leading the field of catalysis due to their exceptional performance. The maximum utilization rate of atoms, low cost, well-defined coordination structure, and active sites are the most prominent advantages of SAzymes that researchers favor. This review systematically categorizes SAzymes based on their support type and describes their specific applications. Additionally, we discuss regulation strategies for SAzyme activity and provide a comprehensive summary of biosafety challenges associated with these enzymes.


Assuntos
Nanoestruturas , Nanoestruturas/química , Catálise , Domínio Catalítico
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