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1.
Adv Mater ; : e2403584, 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38897229

RESUMO

Despite multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters with small full-width at half maximum are attractive for wide color-gamut display and eye-protection lighting applications, their inefficient reverse intersystem crossing (RISC) process and long exciton lifetime induce serious efficiency roll-off, which significantly limits their development. Herein, a novel device concept of building highly efficient tricomponent exciplex with multiple RISC channels is proposed to realize reduced exciton quenching and enhanced upconversion of nonradiative triplet excitons, and subsequently used as a host for high-performance MR-TADF organic light-emitting diodes (OLEDs). Compared with traditional binary exciplex, the tricomponent exciplex exhibits obviously improved photoluminescence quantum yield, emitting dipole orientation and RISC rate constant, and a record-breaking external quantum efficiency (EQE) of 30.4% is achieved for tricomponent exciplex p-PhBCzPh: PO-T2T: DspiroAc-TRZ (50: 20: 30) based OLED. Remarkably, maximum EQEs of 36.2% and 40.3% and ultralow efficiency roll-off with EQEs of 26.1% and 30.0% at 1000 cd m-2 are respectively achieved for its sky-blue and pure-green MR-TADF doped OLEDs. Additionally, the blue emission unit hosted by tricomponent exciplex is combined with an orange-red TADF emission unit to achieve a double-emission-layer blue-hazard-free warm white OLED with an EQEmax of 30.3% and stable electroluminescence spectra over a wide brightness range.

2.
Respir Res ; 25(1): 244, 2024 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-38886760

RESUMO

BACKGROUND: Evidence suggests that radiotherapy is a potent immunomodulator in non-small cell lung cancer (NSCLC). Conversely, it has rarely been demonstrated if immune infiltration can influence radiotherapy efficacy. Herein, we explored the effect of tumor-infiltrating lymphocytes (TILs) on the response to postoperative radiotherapy (PORT) in completely resected stage III-pN2 NSCLC. METHODS: This retrospective study included 244 patients with pathologically confirmed stage III-N2 NSCLC who underwent complete resection at our institution between 2014 and 2020. TILs were assessed with permanent full-face hematoxylin and eosin (H&E) sections and the evaluation of TILs was based on a published guideline. Patients were stratified into the TILlow or TILhigh group with a cutoff value of 50%. Kaplan-Meier method and Log-rank test were utilized to assess disease-free survival (DFS) and overall survival (OS). Univariate and multivariate Cox regression analysis were conducted to determine prognostic indicators. RESULTS: Among 244 patients, a total of 121 patients received PORT whereas 123 did not. TILs level in patients with PORT was significantly higher than that in patients without PORT (p < 0.001). High TILs level was significantly associated with an improved DFS and OS in all the entire chort (DFS, p < 0.001; OS, p = 0.001), PORT chort (DFS, p = 0.003; OS, p = 0.011) and non-PORT chort (DFS, p < 0.001; OS, p = 0.034). There were no significant survival differences between different treatment modalities in the low TILs infiltration (DFS, p = 0.244; OS, p = 0.404) and high TILs infiltration (DFS, p = 0.167; OS, p = 0.958) groups. CONCLUSIONS: TILs evaluated with H&E sections could represent a prognostic biomarker in patients with completely resected pN2 NSCLC, and high TILs infiltration was associated with favorable survival outcomes.The predictive value of TILs for PORT still need to be further explored in the future.


Assuntos
Biomarcadores Tumorais , Carcinoma Pulmonar de Células não Pequenas , Neoplasias Pulmonares , Linfócitos do Interstício Tumoral , Humanos , Carcinoma Pulmonar de Células não Pequenas/imunologia , Carcinoma Pulmonar de Células não Pequenas/radioterapia , Carcinoma Pulmonar de Células não Pequenas/patologia , Carcinoma Pulmonar de Células não Pequenas/cirurgia , Feminino , Masculino , Estudos Retrospectivos , Linfócitos do Interstício Tumoral/imunologia , Neoplasias Pulmonares/imunologia , Neoplasias Pulmonares/radioterapia , Neoplasias Pulmonares/patologia , Neoplasias Pulmonares/cirurgia , Neoplasias Pulmonares/mortalidade , Pessoa de Meia-Idade , Idoso , Prognóstico , Valor Preditivo dos Testes , Estadiamento de Neoplasias , Radioterapia Adjuvante , Adulto , Pneumonectomia
3.
J Environ Manage ; 365: 121605, 2024 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-38944962

RESUMO

The interfacial charge transfer ability is a decisive factor influencing the photocatalytic performance of composite photocatalysts. Compared with heterojunctions that combine two or more semiconductors with different properties, homojunctions that combine two semiconductors with similar properties can accelerate the interfacial charge shift and achieve higher photocatalyticability. In this study, a Zn3In2S6/ZnIn2S4 homojunction photocatalyst (ZIS-5) with a Zn3In2S6 to ZnIn2S4 molar ratio of 5:1 was synthesized by selecting Zn3In2S6 nano-microspheres as the substrate material and growing ZnIn2S4 flocs on the nano-microspheres. The photocatalytic performance of the ZIS-5 homojunction was assessed by using tetracycline (TC) as a typical pollutant. The photocatalytic performance and mineralization rate of the ZIS-5 homojunction were significantly improved compared with those of Zn3In2S6 and ZnIn2S4, and its photocatalytic performance was increased by 10.2% and 20.9%, compared with Zn3In2S6 and ZnIn2S4, respectively, while the mineralization rate was enhanced by 22.78% and 43.28%, respectively. The results of the comparison experiment revealed that the interfacial electron transfer ability of the ZIS-5 homojunction is 1.6 times that of the g-C3N4/ZnIn2S4-5 heterojunction. The density functional theory (DFT) computation and Mott-Schottky plots verified the formation of an internal electric field. The toxicity analysis showed that the ZIS-5 homojunction system effectively reduced the toxicity of TC. This work supplies a valuable route for inventing catalysts with efficient photocatalytic performances.

4.
Nat Commun ; 15(1): 4293, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38858360

RESUMO

Membrane proteins are critical to biological processes and central to life sciences and modern medicine. However, membrane proteins are notoriously challenging to study, mainly owing to difficulties dictated by their highly hydrophobic nature. Previously, we reported QTY code, which is a simple method for designing water-soluble membrane proteins. Here, we apply QTY code to a transmembrane receptor, histidine kinase CpxA, to render it completely water-soluble. The designed CpxAQTY exhibits expected biophysical properties and highly preserved native molecular function, including the activities of (i) autokinase, (ii) phosphotransferase, (iii) phosphatase, and (iv) signaling receptor, involving a water-solubilized transmembrane domain. We probe the principles underlying the balance of structural stability and activity in the water-solubilized transmembrane domain. Computational approaches suggest that an extensive and dynamic hydrogen-bond network introduced by QTY code and its flexibility may play an important role. Our successful functional preservation further substantiates the robustness and comprehensiveness of QTY code.


Assuntos
Histidina Quinase , Proteínas de Membrana , Solubilidade , Água , Água/química , Água/metabolismo , Histidina Quinase/metabolismo , Histidina Quinase/química , Histidina Quinase/genética , Proteínas de Membrana/metabolismo , Proteínas de Membrana/química , Proteínas de Membrana/genética , Ligação de Hidrogênio , Interações Hidrofóbicas e Hidrofílicas , Engenharia de Proteínas , Domínios Proteicos
5.
Chemistry ; : e202401635, 2024 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-38794783

RESUMO

The adverse aggregated-caused quenching (ACQ) problem of most electroluminescent materials existing in highly doped thin films is one of the key factors impeding the commercialization of high-efficiency organic light-emitting diodes (OLEDs) panel. Whereas, by delicately constructing and modulating moderate intermolecular interactions, some aggregates have been demonstrated to present distinct luminescent properties such as tunable emission spectra, improved photoluminescence quantum yields, different emission mechanism and enhanced horizontal transition dipole ratio (Θ) of emitting layer, providing feasible solution for ACQ problem. The luminescence from newly generated emissive state in aggregates is different from the traditional "isolated" molecules in organic electronics and will possess novel properties and applications. Herein, we summarize the different types of intermolecular interactions within emitter aggregates exhibiting distinct luminescent mechanisms, as well as their effects on photoluminescent and electroluminescent properties, offering reliable reference for the advancement of highly efficient OLEDs utilizing aggregated emitters.

6.
J Mol Biol ; 436(10): 168568, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38583515

RESUMO

Porphyromonas gingivalis, an anaerobic CFB (Cytophaga, Fusobacterium, and Bacteroides) group bacterium, is the keystone pathogen of periodontitis and has been implicated in various systemic diseases. Increased antibiotic resistance and lack of effective antibiotics necessitate a search for new intervention strategies. Here we report a 3.5 Å resolution cryo-EM structure of P. gingivalis RNA polymerase (RNAP). The structure displays new structural features in its ω subunit and multiple domains in ß and ß' subunits, which differ from their counterparts in other bacterial RNAPs. Superimpositions with E. coli RNAP holoenzyme and initiation complex further suggest that its ω subunit may contact the σ4 domain, thereby possibly contributing to the assembly and stabilization of initiation complexes. In addition to revealing the unique features of P. gingivalis RNAP, our work offers a framework for future studies of transcription regulation in this important pathogen, as well as for structure-based drug development.


Assuntos
Proteínas de Bactérias , RNA Polimerases Dirigidas por DNA , Porphyromonas gingivalis , Proteínas de Bactérias/química , Microscopia Crioeletrônica , RNA Polimerases Dirigidas por DNA/química , Escherichia coli , Modelos Moleculares , Porphyromonas gingivalis/enzimologia , Conformação Proteica , Subunidades Proteicas/química
7.
Artigo em Inglês | MEDLINE | ID: mdl-38652619

RESUMO

Cross-modal hashing (CMH) has attracted considerable attention in recent years. Almost all existing CMH methods primarily focus on reducing the modality gap and semantic gap, i.e., aligning multi-modal features and their semantics in Hamming space, without taking into account the space gap, i.e., difference between the real number space and the Hamming space. In fact, the space gap can affect the performance of CMH methods. In this paper, we analyze and demonstrate how the space gap affects the existing CMH methods, which therefore raises two problems: solution space compression and loss function oscillation. These two problems eventually cause the retrieval performance deteriorating. Based on these findings, we propose a novel algorithm, namely Semantic Channel Hashing (SCH). Firstly, we classify sample pairs into fully semantic-similar, partially semantic-similar, and semantic-negative ones based on their similarity and impose different constraints on them, respectively, to ensure that the entire Hamming space is utilized. Then, we introduce a semantic channel to alleviate the issue of loss function oscillation. Experimental results on three public datasets demonstrate that SCH outperforms the state-of-the-art methods. Furthermore, experimental validations are provided to substantiate the conjectures regarding solution space compression and loss function oscillation, offering visual evidence of their impact on the CMH methods. Codes are available at https://github.com/hutt94/SCH.

8.
Exp Eye Res ; 243: 109899, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38636802

RESUMO

Virus-like particles (VLP) are a promising tool for intracellular gene delivery, yet their potential in ocular gene therapy remains underexplored. In this study, we bridged this knowledge gap by demonstrating the successful generation and application of vesicular stomatitis virus glycoprotein (VSVG)-pseudotyped mouse PEG10 (MmPEG10)-VLP for intraocular mRNA delivery. Our findings revealed that PEG10-VLP can efficiently deliver GFP mRNA to adult retinal pigment epithelial cell line-19 (ARPE-19) cells, leading to transient expression. Moreover, we showed that MmPEG10-VLP can transfer SMAD7 to inhibit epithelial-mesenchymal transition (EMT) in RPE cells effectively. In vivo experiments further substantiated the potential of these vectors, as subretinal delivery into adult mice resulted in efficient transduction of retinal pigment epithelial (RPE) cells and GFP reporter gene expression without significant immune response. However, intravitreal injection did not yield efficient ocular expression. We also evaluated the transduction characteristics of MmPEG10-VLP following intracameral delivery, revealing transient GFP protein expression in corneal endothelial cells without significant immunotoxicities. In summary, our study established that VSVG pseudotyped MmPEG10-based VLP can transduce mitotically inactive RPE cells and corneal endothelial cells in vivo without triggering an inflammatory response, underscoring their potential utility in ocular gene therapy.


Assuntos
Técnicas de Transferência de Genes , RNA Mensageiro , Epitélio Pigmentado da Retina , Animais , Camundongos , Epitélio Pigmentado da Retina/metabolismo , RNA Mensageiro/genética , Terapia Genética/métodos , Vetores Genéticos , Camundongos Endogâmicos C57BL , Humanos , Proteínas de Fluorescência Verde/genética , Transição Epitelial-Mesenquimal , Glicoproteínas de Membrana/genética , Glicoproteínas de Membrana/metabolismo
9.
Behav Brain Res ; 465: 114958, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38485056

RESUMO

The lateral hypothalamic nucleus (LHy) is located in the dorsolateral hypothalamus of birds, and it is essential to many life processes. However, limited information is available about the role of LHy in mediating locomotive behaviors. In this work, we investigated the structure and function of LHy in pigeons (Columba livia) by Nissl staining, immunohistochemical (IHC) staining, insituhybridization (ISH) staining and constant current stimulation methods. The results showed that LHy appears crescent in shape, and three-dimensional coordinate value range of LHy is: A: 5.0-8.0 mm, L: 0.7-1.2 mm, D: 9.5-10.3 mm. The dopaminergic neurons in LHy were distributed in small amount and concentrated manner, while the glutamatergic neurons were distributed in a large number and uniform manner. The distribution of the above two neurons at each coronal level showed a significant positive correlation (R2 = 0.7516, P < 0.001). Our work demonstrated that LHy mainly mediates forward movement (P < 0.01) and ipsilateral lateral movement (P < 0.001), and these movements were significantly effected by electrical stimulation intensity. Our results showed that LHy can mediate the generation of directional behavior and this will provide technical support for the study of locomotor behavior regulation in birds.


Assuntos
Columbidae , Região Hipotalâmica Lateral , Animais , Hipotálamo/fisiologia , Neurônios
10.
Sci Total Environ ; 926: 171778, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38513872

RESUMO

Cr(III)-substituted ferrihydrite (Fh-Cr(III)) is widespread in the surrounding environment of mining areas. Fh-Cr(III) is unstable and susceptible to the influence of environmental factors, such as dissolved organic matter (DOM) and light, so Cr species embedded in mineral crystal layers are likely to have more profound negative effects on the environment with the photochemical behaviors of minerals. However, the photochemical behaviors of Fh-Cr(III) in the presence of DOM remains poorly understood. For this reason, citric acid (CA) was chosen as the representative DOM to study its combined effects with visible light irradiation on Fh-Cr(III) dissolution and phase transition. The results showed that CA hindered the agglomeration of Fh-Cr(III) particles, thereby slowing the phase transition of Fh-Cr(III). However, CA exacerbated the release of Fe and Cr by maintaining Fh-Cr(III) under unstable crystal structure. Moreover, due to the occurrence of ligand-metal charge transfer (LMCT) in (CA)n-Fh-Cr(III) formed on the Fh-Cr(III) surface, the synergistic effect between CA and light irradiation greatly promoted the dissolution of Fh-Cr(III). In the mixed system of Fh-Cr(III) (3 g/L) and CA (5 mM) at initial pH 3.0, the maximum concentrations of TFe and TCr were 18.17 and 5.68 mg/L after 6 h of light reaction, which were 1.82 and 3.62 times of those in the corresponding system in the darkness. Meanwhile, the Fe(III)/Fe(II) cycling in solution and solid surfaces was affected by various reactive oxygen species (ROS) generated from the LMCT process, in which the photoproduced Fe(II) further accelerated Cr(III) dissolution under acidic solution. The fast release of Cr(III) may pose greater danger to the environment as the more toxic Cr(VI) can be easily formed through the oxidation of dissolved Cr(III). This work offers fresh insights into the migration and transformation of Cr elements in the natural environment.

11.
ACS Appl Mater Interfaces ; 16(10): 12637-12646, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38441047

RESUMO

Sulfhydryl-based polyimides were synthesized by the nucleophilic ring-opening reaction of thiolactone monomers (BPDA-T, ODPA-T, BTDA-T) with polyethylenimine (PEI), and they were coated on carbon nanotubes as host materials (BPTP@CNT, ODTP@CNT, and BTTP@CNT) of the sulfur cathode. BPTP@CNT/S, ODTP@CNT/S, and BTTP@CNT/S as cathode materials not only promote the covalent bonding of sulfur and polysulfide with sulfhydryl-based polyimides but also reduce the shuttle effect of soluble polysulfide in the redox process. Moreover, sulfhydryl-based polyimides can help improve the compatibility and interfacial contact between sulfur and conductive carbon while alleviating the volume expansion of the cathode. In addition, the conductive network of carbon nanotubes improves the electronic conductivity of the cathode materials. The BTTP@CNT/S cathode showed superior stability (the initial capacity was 902 mAh g-1 at 1C, and the capacity retention rate was 88.58% after 500 cycles) and the initial capacity could reach 718 mAh g-1 when the sulfur loading was 4.8 mg cm-2 (electrolyte/sulfur ratio: 10 µL mg-1), which fully proves the feasibility of the large-scale application of sulfhydryl-based polyimide materials.

12.
Sci Total Environ ; 918: 170351, 2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38307288

RESUMO

Iron and manganese (hydrogen) oxides (IMHOs) exhibit excellent redox capabilities for environmental pollutants and are commonly used in situ chemical oxidation (ISCO) technologies for the degradation of organic pollutants. However, the coexisting dissolved organic matter (DOMs) in surface environments would influence the degradation behavior and fate of organic pollutants in IMHOs-based ISCO. This review has summarized the interactions and mechanisms between DOMs and IMHOs, as well as the properties of DOM-IMHOs complexes. Importantly, the promotion or inhibition impact of DOM was discussed from three perspectives. First, the presence of DOMs may hinder the accessibility of active sites on IMHOs, thus reducing their efficiency in degrading organic pollutants. The formation of compounds between DOMs and IMHOs alters their stability and activity in the degradation process. Second, the presence of DOMs may also affect the generation and transport of active species, thereby influencing the oxidative degradation process of organic pollutants. Third, specific components within DOMs also participate and affect the degradation pathways and rates. A comprehensive understanding of the interaction between DOMs and IMHOs helps to better understand and predict the degradation process of organic pollutants mediated by IMHOs in real environmental conditions and contributes to the further development and application of IMHO-mediated ISCO technology.

13.
Mol Oncol ; 18(6): 1649-1664, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38327028

RESUMO

Stage pIIIA/N2 non-small cell lung cancer (NSCLC) is primarily treated by complete surgical resection combined with neoadjuvant/adjuvant therapies. However, up to 40% of patients experience tumor recurrence. Here, we studied 119 stage pIIIA/N2 NSCLC patients who received complete surgery plus adjuvant chemotherapy (CT) or chemoradiotherapy (CRT). The paired tumor and resection margin samples were analyzed using next-generation sequencing (NGS). Although all patients were classified as negative resection margins by histologic methods, NGS revealed that 47.1% of them had molecularly positive surgical margins. Patients who tested positive for NGS-detected residual tumors had significantly shorter disease-free survival (DFS) (P = 0.002). Additionally, metastatic lymph node ratio, erb-b2 receptor tyrosine kinase 2 (ERBB2) mutations, and SWI/SNF-related, matrix-associated, actin-dependent regulator of chromatin, subfamily a, member 4 (SMARCA4) mutations were also independently associated with DFS. We used these four features to construct a COX model that could effectively estimate recurrence risk and prognosis. Notably, mutational profiling through broad-panel NGS could more sensitively detect residual tumors than the conventional histologic methods. Adjuvant CT and adjuvant CRT exhibited no significant difference in eliminating locoregional recurrence risk for stage pIIIA/N2 NSCLC patients with molecularly positive surgical margins.


Assuntos
Carcinoma Pulmonar de Células não Pequenas , Neoplasias Pulmonares , Recidiva Local de Neoplasia , Humanos , Carcinoma Pulmonar de Células não Pequenas/patologia , Carcinoma Pulmonar de Células não Pequenas/genética , Carcinoma Pulmonar de Células não Pequenas/cirurgia , Carcinoma Pulmonar de Células não Pequenas/terapia , Carcinoma Pulmonar de Células não Pequenas/metabolismo , Feminino , Pessoa de Meia-Idade , Masculino , Neoplasias Pulmonares/patologia , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/cirurgia , Prognóstico , Idoso , Recidiva Local de Neoplasia/genética , Recidiva Local de Neoplasia/patologia , Margens de Excisão , Intervalo Livre de Doença , Estadiamento de Neoplasias , Mutação , Adulto , Sequenciamento de Nucleotídeos em Larga Escala
14.
Comput Struct Biotechnol J ; 23: 278-286, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38173876

RESUMO

G protein-coupled receptors (GPCRs) play a pivotal role in fundamental biological processes and disease development. GPCR isoforms, derived from alternative splicing, can exhibit distinct signaling patterns. Some highly-truncated isoforms can impact functional performance of full-length receptors, suggesting their intriguing regulatory roles. However, how these truncated isoforms interact with full-length counterparts remains largely unexplored. Here, we computationally investigated the interaction patterns of three human GPCRs from three different classes, ADORA1 (Class A), mGlu2 (Class C) and SMO (Class F) with their respective truncated isoforms because their homodimer structures have been experimentally determined, and they have truncated isoforms deposited and identified at protein level in Uniprot database. Combining the neural network-based AlphaFold2 and two physics-based protein-protein docking tools, we generated multiple complex structures and assessed the binding affinity in the context of atomistic molecular dynamics simulations. Our computational results suggested all the four studied truncated isoforms showed potent binding to their counterparts and overlapping interfaces with homodimers, indicating their strong potential to block homodimerization of their counterparts. Our study offers insights into functional significance of GPCR truncated isoforms and supports the ubiquity of their regulatory roles.

15.
Proteins ; 92(2): 206-218, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37795805

RESUMO

Therapeutic monoclonal antibodies are the most rapidly growing class of molecular medicine, and they are beneficial to the treatment of a broad spectrum of human diseases. However, the aggregation of antibodies during the process of manufacture, distribution, and storage poses significant challenges, potentially compromising efficacy and inducing adverse immune responses. We previously conceived a QTY (glutamine, threonine, tyrosine) code, a simple tool for enhancing protein water-solubility by systematically pairwise replacing hydrophobic residues L (leucine), V (valine)/I (isoleucine), and F (phenylalanine). The QTY code offers a promising alternative to traditional methods of controlling aggregation in integral transmembrane proteins. In this study, we designed variants of four antibodies applying the QTY code, changing only the ß-sheets. Through the structure-based aggregation analysis, we found that these QTY antibody variants demonstrated significantly decreased aggregation propensity compared to their wild-type counter parts. Our results of molecular dynamics simulations showed that the design by QTY code is capable of maintaining the antigen-binding affinity and structural stability. Our structural informatic and computational study suggests that the QTY code offers a significant potential in mitigating antibody aggregation.


Assuntos
Anticorpos Monoclonais , Tirosina , Humanos , Anticorpos Monoclonais/genética , Anticorpos Monoclonais/química , Tirosina/metabolismo , Simulação de Dinâmica Molecular , Treonina , Biologia Computacional/métodos
16.
J Environ Manage ; 351: 119876, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38157577

RESUMO

The removal of organic pollutants by biochar has been extensively studied. However, the differences in the removal mechanisms of contaminants by biochar obtained from different preparation techniques have not been thoroughly elucidated. In this study, the catalytic performances of hydrochar (HC) and pyrochar (PC) were compared in the dark and light. Owing to more persistent free radicals (PFRs), greater defects and stronger charge transfer ability on the surface, PC could produce a certain concentration of superoxide radicals (•O2-) even in the dark, making its degradation efficiency for benzoic acid (BA) 11% higher than that of HC. On the contrary, when the light was turned on, HC rather than PC can generate a higher amount of hydroxyl radical (•OH), resulting in an 11% higher degradation efficiency of BA compared to PC. The improvement of catalytic performance in HC originated from its oxygen-containing functional groups (OFGs), which was beneficial for its effective production of singlet oxygen (1O2) and ·OH under light exposure. For PC, its photocatalytic activity depended mainly on the formation of 1O2 induced by the triplet of DOM (dissolved organic matter), but the lack of oxidative ·OH in its system leads to a lower degradation efficiency than that of HC. To prove the universal applicability of this rule for biochar materials, HC and PC materials obtained from soybean residue were also prepared for degrading BA. This work is devoted to an in-depth exploration of the catalytic activation mechanism of biochar obtained by different technological methods, and can create conditions for the generation of more dominant reactive oxygen species (ROS) on biochar, thus providing the guidance for environmental remediation.


Assuntos
Carvão Vegetal , Superóxidos , Espécies Reativas de Oxigênio , Radicais Livres/química , Carvão Vegetal/química , Superóxidos/química , Oxigênio/química
17.
Int J Mol Sci ; 24(22)2023 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-38003455

RESUMO

Chemokine receptors play crucial roles in fundamental biological processes. Their malfunction may result in many diseases, including cancer, autoimmune diseases, and HIV. The oligomerization of chemokine receptors holds significant functional implications that directly affect their signaling patterns and pharmacological responses. However, the oligomerization patterns of many chemokine receptors remain poorly understood. Furthermore, several chemokine receptors have highly truncated isoforms whose functional role is not yet clear. Here, we computationally show homo- and heterodimerization patterns of four human chemokine receptors, namely CXCR2, CXCR7, CCR2, and CCR7, along with their interaction patterns with their respective truncated isoforms. By combining the neural network-based AlphaFold2 and physics-based protein-protein docking tool ClusPro, we predicted 15 groups of complex structures and assessed the binding affinities in the context of atomistic molecular dynamics simulations. Our results are in agreement with previous experimental observations and support the dynamic and diverse nature of chemokine receptor dimerization, suggesting possible patterns of higher-order oligomerization. Additionally, we uncover the strong potential of truncated isoforms to block homo- and heterodimerization of chemokine receptors, also in a dynamic manner. Our study provides insights into the dimerization patterns of chemokine receptors and the functional significance of their truncated isoforms.


Assuntos
Simulação de Dinâmica Molecular , Transdução de Sinais , Humanos , Dimerização , Isoformas de Proteínas
18.
Nat Neurosci ; 26(12): 2081-2089, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37996529

RESUMO

It is generally thought that under basal conditions, neurons produce ATP mainly through mitochondrial oxidative phosphorylation (OXPHOS), and glycolytic activity only predominates when neurons are activated and need to meet higher energy demands. However, it remains unknown whether there are differences in glucose metabolism between neuronal somata and axon terminals. Here, we demonstrated that neuronal somata perform higher levels of aerobic glycolysis and lower levels of OXPHOS than terminals, both during basal and activated states. We found that the glycolytic enzyme pyruvate kinase 2 (PKM2) is localized predominantly in the somata rather than in the terminals. Deletion of Pkm2 in mice results in a switch from aerobic glycolysis to OXPHOS in neuronal somata, leading to oxidative damage and progressive loss of dopaminergic neurons. Our findings update the conventional view that neurons uniformly use OXPHOS under basal conditions and highlight the important role of somatic aerobic glycolysis in maintaining antioxidant capacity.


Assuntos
Glicólise , Fosforilação Oxidativa , Animais , Camundongos , Fosfotransferases/metabolismo , Estresse Oxidativo , Glucose/metabolismo
19.
Nat Commun ; 14(1): 5836, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37730807

RESUMO

Hydrogen spillover is the migration of activated hydrogen atoms from a metal particle onto the surface of catalyst support, which has made significant progress in heterogeneous catalysis. The phenomenon has been well researched on oxide supports, yet its occurrence, detection method and mechanism on non-oxide supports such as metal-organic frameworks (MOFs) remain controversial. Herein, we develop a facile strategy for efficiency enhancement of hydrogen spillover on various MOFs with the aid of water molecules. By encapsulating platinum (Pt) nanoparticles in MOF-801 for activating hydrogen and hydrogenation of C=C in the MOF ligand as activated hydrogen detector, a research platform is built with Pt@MOF-801 to measure the hydrogenation region for quantifying the efficiency and spatial extent of hydrogen spillover. A water-assisted hydrogen spillover path is found with lower migration energy barrier than the traditional spillover path via ligand. The synergy of the two paths explains a significant boost of hydrogen spillover in MOF-801 from imperceptible existence to spanning at least 100-nm-diameter region. Moreover, such strategy shows universality in different MOF and covalent organic framework materials for efficiency promotion of hydrogen spillover and improvement of catalytic activity and antitoxicity, opening up new horizons for catalyst design in porous crystalline materials.

20.
Heliyon ; 9(8): e18324, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37554834

RESUMO

Aging is the strongest risk factor for cardiovascular disease, with progressive decline in the function of vascular endothelial cells (ECs) with age. Systematic analyses of the effects of aging on different cardiac EC types remain limited. Here, we constructed a scRNA atlas of EC transcriptomes in young and old mouse hearts. We identified 10 EC subclusters. The multidimensionally differential genes (DEGs) analysis across different EC clusters shows molecular changes with aging, showing the increase in the overall inflammatory microenvironment and the decrease in angiogenesis and cytoskeletal support capacity of aged ECs. And we performed an in-depth analysis of 3 special ECs, Immunology, Proliferating and Angiogenic. The Immunology EC seems highly associated with some immune regulatory functions, which decline with aging at different degrees. Analysis of two types of neovascular ECs, Proliferating, Angiogenic, implied that Angiogenic ECs can differentiate into multiple EC directions after initially originating from proliferating ECs. And aging leads to a decrease in the ability of vascular angiogenesis and differentiation. Finally, we summarized the effects of aging on cell signaling communication between different EC clusters. This cardiac EC atlas offers comprehensive insights into the molecular regulations of cardiovascular aging, and provides new directions for the prevention and treatment of age-related cardiovascular disease.

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