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1.
J Environ Radioact ; 278: 107493, 2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38970971

RESUMO

The presence of carbonates or humic substances (HS) will significantly affect the species and chemical behavior of U(VI) in solution, but lacking systematic exploration of the coupling effect of carbonates and HS under near real environmental conditions at present. Herein, the sorption behavior of U(VI) on illite was systematically studied in the co-existence of carbonates and HS including both humic acid (HA) and fulvic acid (FA) by batch technique. The distribution coefficients (Kd) increased as function of time and temperature but decreased with increasing concentrations of initial U(VI), Ca2+, and Mg2+, as well as ion strength. At pH 2.0-10.5, the Kd values first increased rapidly and then decreased visibly, with its maximum value appearing at pH 5.0, owning to the changes in the interaction between illite and the dominant species of U(VI) from electrostatic attraction to electrostatic repulsion. The sorption was a heterogeneous, spontaneous, and endothermic chemical process, which could be well described by pseudo-second-order kinetic and Flory-Huggins isotherm models. When carbonates and HA/FA coexisted, the Kd values always increased first and then decreased as a function of pH, with the only difference for HA and FA being the key pH (pHkey) at which the promoting and inhibiting effects on the sorption of U(VI) onto illite undergo a transition. The carbonates and HS have a synergistic inhibitory effect on the U(VI) sorption onto illite at pH 7.8. FTIR and XPS spectra demonstrated that the hydroxyl groups on the illite surface and in the HS were involved in U(VI) sorption on illite in the presence of carbonates. These results provide valuable data for a deeper understanding of U(VI) migration in geological media.

2.
J Colloid Interface Sci ; 676: 1-12, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-39018802

RESUMO

Spinel Li4Ti5O12 (LTO), a zero-strain material, is a promising anode material for solid-state thin-film lithium-ion batteries (TFB). However, the preparation of high-performance Li4Ti5O12 thin-film electrodes through facile methods remains a significant challenge. Herein, we present a novel approach to prepare a binder- and conductor-free porous Li4Ti5O12 (P-LTO) thin-film. This approach polyvinyl alcohol (PVA)-assisted spray deposition and does not require the use of complex or expensive methods. Adding PVA to the precursor solution effectively prevents thin-film cracking during high-temperature annealing, enhances adhesion, and forms a highly interconnected porous structure. This unique structure shortens the lithium-ion diffusion pathways and facilitates electron transport. Therefore, P-LTO thin film electrodes demonstrate exceptional rate capacity of 104.1 mAh/g at a current density of 100C. In addition, the electrodes exhibit ultra-long cycle stability, retaining 80.9 % capacity after 10,000 cycles at 10C. This work offers a novel approach for the preparation of high-performance thin-film electrodes for TFBs.

3.
ACS Appl Mater Interfaces ; 16(26): 33657-33668, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38904104

RESUMO

Reduction of soluble U(VI) to insoluble U(IV) based on photocatalysts is a simple, environmentally friendly, and efficient method for treating radioactive wastewater. The present study involved the systematic comparison of the photoelectric properties of three metalloporphyrins with different metal centers and the synthesis of a novel porphyrin-based hydrogen-bonded organic framework (Ni-pHOF) photocatalyst by modulating the surface charge microenvironment in porphyrin for enhanced photocatalytic removal of U(VI) from wastewater. Compared to the metal-free HOF, the surface charge microenvironment around the Ni atom in Ni-pHOF accelerated the reduction kinetics of U(VI) under visible light illumination at the initial moment, showing a high removal rate, even in air. The removal rate of U(VI) from aqueous solution by Ni-pHOF can achieve over 98% in the presence of coexisting nonoxidizing cations and only decreased by less than 8% after five cycles, exhibiting high selectivity and good reusability. Furthermore, Ni-pHOF can remove 86.74% of U(VI) from real low-level radioactive wastewater after 120 min of illumination, showcasing practical application potential. Density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) spectra indicated that modulating the surface charge microenvironment in Ni-pHOF through porphyrin metallization is conducive to improving the charge separation efficiency, prompting more e- and •O2- to participate in the reduction reaction of U(VI). This work provides new insights into the metallization of porphyrin-based HOFs and paves a new way for the tailoring of porphyrin-based HOFs/COFs by modulating the surface charge microenvironment to achieve efficient recovery of U(VI) from real radioactive wastewater.

4.
Eur J Med Chem ; 271: 116410, 2024 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-38615409

RESUMO

With the increasing reports of antibiotic resistance in this species, Pseudomonas aeruginosa is a common human pathogen with important implications for public health. Bacterial quorum sensing (QS) systems are potentially broad and versatile targets for developing new antimicrobial compounds. While previous reports have demonstrated that certain amide compounds can inhibit bacterial growth, there are few reports on the specific inhibitory effects of these compounds on bacterial quorum sensing systems. In this study, thirty-one amide derivatives were synthesized. The results of the biological activity assessment indicated that A9 and B6 could significantly inhibit the expression of lasB, rhlA, and pqsA, effectively reducing several virulence factors regulated by the QS systems of PAO1. Additionally, compound A9 attenuated the pathogenicity of PAO1 to Galleria mellonella larvae. Meanwhile, RT-qPCR, SPR, and molecular docking studies were conducted to explore the mechanism of these compounds, which suggests that compound A9 inhibited the QS systems by binding with LasR and PqsR, especially PqsR. In conclusion, amide derivatives A9 and B6 exhibit promising potential for further development as novel QS inhibitors in P. aeruginosa.


Assuntos
Amidas , Antibacterianos , Descoberta de Drogas , Simulação de Acoplamento Molecular , Pseudomonas aeruginosa , Percepção de Quorum , Pseudomonas aeruginosa/efeitos dos fármacos , Percepção de Quorum/efeitos dos fármacos , Amidas/farmacologia , Amidas/química , Amidas/síntese química , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/síntese química , Relação Estrutura-Atividade , Estrutura Molecular , Testes de Sensibilidade Microbiana , Relação Dose-Resposta a Droga , Animais
5.
Chemistry ; 30(9): e202303298, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38050716

RESUMO

Theranostic nanomedicine combined bioimaging and therapy probably rises more helpful and interesting opportunities for personalized medicine. In this work, 177 Lu radiolabeling and surface PEGylation of biocompatible covalent polymer nanoparticles (CPNs) have generated a new theranostic nanoformulation (177 Lu-DOTA-PEG-CPNs) for targeted diagnosis and treatment of breast cancer. The in vitro anticancer investigations demonstrate that 177 Lu-DOTA-PEG-CPNs possess excellent bonding capacity with breast cancer cells (4T1), inhibiting the cell viability, leading to cell apoptosis, arresting the cell cycle, and upregulating the reactive oxygen species (ROS), which can be attributed to the good targeting ability of the nanocarrier and the strong relative biological effect of the radionuclide labelled compound. Single photon emission computed tomography/ computed tomography (SPECT/CT) imaging and in vivo biodistribution based on 177 Lu-DOTA-PEG-CPNs reveal that notable radioactivity accumulation at tumor site in murine 4T1 models with both intravenous and intratumoral administration of the prepared radiotracer. Significant tumor inhibition has been observed in mice treated with 177 Lu-DOTA-PEG-CPNs, of which the median survival was highly extended. More strikingly, 50 % of mice intratumorally injected with 177 Lu-DOTA-PEG-CPNs was cured and showed no tumor recurrence within 90 days. The outcome of this work can provide new hints for traditional nanomedicines and promote clinical translation of 177 Lu radiolabeled compounds efficiently.


Assuntos
Nanopartículas , Neoplasias , Animais , Camundongos , Medicina de Precisão , Polímeros , Distribuição Tecidual , Linhagem Celular Tumoral , Radioisótopos/uso terapêutico , Lutécio/uso terapêutico , Compostos Radiofarmacêuticos/uso terapêutico , Neoplasias/tratamento farmacológico
6.
Bioorg Med Chem ; 96: 117517, 2023 12 15.
Artigo em Inglês | MEDLINE | ID: mdl-37939492

RESUMO

Recently, endoradiotherapy based on actinium-225 (225Ac) has attracted increasing attention, which is due to its α particles can generate maximal damage to cancer cells while minimizing unnecessary radiation effects on healthy tissues. Herein, 111In/225Ac-radiolabeled conjugated polymer nanoparticles (CPNs) coated with amphiphilic polymer DSPE-PEG-DOTA have been developed as a new injectable nano-radiopharmaceuticals for cancer endoradiotherapy under the guidance of nuclear imaging. Single photon emission computed tomography/computed tomography (SPECT/CT) using 111In-DOTA-PEG-CPNs as nano probe indicates a prolonged retention of radiolabeled nanocarriers, which was consistent with the in vivo biodistribution examined by direct radiometry analysis. Significant inhibition of tumor growth has been observed in murine 4T1 models treated with 225Ac-DOTA-PEG-CPNs when compared to mice treated with PBS or DOTA-PEG-CPNs. The 225Ac-DOTA-PEG-CPNs group experienced no single death within 24 days with the median survival considerably extended to 35 days, while all the mice treated with PBS or DOTA-PEG-CPNs died at 20 days post injection. Additionally, the histopathology studies demonstrated no obvious side effects on healthy tissues after treatment with 225Ac-DOTA-PEG-CPNs. All these results reveal that the new 225Ac-labeled DOTA-PEG-CPNs is promising as paradigm for endoradiotherapy.


Assuntos
Nanopartículas , Neoplasias , Animais , Camundongos , Polímeros , Distribuição Tecidual , Compostos Radiofarmacêuticos/farmacologia , Compostos Radiofarmacêuticos/uso terapêutico , Linhagem Celular Tumoral
7.
RSC Adv ; 13(48): 33905-33910, 2023 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-38019995

RESUMO

The Ni-rich NCM622 is a promising cathode material for future high energy lithium ion batteries, but unstable electrochemical performance of NCM622 hinder its large scale commercial application. The cycling peformance of nickel-rich LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode materials can be improved by surface coating. Here, a one-step approach based on TiF4 is used to successfully manufacture modified NCM622 cathode materials with a TiO2-LiF coating. The TiO2-LiF coated NCM622 preserves 79.7% capacity retention which is higher than the pure NCM622 (68.9%) at 1C after 200 cycles within 2.7-4.3 V. This material serves as the cathode for lithium-ion batteries (LIBs). The uniform TiO2-LiF coating layer can alleviate structural degradation brought on by unfavorable side reactions with the electrolyte has been validated. TiO2-LiF coated on NCM622 cathode materials can be modified easily by one-step approach.

8.
Bioorg Chem ; 141: 106871, 2023 12.
Artigo em Inglês | MEDLINE | ID: mdl-37734193

RESUMO

Bacterial leaf blight (BLB) caused by Xanthomonas oryzae pv. oryzae (Xoo) has a significant impact on rice yield and quality worldwide. Traditionally, bactericide application has been commonly used to control this devastating disease. However, the overuse of fungicides has led to a number of problems such as the development of resistance and environmental pollution. Therefore, the development of new methods and approaches for disease control are still urgent. In this paper, a series of cinnamic acid derivatives were designed and synthesized, and three novel T3SS inhibitors A10, A12 and A20 were discovered. Novel T3SS inhibitors A10, A12 and A20 significantly inhibited the hpa1 promoter activity without affecting Xoo growth. Further studies revealed that the title compounds A10, A12 and A20 significantly impaired hypersensitivity in non-host plant tobacco leaves, while applications on rice significantly reduced symptoms of bacterial leaf blight. RT-PCR showed that compound A20 inhibited the expression of T3SS-related genes. In summary, this work exemplifies the potential of the title compound as an inhibitor of T3SS and its efficacy in the control of bacterial leaf blight.


Assuntos
Oryza , Xanthomonas , Sistemas de Secreção Tipo III/genética , Sistemas de Secreção Tipo III/metabolismo , Cinamatos/farmacologia , Cinamatos/metabolismo , Xanthomonas/metabolismo , Oryza/metabolismo
9.
ACS Appl Mater Interfaces ; 15(39): 45713-45724, 2023 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-37738473

RESUMO

Nano-metal-organic frameworks (nano-MOFs) labeled with radionuclides have shown great potential in the anticancer field. In this work, we proposed to combine fluorescence imaging (FI) with nuclear imaging to systematically evaluate the tumor inhibition of new nanomedicines from living cancer cells to the whole body, guiding the design and application of a high-performance anticancer radiopharmaceutical to glioma. An Fe-based nano-MOF vector, MIL-101(Fe)/PEG-FA, was decorated with fluorescent sulfo-cyanine7 (Cy7) to investigate the binding affinity of the targeting nanocarriers toward glioma cells in vitro, as well as possible administration modes for in vivo cancer therapy. Then, lutetium-177 (177Lu)-labeled MIL-101(Fe)/PEG-FA was prepared for high-sensitive imaging and targeted radiotherapy of glioma in vivo. It has been demonstrated that the obtained 177Lu-labeled MIL-101(Fe)/PEG-FA can work as a complementary probe to rectify the cancer binding affinity of the prepared nanocarrier given by fluorescence imaging, providing more precise biodistribution information. Besides, 177Lu-labeled MIL-101(Fe)/PEG-FA has excellent antitumor effect, leading to cell proliferation inhibition, upregulation of intracellular reactive oxygen species, tumor growth suppression, and immune response-related protein and cytokine upregulation. This work reveals that optical imaging and nuclear imaging can work complementarily as multimodal imaging in the design and evaluation of anticancer nanomedicine, offering a MIL-101(Fe)/PEG-FA-based pharmaceutical with potential in tumor endoradiotherapy.


Assuntos
Glioma , Estruturas Metalorgânicas , Humanos , Nanomedicina , Distribuição Tecidual , Imagem Multimodal , Glioma/diagnóstico por imagem , Glioma/tratamento farmacológico
10.
J Environ Radioact ; 270: 107286, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37633243

RESUMO

The sorption behavior of U(VI) on Tamusu clay sampled from a pre-selected high-level radioactive waste (HLW) disposal site in Inner Mongolia (China) was studied systematically in the U(VI)-CO3 solution at pH 7.8 by batch experiments. The results demonstrated that the distribution coefficients (Kd) decreased with the increasing values of pHinitial, [U(VI)]initial, and ionic strength, but increased with the extended time and the rising temperature. The sorption was a pH-dependent, heterogeneous, spontaneous, and endothermic chemical process, which could be better described by Freundlich isothermal model and pseudo-second-order kinetic model. The presence of humic acid (HA) or fulvic acid (FA) significantly inhibited the U(VI) sorption, due to the enhanced electrostatic repulsion between the negatively charged HA/FA adsorbed on the clay surface and the negative U(VI) species, as well as the well dispersed HA/FA aggregates in solution wrapping the U(VI) species. The FTIR and XPS spectra indicated that the HCO3- groups on the surface of Tamusu clay after hydroxylation and the ‒OH groups in HA/FA were involved in the U(VI) sorption. The results reported here provide valuable insights into the further understanding of U(VI) migration in geological media.


Assuntos
Monitoramento de Radiação , Urânio , Argila , Adsorção , Concentração de Íons de Hidrogênio , Urânio/química , Substâncias Húmicas
11.
J Hazard Mater ; 459: 132179, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37531757

RESUMO

The reduction of soluble U(VI) to insoluble U(IV) precipitates by visible light is an environmentally friendly and highly effective strategy to remove uranium from uranium-containing radioactive wastewater. Herein, a porous hydrogen-bonded organic framework (HOF) of UPC-H4a was self-assembled by intermolecular hydrogen bonds of 5,10,15,20-tetra(4-(2,4-diaminotriazine)phenyl) porphyrin to remove U(VI) from aqueous solution. UPC-H4a has high crystallinity with permanent porosity, excellent photocatalytic property, good chemical stability, and strong photocatalytic reducibility. The experiments showed that UPC-H4a removed 98.18% of U(VI) after illumination for 120 min, with high selectivity, strong ion interference resistance, and good reusability. A real low-level radioactive wastewater was employed to estimate the potential of UPC-H4a for practical application and its removal rate can reach 66.14% in the presence of redox competing metal ions, exhibiting great potential for practical application. The DFT calculations and EPR spectra revealed that a more negative electrostatic potential of DAT-porphyrin and the formed intermolecular hydrogen bonds in UPC-H4a can facilitate the participation of photogenerated electrons in the O2/∙O2- reaction, and the radical of ∙O2- was proved to be the critical participant in U(VI) photoreduction. The discovery of UPC-H4a in this work will help to develop more potential applications of HOFs as photocatalysts in radioactive wastewater treatment.

12.
Skin Res Technol ; 29(7): e13405, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37522491

RESUMO

OBJECTIVE: To investigate the effects of secukinumab treatment for psoriasis on different functional cytokines and inflammatory mediators in patients' serum METHODS: Enzyme-linked immunosorbent assay was used to detect interleukin (IL)-1ß and IL-1RA associated with intrinsic immunity; IL-6, IL-18, and growth regulated oncogene alpha (GROα) associated with neutrophils; IL-12, tumour necrosis factor (TNF)-α, and interferon (IFN)-γ associated with Th1; IL-23, IL-17A, and IL-22 associated with Th17; Thymus activation regulated chemokine (TARC), IL-13, and defensin beta 2 (DEFB2) associated with Th2; Vascular endothelial growth factor (VEGF)-A and IL-10 associated with angiogenesis; and IFN-γ associated with sepsis in the peripheral blood of 12 patients with common psoriasis treated with secukinumab and 15 healthy controls. IL-23, IL-17A, IL-22 associated with Th17; TARC, IL-13, DEFB2 associated with Th2; VEGF-A, IL-10 associated with angiogenesis and procalcitonin (PCT) associated with sepsis. The differences in expression of the above cytokines before and after treatment and the correlation with psoriasis disease severityï¼»Psoriasis Area Severity Index(PASI) scoreï¼½, age, and disease duration were analyzed. RESULTS: The mean PASI score of the enrolled patients with moderate to severe psoriasis was 21.6 ± 11.0 before treatment and decreased to below 1 after treatment. Serum IL-6; IL-18, GROα, IFN-γ, TNF-α, VEGF-A, and IL-17A were significantly higher than normal. And IL-17A and IFN-γ were positively correlated with disease duration and age, and IL-18 was positively correlated with PASI score. The expression levels of IL-6, GROα, VEGF-A, IFN-γ, TNF-α, IL-17A and IL-23 were significantly lower after secukinumab treatment compared with those before treatment, but the expression levels of IFN-γ, VEGF-A, TARC, IL-13, and DEFB2 were still significantly higher than those of normal subjects after treatment CONCLUSIONS: secukinumab clears skin lesions by antagonizing IL-17A and simultaneously decreasing the expression levels of IL-6, GRO α, VEGF-A, IFN-γ, TNF-α, IL-17A, and IL-23.

13.
Environ Sci Technol ; 57(28): 10339-10347, 2023 07 18.
Artigo em Inglês | MEDLINE | ID: mdl-37399448

RESUMO

Using molecular dynamics simulations, this work targets a molecular understanding on the rigidity and flexibility of fulvic acid (FA) in uranyl sorption on graphene oxide (GO). The simulations demonstrated that both rigid Wang's FA (WFA) and flexible Suwannee River FA (SRFA) can provide multiple sites to cooperate with GO for uranyl sorption and act as "bridges" to connect uranyl and GO to form GO-FA-U (type B) ternary surface complexes. The presence of flexible SRFA was more beneficial to uranyl sorption on GO. The interactions of WFA and SRFA with uranyl were primarily driven by electrostatics, and the electrostatic interaction of SRFA-uranyl was significantly stronger owing to the formation of more complexes. The flexible SRFA could markedly enhance the bonding strength of uranyl with GO by folding itself to provide more sites to coordinate with uranyl. The rigid WFAs tended to be adsorbed on the GO surface in parallel due to π-π interactions, whereas the flexible SRFAs took more slant configurations resulting from intermolecular hydrogen bonds. This work provides new insights into the sorption dynamics, structure, and mechanism and addresses the effect of molecular rigidity and flexibility, with great significance for FA-based remediation strategies of uranium-contaminated sites.


Assuntos
Grafite , Simulação de Dinâmica Molecular , Benzopiranos/química , Grafite/química
14.
Pest Manag Sci ; 79(10): 3666-3675, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37184259

RESUMO

BACKGROUND: Cruciferous black rot is caused by Xanthomonas campestris pv. campestris (Xcc) infection and is a widespread disease worldwide. Excessive and repeated use of bactericide is an important cause of the development of bacterial resistance. It is imperative to take new approaches to screening compounds that target virulence factors rather than kill bacterial pathogens. The type III secretion system (T3SS) invades a variety of cells by transporting virulence effector factors into the cytoplasm and is an attractive antitoxic target. Toward the search of new T3SS inhibitors, an alternative series of novel pyrimidin-4-one derivatives were designed and synthesized and assessed for their effect in blocking the virulence. RESULTS: All of the target compounds were characterized by proton (1 H) nuclear magnetic resonance (NMR), carbon-13 (13 C) NMR, fluorine-19 (19 F) NMR and high-resolution mass spectrometry (HRMS). All compounds were evaluated using high-throughput screening systems against Xcc. The results of the biological activity test revealed that the compound SPF-9 could highly inhibit the activity of xopN gene promoter and the hypersensitivity (HR) of tobacco without affecting bacterial growth. Moreover, messenger RNA (mRNA) level measurements showed that compound SPF-9 inhibited the expression of some representative genes (hrp/hrc genes). Compound SPF-9 weakened the pathogenicity of Xcc to Raphanus sativus L. CONCLUSION: Compound SPF-9 has good potential for further development as a novel T3SS inhibitor against Xcc. © 2023 Society of Chemical Industry.


Assuntos
Xanthomonas campestris , Xanthomonas campestris/genética , Xanthomonas campestris/metabolismo , Proteínas de Bactérias/genética , Sistemas de Secreção Tipo III/genética , Sistemas de Secreção Tipo III/metabolismo , Virulência/genética , Fatores de Virulência/metabolismo
15.
Polymers (Basel) ; 15(9)2023 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-37177296

RESUMO

In this work, a novel metal-organic frameworks (MOFs)-based ion-imprinted polymer (MIIP) was prepared to remove Co(II) from simulated radioactive wastewater. The batch experiments indicated that the sorption was well described by the pseudo-second-order kinetic and Langmuir models, and it is monolayer chemisorption. The theoretical maximum sorption capacity was estimated to be 181.5 mg∙g-1, which is by far the reported maximum value of Co(II) sorption by the imprinted materials. The MIIP presented an excellent selectivity for Co(II) in the presence of common monovalent and divalent metal ions, and the selectivity coefficients were 44.31, 33.19, 10.84, 27.71, 9.45, 16.25, and 7.60 to Li(I), K(I), Mg(II), Ca(II), Mn(II), Ba(II), and Cd(II), respectively. The sorption mechanism was explored by X-ray photoelectron spectroscopy (XPS) technology and density functional theory (DFT) calculations, suggesting that Co(II) was adsorbed by the MIIP via the chelation of 4-vinylpyridine (VP) ligands with Co(II), which was a spontaneous process, and the optimal coordination ratio of VP to Co(II) was 6. This work suggested that the MIIP has a high sorption capacity and excellent selectivity for Co(II), which is of great significance for the selective separation of Co-60 from radioactive wastewater.

16.
ACS Appl Mater Interfaces ; 15(13): 16343-16354, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36947054

RESUMO

The combination of chemotherapy and phototherapy has received tremendous attention in multimodal cancer therapy. However, satisfactory therapeutic outcomes of chemo-photothermal therapy (chemo-PTT) still remain challenging. Herein, a biocompatible smart nanoplatform based on benzothiazole-linked conjugated polymer nanoparticles (CPNs) is rationally designed, for effectively loading doxorubicin (DOX) and Mo-based polyoxometalate (POM) through both dynamic chemical bond and intermolecular interactions, with an expectation to obtain new anticancer drugs with multiple stimulated responses to the tumor microenvironment (TME) and external laser irradiation. Controlled drug release of DOX from the obtained nanoformulation (CPNs-DOX-PEG-cRGD-BSA@POM) triggered by both endogenous stimulations (GSH and low pH) and exogenous laser irradiation has been well demonstrated by pharmacodynamics investigations. More intriguingly, incorporating POM into the nanoplatform not only enables the nanomedicine to achieve mild hyperthermia but also makes it exhibit self-assembly behavior in acidic TME, producing enhanced tumor retention. Benefiting from the versatile functions, the prepared CPNs-DOX-PEG-cRGD-BSA@POM exhibited excellent tumor targeting and therapeutic effects in murine xenografted models, showing great potential in practical cancer therapy.


Assuntos
Hipertermia Induzida , Nanopartículas , Neoplasias , Animais , Camundongos , Terapia Fototérmica , Polímeros , Doxorrubicina/química , Fototerapia , Neoplasias/patologia , Nanopartículas/química , Benzotiazóis , Microambiente Tumoral
17.
J Environ Radioact ; 261: 107126, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36805950

RESUMO

Uranium biomineralization can slow uranium migration in the environment and thus prevent it from further contaminating the surroundings. Investigations into the uranium species, pH, inorganic phosphate (Pi) concentration, and microbial viability during biomineralization by microorganisms are crucial for understanding the mineralization mechanism. In this study, Bacillus thuringiensis X-27 was isolated from soil contaminated with uranium and was used to investigate the formation process of uranium biominerals induced by X-27. The results showed that as biomineralization proceeded, amorphous uranium-containing deposits were generated and transformed into crystalline minerals outside cells, increasing the overall concentration of uramphite. This is a cumulative rather than abrupt process. Notably, B. thuringiensis X-27 precipitated uranium outside the cell surface within 0.5 h, while the release of Pi into the extracellular environment and the change of pH to alkalescence further promoted the formation of uramphite. In addition, cell viability determination showed that the U(VI) biomineralization induced by B. thuringiensis X-27 was instrumental in alleviating the toxicity of U(VI) to cells. This work offers insight into the mechanism of U(VI) phosphate biomineralization and is a reference for bioremediation-related studies.


Assuntos
Bacillus thuringiensis , Monitoramento de Radiação , Urânio , Bacillus thuringiensis/metabolismo , Urânio/metabolismo , Biomineralização , Biodegradação Ambiental , Fosfatos/farmacologia
18.
J Environ Sci (China) ; 124: 915-922, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36182194

RESUMO

As a biosorbent, algae are frequently used for the biotreatment or bioremediation of water contaminated by heavy metal or radionuclides. However, it is unclear that whether or not the biomineralization of these metal or radionuclides can be induced by algae in the process of bioremediation and what the mechanism is. In this work, Ankistrodsemus sp. has been used to treat the uranium-contaminated water, and more than 98% of uranium in the solution can be removed by the alga, when the initial uranium concentration ranges from 10 to 80 mg/L. Especially, an unusual phenomenon of algae-induced uranium biomineralization has been found in the process of uranium bioremediation and its mineralization mechanism has been explored by multiple approaches. It is worth noticing that the biomineralization of uranium induced by Ankistrodsemus sp. is significantly affected by contact time and pH. Uranium is captured rapidly on the cell surface via complexation with the carboxylate radical, amino and amide groups of the microalgae cells, which provides nucleation sites for the precipitation of insoluble minerals. Uranium stimulates Ankistrodsemus sp. to metabolize potassium ions (K+), which may endow algae with the ability to biomineralize uranium into the rose-like compreignacite (K2[(UO2)6O4(OH)6]•8H2O). As the time increased, the amorphous gradually converted into compreignacite crystals and a large number of crystals would expand over both inside and outside the cells. To the best of our knowledge, this is the first investigated microalgae with a time-dependent uranium biomineralization ability and superior tolerance to uranium. This work validates that Ankistrodsemus sp. is a promising alga for the treatment of uranium-contaminated wastewater.


Assuntos
Clorófitas , Urânio , Amidas , Biomineralização , Minerais/química , Potássio , Radioisótopos , Urânio/química , Compostos de Urânio , Águas Residuárias , Água
19.
Mol Pharm ; 19(9): 3206-3216, 2022 09 05.
Artigo em Inglês | MEDLINE | ID: mdl-35993583

RESUMO

Targeted radionuclide therapy based on α-emitters plays an increasingly important role in cancer treatment. In this study, we proposed to apply a heterodimeric peptide (iRGD-C6-lys-C6-DA7R) targeting both VEGFR and integrins as a new vector for 211At radiolabeling to obtain high-performance radiopharmaceuticals with potential in targeted alpha therapy (TAT). An astatinated peptide, iRGD-C6-lys(211At-ATE)-C6-DA7R, was prepared with a radiochemical yield of ∼45% and high radiochemical purity of >95% via an electrophilic radioastatodestannylation reaction. iRGD-C6-lys(211At-ATE)-C6-DA7R showed good stability in vitro and high binding ability to U87MG (glioma) cells. Systematic in vitro antitumor investigations involving cytotoxicity, apoptosis, distribution of the cell cycle, and reactive oxygen species (ROS) clearly demonstrated that 211At-labeled heterodimeric peptides could significantly inhibit cell viability, induce cell apoptosis, arrest the cell cycle in G2/M phase, and increase intracellular ROS levels in a dose-dependent manner. Biodistribution revealed that iRGD-C6-lys(211At-ATE)-C6-DA7R had rapid tumor accumulation and fast normal tissue/organ clearance, which was mainly excreted through the kidneys. Moreover, in vivo therapeutic evaluation indicated that iRGD-C6-lys(211At-ATE)-C6-DA7R was able to obviously inhibit tumor growth and prolong the survival of mice bearing glioma xenografts without notable toxicity to normal organs. All these results suggest that TAT mediated by iRGD-C6-lys(211At-ATE)-C6-DA7R can provide an effective and promising strategy for the treatment of glioma and some other tumors.


Assuntos
Glioma , Integrinas , Animais , Linhagem Celular Tumoral , Glioma/metabolismo , Humanos , Integrinas/metabolismo , Camundongos , Peptídeos/metabolismo , Compostos Radiofarmacêuticos/farmacologia , Compostos Radiofarmacêuticos/uso terapêutico , Espécies Reativas de Oxigênio/uso terapêutico , Distribuição Tecidual
20.
Chemosphere ; 298: 134196, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35276103

RESUMO

The important role of microbes in the biomineralization and migration behavior of uranium in the field of environmental chemistry has been well emphasized in previous work. However, limited work on mineralization processes of indigenous microorganism has prevented us from a deeper understanding of the process and mechanisms of uranium biomineralization. In this work, the dynamic process and mechanism of uranium biomineralization in Enterobacter sp. X57, a novel uranium-tolerant microorganism separated from uranium contaminated soil, were systematically investigated. Enterobacter sp. X57 can induce intracellular mineralization of U (VI) to Uramphite (NH4UO2PO4·3H2O) under neutral conditions by alkaline phosphatase. In this biomineralization process, soluble U (VI) first bonded with the amino and phosphate groups on the plasma membrane, providing initial nucleation site for the formation of U (VI) biominerals. Then the impairment of cell barrier function and the enhancement of alkaline phosphatase metabolism occurred with the accumulation of uranium in cells, creating a possible pathway for soluble U (VI) to diffuse into the cell and be further mineralized into U (VI)-phosphate minerals. All the results revealed that the intracellular biomineralization of uranium by Enterobacter sp. X57 was a combined result of biosorption, intracellular accumulation and phosphatase metabolism. These findings may contribute to a better understanding of uranium biomineralization behavior and mechanism of microorganisms, as well as possible in-situ bioremediation strategies for uranium by indigenous microorganisms.


Assuntos
Urânio , Fosfatase Alcalina/metabolismo , Biodegradação Ambiental , Biomineralização , Enterobacter/metabolismo , Fosfatos/metabolismo , Urânio/química
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