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1.
J Environ Sci (China) ; 147: 561-570, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39003071

RESUMO

In the present study, we investigated the influence of surface fluorine (F) on TiO2 for the photocatalytic oxidation (PCO) of toluene. TiO2 modified with different F content was prepared and tested. It was found that with the increasing of F content, the toluene conversion rate first increased and then decreased. However, CO2 mineralization efficiency showed the opposite trend. Based on the characterizations, we revealed that F substitutes the surface hydroxyl of TiO2 to form the structure of Ti-F. The presence of the appropriate amount of surface Ti-F on TiO2 greatly enhanced the separation of photogenerated carriers, which facilitated the generation of ·OH and promoted the activity for the PCO of toluene. It was further revealed that the increase of only ·OH promoted the conversion of toluene to ring-containing intermediates, causing the accumulation of intermediates and then conversely inhibited the ·OH generation, which led to the decrease of the CO2 mineralization efficiency. The above results could provide guidance for the rational design of photocatalysts for toluene oxidation.


Assuntos
Fluoretos , Oxirredução , Titânio , Tolueno , Tolueno/química , Titânio/química , Catálise , Fluoretos/química , Processos Fotoquímicos , Modelos Químicos
2.
J Environ Sci (China) ; 146: 226-236, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38969450

RESUMO

Defluoridation of coal mining water is of great significance for sustainable development of coal industry in western China. A novel one-step mechanochemical method was developed to prepare polymeric aluminum modified powder activated carbon (PAC) for effective fluoride removal from coal mining water. Aluminum was stably loaded on the PAC through facile solid-phase reaction between polymeric aluminum (polyaluminum chloride (PACl) or polyaluminum ferric chloride (PAFC)) and PAC (1:15 W/W). Fluoride adsorption on PACl and PAFC modified PAC (C-PACl and C-PAFC) all reached equilibrium within 5 min, at rate of 2.56 g mg-1 sec-1 and 1.31 g mg-1 sec-1 respectively. Larger increase of binding energy of Al on C-PACl (AlF bond: 76.64 eV and AlFOH bond: 77.70 eV) relative to that of Al on C-PAFC (AlF bond: 76.52 eV) explained higher fluoride uptake capacity of C-PACl. Less chloride was released from C-PACl than that from C-PAFC due to its higher proportion of covalent chlorine and lower proportion of ionic chlorine. The elements mapping and atomic composition proved the stability of Al loaded on the PAC as well as the enrichment of fluoride on both C-PACl and C-PAFC. The Bader charge, formation energy and bond length obtained from DFT computational results explained the fluoride adsorption mechanism further. The carbon emission was 7.73 kg CO2-eq/kg adsorbent prepared through mechanochemical process, which was as low as 1:82.3 to 1:8.07 × 104 compared with the ones prepared by conventional hydrothermal methods.


Assuntos
Carvão Vegetal , Minas de Carvão , Fluoretos , Poluentes Químicos da Água , Fluoretos/química , Poluentes Químicos da Água/química , Carvão Vegetal/química , Adsorção , Alumínio/química , Polímeros/química , Purificação da Água/métodos , Eliminação de Resíduos Líquidos/métodos
3.
Environ Sci Pollut Res Int ; 31(31): 44348-44360, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38951394

RESUMO

Aluminum electrolyte is a necessity for aluminum reduction cells; however, its stock is rising every year due to several factors, resulting in the accumulation of solid waste. Currently, it has become a favorable material for the resources of lithium, potassium, and fluoride. In this study, the calcification roasting-two-stage leaching process was introduced to extract lithium and potassium separately from aluminum electrolyte wastes, and the fluoride in the form of CaF2 was recycled. The separation behaviors of lithium and potassium under different conditions were investigated systematically. XRD and SEM-EDS were used to elucidate the phase evolution of the whole process. During calcification roasting-water leaching, the extraction efficiency of potassium was 98.7% under the most suitable roasting parameters, at which the lithium extraction efficiency was 6.6%. The mechanism analysis indicates that CaO combines with fluoride to form CaF2, while Li-containing and K-containing fluorides were transformed into water-insoluble LiAlO2 phase and water-soluble KAlO2 phase, respectively, thereby achieving the separation of two elements by water leaching. In the second acid-leaching stage, the extraction efficiency of lithium was 98.8% from water-leached residue under the most suitable leaching conditions, and CaF2 was obtained with a purity of 98.1%. The present process can provide an environmentally friendly and promising method to recycle aluminum electrolyte wastes and achieve resource utilization.


Assuntos
Alumínio , Fluoretos , Lítio , Potássio , Fluoretos/química , Lítio/química , Alumínio/química , Potássio/química , Eletrólitos/química , Reciclagem
4.
Water Sci Technol ; 90(1): 32-44, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-39007305

RESUMO

Developing a feasible and low-cost strategy for the recovery of calcium fluoride efficiently from fluoride-containing wastewater is very essential for the recycle of fluoride resources. Herein, a modified lime precipitation method was employed to recover CaF2 from fluorinated wastewater using a special icy lime solution. Intriguingly, the highest F- removal was greater than 95% under the optimal condition, leaving a fluoride concentration from 200 to 8.64 mg/L, while the lime dosage was much lower than that of industry. Importantly, spherical-shaped CaF2 particles with a 93.47% purity and size smaller than 600 nm were recovered, which has a high potential for the production of hydrofluoric acid. Besides, the precipitation was significantly affected by Ca/F molar ratio, stirring time, temperature, and solution pH. Furthermore, the thermodynamics and kinetics were investigated in detail to reveal the crystallization process. As a result, the defluorination reaction followed the pseudo-second order reaction kinetics model. Also, CO2 in the air adversely influenced the CaF2 purity. Based on this facile method, a high lime utilization efficiency was applied to defluorination, which contributed to protecting the environment and saving costs. This study, therefore, provides a feasible approach for the green recovery of fluorine resources and has significance for related research.


Assuntos
Compostos de Cálcio , Fluoreto de Cálcio , Flúor , Óxidos , Águas Residuárias , Fluoreto de Cálcio/química , Águas Residuárias/química , Flúor/química , Compostos de Cálcio/química , Óxidos/química , Poluentes Químicos da Água/química , Eliminação de Resíduos Líquidos/métodos , Fluoretos/química
5.
Clin Oral Investig ; 28(8): 430, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-39012388

RESUMO

OBJECTIVES: This in vitro study examined the marginal integrity of experimental composite materials doped with bioactive glass (BG). MATERIALS AND METHODS: Class-II MOD cavities were prepared and restored with one of the following composite materials: a commercial composite material as a reference (Filtek Supreme XTE), an experimental composite doped with BG 45S5 (C-20), and an experimental composite doped with a fluoride-containing BG (F-20). Six experimental groups (n = 8) were used, as each of the three composites was applied with (+) or without (-) a universal adhesive (Adper Scotchbond Multipurpose). All specimens were subjected to thermocycling (10,000 x, 5-55 °C) and then additionally stored in artificial saliva for eight weeks. Scanning electron micrographs of the mesial and the distal box were taken at three time points (initial, after thermocycling, and after eight weeks of storage in artificial saliva). The margins were classified as "continuous" and "non-continuous" and the percentage of continuous margins (PCM) was statistically analyzed (α = 0.05). RESULTS: In most experimental groups, thermocycling led to a significant decrease in PCM, while the additional 8-week aging had no significant effect. F-20 + performed significantly better (p = 0.005) after 8 weeks storage in artificial saliva than the reference material with adhesive, while no statistically significant differences were observed at the other two time points. C-20 + exhibited significantly better PCM than the reference material with adhesive after thermocycling (p = 0.026) and after 8 weeks (p = 0.003). CONCLUSIONS: Overall, the experimental composites with BG showed at least as good marginal adaptation as the commercial reference, with an indication of possible re-sealing of marginal gaps. CLINICAL RELEVANCE: Maintaining or improving the marginal integrity of composite restorations is important to prevent microleakage and its likely consequences such as pulp irritation and secondary caries.


Assuntos
Resinas Compostas , Adaptação Marginal Dentária , Restauração Dentária Permanente , Vidro , Teste de Materiais , Microscopia Eletrônica de Varredura , Saliva Artificial , Propriedades de Superfície , Resinas Compostas/química , Técnicas In Vitro , Vidro/química , Restauração Dentária Permanente/métodos , Saliva Artificial/química , Humanos , Preparo da Cavidade Dentária , Cerâmica/química , Cimentos de Resina/química , Fluoretos/química
6.
Clin Oral Investig ; 28(8): 435, 2024 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-39028340

RESUMO

OBJECTIVES: This study aimed to synthesize and characterize colloidal chitosan-silver nanoparticles-fluoride nanocomposite (CCAgNPF) and evaluate its efficacy compared to chlorhexidine on salivary Streptococcus mutans in orthodontic patients. MATERIALS AND METHODS: AgNPs stabilized with chitosan were synthesized by chemical reduction of AgNO3. The nanoparticles were characterized with SEM, FTIR, DLS and ICP-OES. The MIC and MBC against S. mutans and IC50 concentration of CCAgNPF were obtained for antibacterial and cytotoxicity evaluations, respectively. For the clinical study, a total of 45 orthodontic patients were divided into three groups of 15 and used the following mouthwashes twice a day for 1 month: CCAgNPF, chlorhexidine 0.2% and the combination of these mouthwashes. The colony count of salivary S. mutans was evaluated before and after using the mouthwashes. The data were analyzed using One-way ANOVA and Tukey's test. RESULTS: Stabilized AgNPs were spherical with a diameter of 25.3 ± 3.3 nm. The MIC, MBC and IC50 of CCAgNPF were 4.42, 8.85 and 18.89 µg/ml. All mouthwashes reduced the salivary S. mutans of the orthodontic patients, however, no significant difference was found between the efficacy of CCAgNPF and chlorhexidine (P-value > 0.05). The best results were achieved by the combination of CCAgNPF and chlorhexidine mouthwashes (P-value < 0.05). CONCLUSION: The CCAgNPF and its combination with chlorhexidine present potent bactericidal, biocompatible and effective anti-carious mouthwashes for orthodontic patients. CLINICAL RELEVANCE: This study proved CCAgNPF as an antibacterial mouthwash with lower cytotoxicity and side effects for patients undergoing orthodontic treatments to maintain oral hygiene and reduce salivary S. mutans.


Assuntos
Antibacterianos , Quitosana , Clorexidina , Fluoretos , Nanopartículas Metálicas , Antissépticos Bucais , Nanocompostos , Prata , Streptococcus mutans , Humanos , Streptococcus mutans/efeitos dos fármacos , Quitosana/farmacologia , Quitosana/química , Prata/farmacologia , Prata/química , Antissépticos Bucais/farmacologia , Antissépticos Bucais/química , Nanocompostos/química , Nanopartículas Metálicas/química , Antibacterianos/farmacologia , Feminino , Masculino , Fluoretos/farmacologia , Fluoretos/química , Clorexidina/farmacologia , Saliva/microbiologia , Adolescente , Testes de Sensibilidade Microbiana
7.
Sci Adv ; 10(29): eado2957, 2024 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-39018407

RESUMO

Enzymatic cleavage of C─F bonds in per- and polyfluoroalkyl substances (PFAS) is largely unknown but avidly sought to promote systems biology for PFAS bioremediation. Here, we report the reductive defluorination of α, ß-unsaturated per- and polyfluorocarboxylic acids by Acetobacterium spp. The microbial defluorination products were structurally confirmed and showed regiospecificity and stereospecificity, consistent with their formation by enzymatic reactions. A comparison of defluorination activities among several Acetobacterium species indicated that a functional fluoride exporter was required for the detoxification of the released fluoride. Results from both in vivo inhibition tests and in silico enzyme modeling suggested the involvement of enzymes of the flavin-based electron-bifurcating caffeate reduction pathway [caffeoyl-CoA reductase (CarABCDE)] in the reductive defluorination. This is a report on specific microorganisms carrying out enzymatic reductive defluorination of PFAS, which could be linked to electron-bifurcating reductases that are environmentally widespread.


Assuntos
Acetobacterium , Fluoretos , Fluoretos/metabolismo , Fluoretos/química , Acetobacterium/metabolismo , Ácidos Carboxílicos/metabolismo , Ácidos Carboxílicos/química , Elétrons , Biodegradação Ambiental , Halogenação , Proteínas de Bactérias/metabolismo , Proteínas de Bactérias/química , Fluorocarbonos/metabolismo , Fluorocarbonos/química
8.
Biomed Mater ; 19(5)2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38870928

RESUMO

In this investigation, we embarked on the synthesis of polyethylene glycol coated NaGdF4:Tm3+/Yb3+upconversion nanoparticles (UCNPs), aiming to assess their utility in enhancing image contrast within the context of swept source optical coherence tomography (OCT) and photo-thermal OCT imaging. Our research unveiled the remarkable UC emissions stemming from the transitions of Tm3+ions, specifically the1G4→3H6transitions, yielding vibrant blue emissions at 472 nm. We delved further into the UC mechanism, meticulously scrutinizing decay times and the nanoparticles' capacity to convert radiation into heat. Notably, these nanoparticles exhibited an impressive photo-thermal conversion efficiency of 37.5%. Furthermore, our investigations into their bio-compatibility revealed a promising outcome, with more than 90% cell survival after 24 h of incubation with HeLa cells treated with UCNPs. The nanoparticles demonstrated a notable thermal sensitivity of 4.7 × 10-3K-1at 300 K, signifying their potential for precise temperature monitoring at the cellular level.


Assuntos
Sobrevivência Celular , Meios de Contraste , Nanopartículas , Polietilenoglicóis , Tomografia de Coerência Óptica , Itérbio , Tomografia de Coerência Óptica/métodos , Humanos , Células HeLa , Polietilenoglicóis/química , Itérbio/química , Nanopartículas/química , Meios de Contraste/química , Termometria/métodos , Gadolínio/química , Túlio/química , Fluoretos/química , Temperatura , Materiais Revestidos Biocompatíveis/química , Raios Infravermelhos
9.
J Environ Manage ; 365: 121597, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38941855

RESUMO

Some studies have reported the removal of As (As) and fluoride (F-) using different sacrificial anodes; however, they have been tested with a synthetic solution in a batch system without hydrated silica (SiO2) interaction. Due to the above, concurrent removal of As, F-, and SiO2 from natural deep well water was evaluated (initial concentration: 35.5 µg L-1 As, 1.1 mg L-1F-, 147 mg L-1 SiO2, pH 8.6, and conductivity 1024 µS cm-1), by electrocoagulation (EC) process in continuous mode comparing three different configurations of sacrificial anodes (Al, Fe, and Al-Fe). EC was performed in a new reactor equipped with a small flow distributor and turbulence promoter at the entrance of the first channel to homogenize the flow. The best removal was found at j = 5 mA cm-2 and u = 1.3 cm s-1, obtaining arsenic residual concentrations (CAs) of 1.33, 0.45, and 0.77 µg L-1, fluoride residual concentration ( [Formula: see text] ) of 0.221, 0.495, and 0.622 mg L-1, and hydrated silica residual concentration ( [Formula: see text] ) of 21, 34, and 56 mg L-1, with costs of approximately 0.304, 0.198, and 0.228 USD m-3 for the Al, Fe and Al-Fe anodes, respectively. Al anode outperforms Fe and Al-Fe anodes in concurrently removing As, F- and SiO2. The residual concentrations of As and F- complied with the recommendations of the World Health Organization (WHO) (As < 10 µg L-1 and F- < 1 mg L-1). The spectroscopic analyses of the Al, Fe, and Al-Fe aggregates showed the formation of aluminosilicates, iron oxyhydroxides and oxides, and calcium and sodium silicates involved in removing As, F-, and SiO2. It is concluded that Al would serve as the most suitable sacrificial anode.


Assuntos
Arsênio , Eletrodos , Fluoretos , Dióxido de Silício , Fluoretos/química , Dióxido de Silício/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Alumínio/química , Ferro/química , Poços de Água , Eletrocoagulação/métodos
10.
Mikrochim Acta ; 191(7): 401, 2024 06 17.
Artigo em Inglês | MEDLINE | ID: mdl-38884887

RESUMO

The simultaneous discrimination and detection of multiple anions in an aqueous solution has been a major challenge due to their structural similarity and low charge radii. In this study, we have constructed a supramolecular fluorescence sensor array based on three host-guest complexes to distinguish five anions (F-, Cl-, Br-, I-, and ClO-) in an aqueous solution using anionic-induced fluorescence quenching combined with linear discriminant analysis. Due to the different affinities of the three host-guest complexes for each anion the anion quenching efficiency for each host-guest complex was likewise different, and the five anions were well recognized. The fluorescence sensor array not only distinguished anions at different concentrations (0.5, 10, and 50 µM) with 100% accuracy but also showed good linearity within a certain concentration range. The limit of detection (LOD) was < 0.5 µM. Our interference study showed that the developed sensor array had good anti-interference ability. The practicability of the developed sensor array was also verified by the identification and differentiation of toothpaste brands with different fluoride content and the prediction of the iodine concentration in urine combined with machine learning.


Assuntos
Ânions , Iodo , Limite de Detecção , Aprendizado de Máquina , Espectrometria de Fluorescência , Ânions/urina , Ânions/química , Iodo/urina , Iodo/química , Espectrometria de Fluorescência/métodos , Cremes Dentais/química , Corantes Fluorescentes/química , Fluoretos/química , Fluoretos/urina , Análise Discriminante
11.
Int J Biol Macromol ; 272(Pt 1): 132925, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38844281

RESUMO

An eco-friendly macroparticle biochar (BC)-based Ce(III)-La(III) crosslinked sodium alginate (SA) hybrid hydrogel (BC/Ce-SA-La) was synthesized by droplet polymerization and characterized by SEM-EDS, XRD, FTIR, UV-Vis and XPS. The effects of dosage, pH, contact time, temperature and coexisting ions on the F- ions removal by hybrid hydrogel, and the adsorption performance, interaction mechanism and reusability were investigated. The results demonstrate that the composite has a fancy wrinkle structure with a particle size of about 1.8 mm and abundant porosity on the surface. The removal rate of F- ions by BC/Ce-SA-La reached 90.2 % under the conditions of pH 2.0, 200 min of contact time and 298 K. The adsorption behavior was perfectly explained by Langmuir model, and the maximum adsorption capacity reached 129 mg/g. The adsorption process was an endothermic spontaneous reaction and followed Pseudo-second-order rate model. The strong adsorption was attributed to multi-interactions including complexation, hydrogen bonding and electrostatic adsorption between the composite and F- ions. Coexisting ions hardly interfered with the adsorption of F- ions by BC/Ce-SA-La except for a slight effect of phosphate. The composite after F- ion adsorption was easily separated and could be reused at least three times. BC/Ce-SA-La is a cost-effective and promising granular biosorbent.


Assuntos
Alginatos , Carvão Vegetal , Fluoretos , Hidrogéis , Poluentes Químicos da Água , Purificação da Água , Carvão Vegetal/química , Alginatos/química , Adsorção , Fluoretos/química , Fluoretos/isolamento & purificação , Hidrogéis/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Concentração de Íons de Hidrogênio , Cério/química , Lantânio/química , Temperatura , Cinética , Água/química
12.
BMC Oral Health ; 24(1): 713, 2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38902666

RESUMO

BACKGROUND: Low mechanical properties are the main limitation of glass ionomer cements (GICs). The incorporation of elastomeric micelles is expected to enhance the strength of GICs without detrimentally affecting their physical properties and biocompatibility. This study compared the chemical and mechanical properties, as well as the cytotoxicity, of elastomeric micelles-containing glass ionomer cement (DeltaFil, DT) with commonly used materials, including EQUIA Forte Fil (EF), Fuji IX GP Extra (F9), and Ketac Molar (KT). METHOD: Powder particles of GICs were examined with SEM-EDX. Setting kinetics were assessed using ATR-FTIR. Biaxial flexural strength/modulus and Vickers surface microhardness were measured after immersion in water for 24 h and 4 weeks. The release of F, Al, Sr, and P in water over 8 weeks was analyzed using a fluoride-specific electrode and ICP-OES. The toxicity of the material extract on mouse fibroblasts was also evaluated. RESULTS: High fluoride levels in the powder were detected with EF and F9. DT demonstrated an initial delay followed by a faster acid reaction compared to other cements, suggesting an improved snap set. DT also exhibited superior flexural strength than other materials at both 24 h and 4 weeks but lower surface microhardness (p < 0.05). EF and F9 showed higher release of F, Al, and P than DT and KT. There was no statistically significant difference in fibroblast viability among the tested materials (p > 0.05). CONCLUSIONS: Elastomeric micelles-containing glass ionomer cement (DT) exhibited satisfactory mechanical properties and cytocompatibility compared with other materials. DT could, therefore, potentially be considered an alternative high-strength GIC for load-bearing restorations.


Assuntos
Elastômeros , Fibroblastos , Resistência à Flexão , Cimentos de Ionômeros de Vidro , Dureza , Teste de Materiais , Micelas , Cimentos de Ionômeros de Vidro/toxicidade , Cimentos de Ionômeros de Vidro/química , Animais , Camundongos , Fibroblastos/efeitos dos fármacos , Elastômeros/química , Elastômeros/toxicidade , Alumínio/química , Fluoretos/química , Estrôncio/química , Cimento de Policarboxilato/química , Cimento de Policarboxilato/toxicidade , Sobrevivência Celular/efeitos dos fármacos , Microscopia Eletrônica de Varredura , Propriedades de Superfície , Maleabilidade , Cinética , Espectroscopia de Infravermelho com Transformada de Fourier , Estresse Mecânico , Fatores de Tempo , Materiais Biocompatíveis/química
13.
Radiat Prot Dosimetry ; 200(10): 919-937, 2024 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-38851183

RESUMO

The features of the glow curves of LiF:Mg,Ti are dependent on many parameters of irradiation, storage, ionisation density and readout. These are presented herein with emphasis on their complexity. Successful applications require some understanding of the great diversity of the glow curves. Glow curve analysis/deconvolution in order to better understand the mechanisms is a 'tricky business' even with Tm-Tstop analysis. In the theoretical framework of spatially correlated trapping and luminescent centres, a mechanism is described which simulates the behaviour of composite peak 5 at different cooling rates and following photon bleaching at 3.65 eV.


Assuntos
Fluoretos , Compostos de Lítio , Magnésio , Dosimetria Termoluminescente , Titânio , Compostos de Lítio/química , Magnésio/química , Fluoretos/efeitos da radiação , Fluoretos/química , Dosimetria Termoluminescente/instrumentação , Dosimetria Termoluminescente/métodos , Titânio/química , Luminescência , Fótons
14.
Talanta ; 276: 126300, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38795647

RESUMO

N-myristoylation is one of the most widespread and important lipidation in eukaryotes and some prokaryotes, which is formed by covalently attaching various fatty acids (predominantly myristic acid C14:0) to the N-terminal glycine of proteins. Disorder of N-myristoylation is critically implicated in numerous physiological and pathological processes. Here, we presented a method for purification and comprehensive characterization of endogenous, intact N-glycine lipid-acylated peptides, which combined the negative selection method for N-terminome and the nanographite fluoride-based solid-phase extraction method (NeS-nGF SPE). After optimizing experimental conditions, we conducted the first global profiling of the endogenous and heterogeneous modification states for N-terminal glycine, pinpointing the precise sites and their associated lipid moieties. Totally, we obtained 76 N-glycine lipid-acylated peptides, including 51 peptides with myristate (C14:0), 10 with myristoleate (C14:1), 6 with tetradecadienoicate (C14:2), 5 with laurate (C12:0) and 4 with lauroleate (C12:1). Therefore, our proteomic methodology could significantly facilitate precise and in-depth analysis of the endogenous N-myristoylome and its heterogeneity.


Assuntos
Ácido Mirístico , Extração em Fase Sólida , Extração em Fase Sólida/métodos , Ácido Mirístico/química , Ácido Mirístico/análise , Proteômica/métodos , Fluoretos/química , Fluoretos/análise , Glicina/química , Glicina/análise , Peptídeos/química , Peptídeos/análise
15.
Nature ; 630(8015): 206-213, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38778111

RESUMO

Targeted radionuclide therapy, in which radiopharmaceuticals deliver potent radionuclides to tumours for localized irradiation, has addressed unmet clinical needs and improved outcomes for patients with cancer1-4. A therapeutic radiopharmaceutical must achieve both sustainable tumour targeting and fast clearance from healthy tissue, which remains a major challenge5,6. A targeted ligation strategy that selectively fixes the radiopharmaceutical to the target protein in the tumour would be an ideal solution. Here we installed a sulfur (VI) fluoride exchange (SuFEx) chemistry-based linker on radiopharmaceuticals to prevent excessively fast tumour clearance. When the engineered radiopharmaceutical binds to the tumour-specific protein, the system undergoes a binding-to-ligation transition and readily conjugates to the tyrosine residues through the 'click' SuFEx reaction. The application of this strategy to a fibroblast activation protein (FAP) inhibitor (FAPI) triggered more than 80% covalent binding to the protein and almost no dissociation for six days. In mice, SuFEx-engineered FAPI showed 257% greater tumour uptake than did the original FAPI, and increased tumour retention by 13-fold. The uptake in healthy tissues was rapidly cleared. In a pilot imaging study, this strategy identified more tumour lesions in patients with cancer than did other methods. SuFEx-engineered FAPI also successfully achieved targeted ß- and α-radionuclide therapy, causing nearly complete tumour regression in mice. Another SuFEx-engineered radioligand that targets prostate-specific membrane antigen (PSMA) also showed enhanced therapeutic efficacy. Considering the broad scope of proteins that can potentially be ligated to SuFEx warheads, it might be possible to adapt this strategy to other cancer targets.


Assuntos
Terapia de Alvo Molecular , Neoplasias da Próstata , Radioisótopos , Compostos Radiofarmacêuticos , Animais , Humanos , Masculino , Camundongos , Antígenos de Superfície/química , Antígenos de Superfície/metabolismo , Linhagem Celular Tumoral , Fluoretos/química , Fluoretos/metabolismo , Glutamato Carboxipeptidase II/química , Glutamato Carboxipeptidase II/metabolismo , Ligantes , Proteínas de Membrana/metabolismo , Proteínas de Membrana/química , Terapia de Alvo Molecular/métodos , Projetos Piloto , Neoplasias da Próstata/metabolismo , Neoplasias da Próstata/radioterapia , Radioisótopos/uso terapêutico , Compostos Radiofarmacêuticos/química , Compostos Radiofarmacêuticos/uso terapêutico , Compostos Radiofarmacêuticos/metabolismo , Compostos Radiofarmacêuticos/farmacocinética , Compostos de Enxofre/química , Compostos de Enxofre/metabolismo , Tirosina/metabolismo , Tirosina/química , Ensaios Antitumorais Modelo de Xenoenxerto
16.
ACS Appl Bio Mater ; 7(6): 3821-3827, 2024 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-38787698

RESUMO

Near-infrared fluorescence (NIRF) thermometry is an emerging method for the noncontact measurement of in vivo deep temperatures. Fluorescence-lifetime-based methods are effective because they are unaffected by optical loss due to excitation or detection paths. Moreover, the physiological changes in body temperature in deep tissues and their pharmacological effects are yet to be fully explored. In this study, we investigated the potential application of the NIRF lifetime-based method for temperature measurement of in vivo deep tissues in the abdomen using rare-earth-based particle materials. ß-NaYF4 particles codoped with Nd3+ and Yb3+ (excitation: 808 nm, emission: 980 nm) were used as NIRF thermometers, and their fluorescence decay curves were exponential. Slope linearity analysis (SLA), a screening method, was proposed to extract pixels with valid data. This method involves performing a linearity evaluation of the semilogarithmic plot of the decay curve collected at three delay times after cutting off the pulsed laser irradiation. After intragastric administration of the thermometer, the stomach temperature was monitored by using an NIRF time-gated imaging setup. Concurrently, a heater was attached to the lower abdomens of the mice under anesthesia. A decrease in the stomach temperature under anesthesia and its recovery via the heater indicated changes in the fluorescence lifetime of the thermometer placed inside the body. Thus, NaYF4:Nd3+/Yb3+ functions as a fluorescence thermometer that can measure in vivo temperature based on the temperature dependence of the fluorescence lifetime at 980 nm under 808 nm excitation. This study demonstrated the ability of a rare-earth-based NIRF thermometer to measure deep tissues in live mice, with the proposed SLA method for excluding the noisy deviations from the analysis for measuring temperature using the NIRF lifetime of a rare-earth-based thermometer.


Assuntos
Fluoretos , Imagem Óptica , Itérbio , Ítrio , Animais , Camundongos , Ítrio/química , Itérbio/química , Fluoretos/química , Neodímio/química , Materiais Biocompatíveis/química , Teste de Materiais , Tamanho da Partícula , Temperatura , Termometria/métodos , Raios Infravermelhos
17.
Biomed Mater ; 19(4)2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38810617

RESUMO

Dental caries, a chronic infectious disease characterized by tooth mineral loss caused by plaque, is one of the major global public health problems. Silver diamine fluoride (SDF) has been proven to be a highly effective anti-caries drug due to its high bacterial inhibition and remineralization ability. However, the SDF solution is unstable, which immensely limits its clinical application. Therefore, new silver-load clay named AgF@Hec was designed by replacing the NH3with hectorite in this study. Fourier transform infrared spectroscopy and x-ray diffraction spectroscopy were employed to confirm the structure of AgF@Hec. Dynamic light scattering analysis was used to reveal the effect of different hectorite concentrations on the stability of AgF@Hec. Moreover, AgF@Hec exhibits significant remineralization and hardness recovery of the initial carious lesions. Bacteriostatic experiments also proved that it has a significant inhibitory effect onA. Viscosus, S. mutans, S. sanguinis, S. salivarius, Lactobacillus sp.and both gram-positive and gram-negative bacteria. We therefore believed that AgF@Hec should be a promising biomaterial that can be applied in the prevention of dental caries.


Assuntos
Argila , Cárie Dentária , Compostos de Amônio Quaternário , Compostos de Prata , Prata , Difração de Raios X , Cárie Dentária/prevenção & controle , Argila/química , Compostos de Prata/química , Compostos de Prata/farmacologia , Espectroscopia de Infravermelho com Transformada de Fourier , Compostos de Amônio Quaternário/química , Compostos de Amônio Quaternário/farmacologia , Prata/química , Prata/farmacologia , Fluoretos/química , Antibacterianos/farmacologia , Antibacterianos/química , Remineralização Dentária/métodos , Streptococcus mutans/efeitos dos fármacos , Humanos , Dureza , Teste de Materiais , Animais , Testes de Sensibilidade Microbiana , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Fluoretos Tópicos
18.
Environ Geochem Health ; 46(6): 190, 2024 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-38695943

RESUMO

A magnetic nanocomposite of hydroxyapatite and biomass (HAp-CM) was synthesized through a combined ultrasonic and hydrothermal method, aiming for efficient adsorption of arsenic (As) and fluoride (F-) from drinking water in natural environments. The characterization of HAp-CM was carried out using TG, FTIR, XRD, SEM, SEM-EDS, and TEM techniques, along with the determination of pHpzc charge. FTIR analysis suggested that coordinating links are the main interactions that allow the formation of the nanocomposite. XRD data indicated that the crystalline structure of the constituent materials remained unaffected during the formation of HAp-CM. SEM-EDS analysis revelated a Ca/P molar ratio of 1.78. Adsorption assays conducted in batches demonstrated that As and F- followed a PSO kinetic model. Furthermore, As adsorption fitting well to the Langmuir model, while F- adsorption could be explained by both Langmuir and Freundlich models. The maximum adsorption capacity of HAp-CM was found to be 5.0 mg g-1 for As and 10.2 mg g-1 for F-. The influence of sorbent dosage, pH, and the presence of coexisting species on adsorption capacity was explored. The pH significantly affected the nanocomposite's efficiency in removing both pollutants. The presence of various coexisting species had different effects on F- removal efficiency, while As adsorption efficiency was generally enhanced, except in the case of PO43-. The competitive adsorption between F- and As on HAp-CM was also examined. The achieved results demonstrate that HAp-CM has great potential for use in a natural environment, particularly in groundwater remediation as a preliminary treatment for water consumption.


Assuntos
Arsênio , Durapatita , Fluoretos , Nanocompostos , Poluentes Químicos da Água , Purificação da Água , Fluoretos/química , Adsorção , Nanocompostos/química , Durapatita/química , Poluentes Químicos da Água/química , Arsênio/química , Purificação da Água/métodos , Concentração de Íons de Hidrogênio , Biomassa , Cinética , Água Potável/química , Espectroscopia de Infravermelho com Transformada de Fourier , Difração de Raios X
19.
Int J Mol Sci ; 25(9)2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38731865

RESUMO

This study explored the feasibility of fluoride removal from simulated semiconductor industry wastewater and its recovery as calcium fluoride using fluidized bed crystallization. The continuous reactor showed the best performance (>90% fluoride removal and >95% crystallization efficiency) at a calcium-to-fluoride ratio of 0.6 within the first 40 days of continuous operation. The resulting particle size increased by more than double during this time, along with a 36% increase in the seed bed height, indicating the deposition of CaF2 onto the silica seed. The SEM-EDX analysis showed the size and shape of the crystals formed, along with the presence of a high amount of Ca-F ions. The purity of the CaF2 crystals was determined to be 91.1% though ICP-OES analysis. Following the continuous experiment, different process improvement strategies were explored. The addition of an excess amount of calcium resulted in the removal of an additional 6% of the fluoride; however, compared to this single-stage process, a two-stage approach was found to be a better strategy to achieve a low effluent concentration of fluoride. The fluoride removal reached 94% with this two-stage approach under the optimum conditions of 4 + 1 h HRT combinations and a [Ca2+]/[F-] ratio of 0.55 and 0.7 for the two reactors, respectively. CFD simulation showed the impact of the inlet diameter, bottom-angle shape, and width-to-height ratio of the reactor on the mixing inside the reactor and the possibility of further improvement in the reactor performance by optimizing the FBR configuration.


Assuntos
Fluoreto de Cálcio , Fluoretos , Águas Residuárias , Fluoreto de Cálcio/química , Fluoretos/química , Fluoretos/isolamento & purificação , Águas Residuárias/química , Purificação da Água/métodos , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Cristalização
20.
Anal Chem ; 96(19): 7697-7705, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38697043

RESUMO

Dual/multimodal imaging strategies are increasingly recognized for their potential to provide comprehensive diagnostic insights in cancer imaging by harnessing complementary data. This study presents an innovative probe that capitalizes on the synergistic benefits of afterglow luminescence and magnetic resonance imaging (MRI), effectively eliminating autofluorescence interference and delivering a superior signal-to-noise ratio. Additionally, it facilitates deep tissue penetration and enables noninvasive imaging. Despite the advantages, only a limited number of probes have demonstrated the capability to simultaneously enhance afterglow luminescence and achieve high-resolution MRI and afterglow imaging. Herein, we introduce a cutting-edge imaging platform based on semiconducting polymer nanoparticles (PFODBT) integrated with NaYF4@NaGdF4 (Y@Gd@PFO-SPNs), which can directly amplify afterglow luminescence and generate MRI and afterglow signals in tumor tissues. The proposed mechanism involves lanthanide nanoparticles producing singlet oxygen (1O2) upon white light irradiation, which subsequently oxidizes PFODBT, thereby intensifying afterglow luminescence. This innovative platform paves the way for the development of high signal-to-background ratio imaging modalities, promising noninvasive diagnostics for cancer.


Assuntos
Elementos da Série dos Lantanídeos , Imageamento por Ressonância Magnética , Nanopartículas , Polímeros , Semicondutores , Imageamento por Ressonância Magnética/métodos , Animais , Elementos da Série dos Lantanídeos/química , Polímeros/química , Nanopartículas/química , Camundongos , Humanos , Gadolínio/química , Luminescência , Oxigênio Singlete/química , Ítrio/química , Fluoretos/química , Camundongos Nus
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