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1.
Chem Rev ; 124(9): 5930-6050, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38687182

RESUMO

Since the last century, we have witnessed the development of molecular magnetism which deals with magnetic materials based on molecular species, i.e., organic radicals and metal complexes. Among them, the broadest attention was devoted to molecule-based ferro-/ferrimagnets, spin transition materials, including those exploring electron transfer, molecular nanomagnets, such as single-molecule magnets (SMMs), molecular qubits, and stimuli-responsive magnetic materials. Their physical properties open the application horizons in sensors, data storage, spintronics, and quantum computation. It was found that various optical phenomena, such as thermochromism, photoswitching of magnetic and optical characteristics, luminescence, nonlinear optical and chiroptical effects, as well as optical responsivity to external stimuli, can be implemented into molecule-based magnetic materials. Moreover, the fruitful interactions of these optical effects with magnetism in molecule-based materials can provide new physical cross-effects and multifunctionality, enriching the applications in optical, electronic, and magnetic devices. This Review aims to show the scope of optical phenomena generated in molecule-based magnetic materials, including the recent advances in such areas as high-temperature photomagnetism, optical thermometry utilizing SMMs, optical addressability of molecular qubits, magneto-chiral dichroism, and opto-magneto-electric multifunctionality. These findings are discussed in the context of the types of optical phenomena accessible for various classes of molecule-based magnetic materials.

2.
Plant J ; 119(2): 658-675, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38678590

RESUMO

Heat stress poses a significant threat to maize, especially when combined with drought. Recent research highlights the potential of water replenishment to ameliorate grain weight loss. However, the mitigating mechanisms of heat in drought stress, especially during the crucial early grain-filling stage, remain poorly understood. We investigated the mechanism for mitigating heat in drought stress by water replenishment from the 12th to the 32nd days after silking in a controlled greenhouse experiment (Exp. I) and field trial (Exp. II). A significant reduction in grain weight was observed in heat stress compared to normal conditions. When water replenishment was applied to increase soil water content (SWC) under heat stress, the grain yield exhibited a notable increase ranging from 28.4 to 76.9%. XY335 variety was used for transcriptome sequencing to analyze starch biosynthesis and amino acid metabolisms in Exp. I. With water replenishment, the transcripts of genes responsible for trehalose 6-phosphate phosphates (TPP), alpha-trehalase (TRE), ADP-glcpyrophosphorylase, and starch synthase activity were stimulated. Additionally, the expression of genes encoding TPP and TRE contributed to an enhanced conversion of trehalose to glucose. This led to the conversion of sucrose from glucose-1-phosphate to ADP-glucose and ADP-glucose to amylopectin, ultimately increasing starch production by 45.1%. Water replenishment to boost SWC during heat stress also elevated the levels of essential amino acids in maize, including arginine, serine, tyrosine, leucine, glutamic acid, and methionine, providing valuable support to maize plants in adversity. Field trials further validated the positive impact of water replenishment on SWC, resulting in a notable increase in grain yield ranging from 7.1 to 9.2%. This study highlights the vital importance of adapting to abiotic stress and underscores the necessity of developing strategies to counteract its adverse effects on crop yield.


Assuntos
Aminoácidos , Secas , Sacarose , Água , Zea mays , Zea mays/genética , Zea mays/fisiologia , Zea mays/metabolismo , Aminoácidos/metabolismo , Água/metabolismo , Sacarose/metabolismo , Grão Comestível/fisiologia , Grão Comestível/genética , Temperatura Alta , Regulação da Expressão Gênica de Plantas , Resposta ao Choque Térmico/fisiologia
3.
J Pathol ; 263(1): 99-112, 2024 05.
Artigo em Inglês | MEDLINE | ID: mdl-38411280

RESUMO

Desmoglein-2 (DSG2) is a transmembrane glycoprotein belonging to the desmosomal cadherin family, which mediates cell-cell junctions; regulates cell proliferation, migration, and invasion; and promotes tumor development and metastasis. We previously showed serum DSG2 to be a potential biomarker for the diagnosis of esophageal squamous cell carcinoma (ESCC), although the significance and underlying molecular mechanisms were not identified. Here, we found that DSG2 was increased in ESCC tissues compared with adjacent tissues. In addition, we demonstrated that DSG2 promoted ESCC cell migration and invasion. Furthermore, using interactome analysis, we identified serine/threonine-protein kinase D2 (PRKD2) as a novel DSG2 kinase that mediates the phosphorylation of DSG2 at threonine 730 (T730). Functionally, DSG2 promoted ESCC cell migration and invasion dependent on DSG2-T730 phosphorylation. Mechanistically, DSG2 T730 phosphorylation activated EGFR, Src, AKT, and ERK signaling pathways. In addition, DSG2 and PRKD2 were positively correlated with each other, and the overall survival time of ESCC patients with high DSG2 and PRKD2 was shorter than that of patients with low DSG2 and PRKD2 levels. In summary, PRKD2 is a novel DSG2 kinase, and PRKD2-mediated DSG2 T730 phosphorylation promotes ESCC progression. These findings may facilitate the development of future therapeutic agents that target DSG2 and DSG2 phosphorylation. © 2024 The Pathological Society of Great Britain and Ireland.


Assuntos
Neoplasias Esofágicas , Carcinoma de Células Escamosas do Esôfago , Humanos , Carcinoma de Células Escamosas do Esôfago/metabolismo , Fosforilação , Proteína Quinase D2 , Neoplasias Esofágicas/patologia , Linhagem Celular Tumoral , Proliferação de Células/fisiologia , Serina , Movimento Celular/fisiologia , Regulação Neoplásica da Expressão Gênica , Desmogleína 2/genética , Desmogleína 2/metabolismo
4.
J Am Chem Soc ; 146(25): 17103-17113, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38869216

RESUMO

Understanding the interfacial hydrogen evolution reaction (HER) is crucial to regulate the electrochemical behavior in aqueous zinc batteries. However, the mechanism of HER related to solvation chemistry remains elusive, especially the time-dependent dynamic evolution of the hydrogen bond (H-bond) under an electric field. Herein, we combine in situ spectroscopy with molecular dynamics simulation to unravel the dynamic evolution of the interfacial solvation structure. We find two critical change processes involving Zn-electroplating/stripping, including the initial electric double layer establishment to form an H2O-rich interface (abrupt change) and the subsequent dynamic evolution of an H-bond (gradual change). Moreover, the number of H-bonds increases, and their strength weakens in comparison with the bulk electrolyte under bias potential during Zn2+ desolvation, forming a diluted interface, resulting in massive hydrogen production. On the contrary, a concentrated interface (H-bond number decreases and strength enhances) is formed and produces a small amount of hydrogen during Zn2+ solvation. The insights on the above results contribute to deciphering the H-bond evolution with competition/corrosion HER during Zn-electroplating/stripping and clarifying the essence of electrochemical window widened and HER suppression by high concentration. This work presents a new strategy for aqueous electrolyte regulation by benchmarking the abrupt change of the interfacial state under an electric field as a zinc performance-enhancement criterion.

5.
Anal Chem ; 96(23): 9370-9378, 2024 06 11.
Artigo em Inglês | MEDLINE | ID: mdl-38683892

RESUMO

The development of sensors for detection of biomarkers exhibits an exciting potential in diagnosis of diseases. Herein, we propose a novel electrochemical sensing strategy for label-free dual-biomarker detection, which is based on the combination of stimulus-responsive molecularly imprinted polymer (MIP)-modified nanopores and a polymeric membrane chronopotentiometric sensor. The ion fluxes galvanostatically imposed on the sensing membrane surface can be blocked by the recognition reaction between the target biomarker in the sample solution and the stimulus-responsive MIP receptor in the nanopores, thus causing a potential change. By using two external stimuli (i.e., pH and temperature), the recognition abilities of the stimulus-responsive MIP receptor can be effectively modulated so that dual-biomarker label-free chronopotentiometric detection can be achieved. Using alpha fetoprotein (AFP) and prostate-specific antigen (PSA) as model biomarkers, the proposed sensor offers detection limits of 0.17 and 0.42 ng/mL for AFP and PSA, respectively.


Assuntos
Biomarcadores , Polímeros Molecularmente Impressos , Nanoporos , Antígeno Prostático Específico , alfa-Fetoproteínas , Antígeno Prostático Específico/análise , Polímeros Molecularmente Impressos/química , alfa-Fetoproteínas/análise , Humanos , Biomarcadores/análise , Limite de Detecção , Técnicas Eletroquímicas/métodos , Concentração de Íons de Hidrogênio , Técnicas Biossensoriais/métodos , Potenciometria/métodos , Polímeros/química , Impressão Molecular , Temperatura
6.
BMC Plant Biol ; 24(1): 57, 2024 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-38238675

RESUMO

γ -aminobutyric acid (GABA) is closely related to the growth, development and stress resistance of plants. Combined with the previous study of GABA to promote the cotton against abiotic stresses, the characteristics and expression patterns of GABA branch gene family laid the foundation for further explaining its role in cotton stress mechanism. Members of GAD, GAB-T and SSADH (three gene families of GABA branch) were identified from the Gossypium hirsutum, Gossypium barbadense, Gossypium arboreum and Gossypium raimondii genome. The GABA branch genes were 10 GAD genes, 4 GABA-T genes and 2 SSADH genes. The promoter sequences of genes mainly contains response-related elements such as light, hormone and environment.Phylogenetic analysis shows that GAD indicating that even in the same species, the homologous sequences in the family. The GABA-T gene of each cotton genus was in sum the family had gene loss in the process of dicotyledon evolution. SSADH families Gossypium hirsutum, Gossypium barbadense, Gossypium arboreum and Gossypium raimondii were closely related to the dicot plants.GABA gene is involved in the regulation of salt stress and high temperature in Gossypium hirsutum.GABA attenuated part of the abiotic stress damage by increasing leaf protective enzyme activity and reducing reactive oxygen species production.This lays the foundation for a thorough analysis of the mechanism of GABA in cotton stress resistance.


Assuntos
Gossypium , Família Multigênica , Gossypium/metabolismo , Filogenia , Genes de Plantas/genética , Estresse Fisiológico/genética , Regulação da Expressão Gênica de Plantas , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Genoma de Planta
7.
Small ; : e2406110, 2024 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-39113670

RESUMO

In this study, state-of-the-art on-line pyrolysis MS (OP-MS) equipped with temperature-controlled cold trap and on-line pyrolysis GC/MS (OP-GC/MS) injected through high-vacuum negative-pressure gas sampling (HVNPGS) programming are originally designed/constructed to identify/quantify the dynamic change of common permanent gases and micromolecule organics from the anode/cathode-electrolyte reactions during thermal runaway (TR) process, and corresponding TR mechanisms are further perfected/complemented. On LiCx anode side, solid electrolyte interphase (SEI) would undergo continuous decomposition and regeneration, and the R-H+ (e.g., HF, ROH, etc.) species derived from electrolyte decomposition would continue to react with Li/LiCx to generate H2. Up to above 200 °C, the O2 would release from the charged NCM cathode and organic radicals would be consumed/oxidized by evolved O2 to form COx, H2O, and more corrosive HF. On the contrary, charged LFP cathode does not present obvious O2 evolution during heating process and the unreacted flammable/toxic organic species would exit in the form of high temperature/high-pressure (HT/HP) vapors within batteries, indicating higher potential safety risks. Additionally, the in depth understanding of the TR mechanism outlined above provides a clear direction for the design/modification of thermostable electrodes and non-flammable electrolytes for safer batteries.

8.
BMC Cancer ; 24(1): 805, 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38969990

RESUMO

BACKGROUND: Differentiation of glioma and solitary brain metastasis (SBM), which requires biopsy or multi-disciplinary diagnosis, remains sophisticated clinically. Histogram analysis of MR diffusion or molecular imaging hasn't been fully investigated for the differentiation and may have the potential to improve it. METHODS: A total of 65 patients with newly diagnosed glioma or metastases were enrolled. All patients underwent DWI, IVIM, and APTW, as well as the T1W, T2W, T2FLAIR, and contrast-enhanced T1W imaging. The histogram features of apparent diffusion coefficient (ADC) from DWI, slow diffusion coefficient (Dslow), perfusion fraction (frac), fast diffusion coefficient (Dfast) from IVIM, and MTRasym@3.5ppm from APTWI were extracted from the tumor parenchyma and compared between glioma and SBM. Parameters with significant differences were analyzed with the logistics regression and receiver operator curves to explore the optimal model and compare the differentiation performance. RESULTS: Higher ADCkurtosis (P = 0.022), frackurtosis (P<0.001),and fracskewness (P<0.001) were found for glioma, while higher (MTRasym@3.5ppm)10 (P = 0.045), frac10 (P<0.001),frac90 (P = 0.001), fracmean (P<0.001), and fracentropy (P<0.001) were observed for SBM. frackurtosis (OR = 0.431, 95%CI 0.256-0.723, P = 0.002) was independent factor for SBM differentiation. The model combining (MTRasym@3.5ppm)10, frac10, and frackurtosis showed an AUC of 0.857 (sensitivity: 0.857, specificity: 0.750), while the model combined with frac10 and frackurtosis had an AUC of 0.824 (sensitivity: 0.952, specificity: 0.591). There was no statistically significant difference between AUCs from the two models. (Z = -1.14, P = 0.25). CONCLUSIONS: The frac10 and frackurtosis in enhanced tumor region could be used to differentiate glioma and SBM and (MTRasym@3.5ppm)10 helps improving the differentiation specificity.


Assuntos
Neoplasias Encefálicas , Glioma , Humanos , Neoplasias Encefálicas/diagnóstico por imagem , Neoplasias Encefálicas/secundário , Neoplasias Encefálicas/patologia , Glioma/diagnóstico por imagem , Glioma/patologia , Feminino , Masculino , Pessoa de Meia-Idade , Adulto , Diagnóstico Diferencial , Idoso , Imagem de Difusão por Ressonância Magnética/métodos , Curva ROC , Imageamento por Ressonância Magnética/métodos
9.
Nucleic Acids Res ; 50(D1): D817-D827, 2022 01 07.
Artigo em Inglês | MEDLINE | ID: mdl-34718748

RESUMO

Virus infections are huge threats to living organisms and cause many diseases, such as COVID-19 caused by SARS-CoV-2, which has led to millions of deaths. To develop effective strategies to control viral infection, we need to understand its molecular events in host cells. Virus related functional genomic datasets are growing rapidly, however, an integrative platform for systematically investigating host responses to viruses is missing. Here, we developed a user-friendly multi-omics portal of viral infection named as MVIP (https://mvip.whu.edu.cn/). We manually collected available high-throughput sequencing data under viral infection, and unified their detailed metadata including virus, host species, infection time, assay, and target, etc. We processed multi-layered omics data of more than 4900 viral infected samples from 77 viruses and 33 host species with standard pipelines, including RNA-seq, ChIP-seq, and CLIP-seq, etc. In addition, we integrated these genome-wide signals into customized genome browsers, and developed multiple dynamic charts to exhibit the information, such as time-course dynamic and differential gene expression profiles, alternative splicing changes and enriched GO/KEGG terms. Furthermore, we implemented several tools for efficiently mining the virus-host interactions by virus, host and genes. MVIP would help users to retrieve large-scale functional information and promote the understanding of virus-host interactions.


Assuntos
Bases de Dados Factuais , Interações entre Hospedeiro e Microrganismos , Viroses , Animais , Sequenciamento de Cromatina por Imunoprecipitação , Ontologia Genética , Genoma Viral , Sequenciamento de Nucleotídeos em Larga Escala , Interações entre Hospedeiro e Microrganismos/genética , Humanos , Metadados , Análise de Sequência de RNA , Software , Transcriptoma , Interface Usuário-Computador , Viroses/genética , Viroses/metabolismo , Navegador
10.
Nucleic Acids Res ; 50(D1): D279-D286, 2022 01 07.
Artigo em Inglês | MEDLINE | ID: mdl-34747466

RESUMO

RNA polymerase III (Pol III) transcribes hundreds of non-coding RNA genes (ncRNAs), which involve in a variety of cellular processes. However, the expression, functions, regulatory networks and evolution of these Pol III-transcribed ncRNAs are still largely unknown. In this study, we developed a novel resource, Pol3Base (http://rna.sysu.edu.cn/pol3base/), to decode the interactome, expression, evolution, epitranscriptome and disease variations of Pol III-transcribed ncRNAs. The current release of Pol3Base includes thousands of regulatory relationships between ∼79 000 ncRNAs and transcription factors by mining 56 ChIP-seq datasets. By integrating CLIP-seq datasets, we deciphered the interactions of these ncRNAs with >240 RNA binding proteins. Moreover, Pol3Base contains ∼9700 RNA modifications located within thousands of Pol III-transcribed ncRNAs. Importantly, we characterized expression profiles of ncRNAs in >70 tissues and 28 different tumor types. In addition, by comparing these ncRNAs from human and mouse, we revealed about 4000 evolutionary conserved ncRNAs. We also identified ∼11 403 tRNA-derived small RNAs (tsRNAs) in 32 different tumor types. Finally, by analyzing somatic mutation data, we investigated the mutation map of these ncRNAs to help uncover their potential roles in diverse diseases. This resource will help expand our understanding of potential functions and regulatory networks of Pol III-transcribed ncRNAs.


Assuntos
Bases de Dados Genéticas , Neoplasias/genética , RNA Polimerase III/genética , RNA não Traduzido/genética , Proteínas de Ligação a RNA/genética , Software , Fatores de Transcrição/genética , Animais , Mineração de Dados , Conjuntos de Dados como Assunto , Evolução Molecular , Regulação da Expressão Gênica , Redes Reguladoras de Genes , Humanos , Internet , Camundongos , Mutação , Neoplasias/classificação , Neoplasias/metabolismo , Neoplasias/patologia , RNA Polimerase III/metabolismo , RNA de Transferência/classificação , RNA de Transferência/genética , RNA de Transferência/metabolismo , RNA não Traduzido/classificação , RNA não Traduzido/metabolismo , Proteínas de Ligação a RNA/classificação , Proteínas de Ligação a RNA/metabolismo , Fatores de Transcrição/classificação , Fatores de Transcrição/metabolismo , Transcrição Gênica
11.
Nucleic Acids Res ; 50(D1): D421-D431, 2022 01 07.
Artigo em Inglês | MEDLINE | ID: mdl-34755848

RESUMO

tRNA-derived small RNA (tsRNA), a novel type of regulatory small noncoding RNA, plays an important role in physiological and pathological processes. However, the understanding of the functional mechanism of tsRNAs in cells and their role in the occurrence and development of diseases is limited. Here, we integrated multiomics data such as transcriptome, epitranscriptome, and targetome data, and developed novel computer tools to establish tsRFun, a comprehensive platform to facilitate tsRNA research (http://rna.sysu.edu.cn/tsRFun/ or http://biomed.nscc-gz.cn/DB/tsRFun/). tsRFun evaluated tsRNA expression profiles and the prognostic value of tsRNAs across 32 types of cancers, identified tsRNA target molecules utilizing high-throughput CLASH/CLEAR or CLIP sequencing data, and constructed the interaction networks among tsRNAs, microRNAs, and mRNAs. In addition to its data presentation capabilities, tsRFun offers multiple real-time online tools for tsRNA identification, target prediction, and functional enrichment analysis. In summary, tsRFun provides a valuable data resource and multiple analysis tools for tsRNA investigation.


Assuntos
Bases de Dados de Ácidos Nucleicos , MicroRNAs/genética , Neoplasias/genética , RNA Mensageiro/genética , Pequeno RNA não Traduzido/genética , RNA de Transferência/genética , Software , Sequenciamento de Cromatina por Imunoprecipitação , Regulação Neoplásica da Expressão Gênica , Genoma Humano , Sequenciamento de Nucleotídeos em Larga Escala , Humanos , Internet , MicroRNAs/classificação , MicroRNAs/metabolismo , Neoplasias/diagnóstico , Neoplasias/metabolismo , Neoplasias/mortalidade , Conformação de Ácido Nucleico , Prognóstico , RNA Mensageiro/classificação , RNA Mensageiro/metabolismo , Pequeno RNA não Traduzido/classificação , Pequeno RNA não Traduzido/metabolismo , RNA de Transferência/classificação , RNA de Transferência/metabolismo , Análise de Sobrevida , Transcriptoma
12.
Mikrochim Acta ; 191(10): 588, 2024 09 10.
Artigo em Inglês | MEDLINE | ID: mdl-39256210

RESUMO

Different morphological Cu2O nanoparticles including cube, truncated cube, and octahedron were successfully prepared by a selective surface stabilization strategy. The prepared cube Cu2O exhibited superior peroxidase-like activity over the other two morphological Cu2O nanoparticles, which can readily oxidize 3,3',5,5'-tetramethylbenzidine (TMB) to form visually recognizable color signals. Consequently, a sensitive and simple colorimetric biosensor was proposed for deoxynivalenol (DON) detection. In this biosensor, the uniform cube Cu2O was employed as the vehicle to label the antibody for the recognition of immunoreaction. The sensing strategy showed a detection limit as low as 0.01 ng/mL, and a wide linear range from 2 to 100 ng/mL. Concurrently, the approximate DON concentration can be immediately and conveniently observed by the vivid color changes. Benefiting from the high sensitivity and selectivity of the designed biosensor, the detection of DON in wheat, corn, and tap water samples was achieved, suggesting the bright prospect of the biosensor for the convenient and intuitive detection of DON in actual samples.


Assuntos
Benzidinas , Técnicas Biossensoriais , Colorimetria , Cobre , Limite de Detecção , Nanopartículas Metálicas , Tricotecenos , Zea mays , Tricotecenos/análise , Tricotecenos/imunologia , Colorimetria/métodos , Cobre/química , Técnicas Biossensoriais/métodos , Benzidinas/química , Zea mays/química , Nanopartículas Metálicas/química , Triticum/química , Peroxidase/química , Anticorpos Imobilizados/imunologia , Contaminação de Alimentos/análise
13.
Nano Lett ; 23(8): 3565-3572, 2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37026665

RESUMO

The prominent problem with graphite anodes in practical applications is the detrimental Li plating, resulting in rapid capacity fade and safety hazards. Herein, secondary gas evolution behavior during the Li-plating process was monitored by online electrochemical mass spectrometry (OEMS), and the onset of local microscale Li plating on the graphite anode was precisely/explicitly detected in situ/operando for early safety warnings. The distribution of irreversible capacity loss (e.g., primary and secondary solid electrolyte interface (SEI), dead Li, etc.) under Li-plating conditions was accurately quantified by titration mass spectroscopy (TMS). Based on OEMS/TMS results, the effect of typical VC/FEC additives was recognized at the level of Li plating. The nature of vinylene carbonate (VC)/fluoroethylene carbonate (FEC) additive modification is to enhance the elasticity of primary and secondary SEI by adjusting organic carbonates and/or LiF components, leading to less "dead Li" capacity loss. Though VC-containing electrolyte greatly suppresses the H2/C2H4 (flammable/explosive) evolution during Li plating, more H2 is released from the reductive decomposition of FEC.

14.
Molecules ; 29(13)2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38999155

RESUMO

The composite photocatalyst FeOOH/g-C3N4 was prepared through thermal polycondensation and co-precipitation methods, followed by XRD, SEM and UV-vis characterization. The stability of FeOOH/g-C3N4 was explored by the recycling test. The active species in the reaction system were investigated by the capture experiment. The results indicated that the optimal preparation condition for g-C3N4 involved calcination at 600 °C for 4 h. XRD analysis revealed that g-C3N4 exhibits a high-purity phase, and Fe in FeOOH/g-C3N4 exists in a highly dispersed amorphous state. SEM analysis showed that FeOOH/g-C3N4 has a rough surface with an irregular layered structure. Element composition analysis confirmed that the content of elements in the prepared catalyst is consistent with the theoretical calculation. FeOOH/g-C3N4 possesses the largest specific surface area of 143.2 m2/g and a suitable pore distribution. UV-vis DRS analysis showed that the absorption intensity of FeOOH/g-C3N4 is stronger than that of g-C3N4. When the catalyst dosage was 1.0 g/L, the H2O2 dosage was 4 mmol/L, the PNP initial concentration was 10 mg/L and the initial pH value was 5, the PNP removal could reach 92% in 120 min. Even after 5 cycles, the efficiency of PNP removal by FeOOH/g-C3N4 remains nearly 80%. The capture experiment indicated that both •OH and •O2- play roles in the photocatalytic degradation of PNP, with •OH being more significant. These findings affirm that FeOOH has been successfully incorporated into g-C3N4, resulting in a conspicuous catalytic effect on the degradation of PNP in the visible light-assisted Fenton-like reaction.

15.
Angew Chem Int Ed Engl ; 63(25): e202401559, 2024 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-38616720

RESUMO

Air self-charging aqueous batteries promise to integrate energy harvesting technology and battery systems, potentially overcoming a heavy reliance on energy and the spatiotemporal environment. However, the exploitation of multifunctional air self-charging battery systems using promising cathode materials and suitable charge carriers remains challenging. Herein, for the first time, we developed low-temperature self-charging aqueous Zn-K hybrid ion batteries (AZKHBs) using a fully conjugated hexaazanonaphthalene (HATN)-based porous aromatic framework as the cathode material, exhibiting redox chemistry using K+ as charge carriers, and regulating Zn-ion solvation chemistry to guide uniform Zn plating/stripping. The unique AZKHBs exhibit the exceptional electrochemical properties in all-climate conditions. Most importantly, the large potential difference causes the AZKHBs discharged cathode to be oxidized using oxygen, thereby initiating a self-charging process in the absence of an external power source. Impressively, the air self-charging AZKHBs can achieve a maximum voltage of 1.15 V, an impressive discharge capacity (466.3 mAh g-1), and exceptional self-charging performance even at -40 °C. Therefore, the development of self-charging AZKHBs offers a solution to the limitations imposed by the absence of a power grid in harsh environments or remote areas.

16.
Angew Chem Int Ed Engl ; 63(13): e202314650, 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38296796

RESUMO

Exploiting advanced amphiphilic solid catalysts is crucial to the development of Pickering emulsion catalysis. Herein, covalent organic framework (COF) nanoparticles constructed with highly hydrophobic monomers as linkers were found to show superior amphiphilicity and they were then developed as a new class of solid emulsifiers for Pickering emulsion catalysis. Employing amphiphilic COFs as solid emulsifiers, Pickering emulsions with controllable emulsion type and droplet sizes were obtained. COF materials have also been demonstrated to serve as porous surface coatings to replace traditional surface modifications for stabilizing Pickering emulsions. After implanting Pd nanoparticles into amphiphilic COFs, the obtained catalyst displayed a 3.9 times higher catalytic efficiency than traditional amphiphilic solid catalysts with surface modifications in the biphasic oxidation reaction of alcohols. Such an enhanced activity was resulted from the high surface area and regular porous structure of COFs. More importantly, because of their tunable pore diameters, Pickering emulsion catalysis with remarkable size selectivity was achieved. This work is the first example that COFs were applied in Pickering emulsion catalysis, providing a platform for exploring new frontiers of Pickering emulsion catalysis.

17.
Angew Chem Int Ed Engl ; : e202412214, 2024 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-39141606

RESUMO

Electrolyte engineering is crucial for improving cathode electrolyte interphase (CEI) to enhance the performance of lithium-ion batteries, especially at high charging cut-off voltages. However, typical electrolyte modification strategies always focus on the solvation structure in the bulk region, but consistently neglect the dynamic evolution of electrolyte solvation configuration at the cathode-electrolyte interface, which directly influences the CEI construction. Herein, we reveal an anti-synergy effect between Li+-solvation and interfacial electric field by visualizing the dynamic evolution of electrolyte solvation configuration at the cathode-electrolyte interface, which determines the concentration of interfacial solvated-Li+. The Li+ solvation in the charging process facilitates the construction of a concentrated (Li+-solvent/anion-rich) interface and anion-derived CEI, while the repulsive force derived from interfacial electric field induces the formation of a diluted (solvent-rich) interface and solvent-derived CEI. Modifying the electrochemical protocols and electrolyte formulation, we regulate the "inflection voltage" arising from the anti-synergy effect and prolong the lifetime of the concentrated interface, which further improves the functionality of CEI architecture.

18.
Angew Chem Int Ed Engl ; 63(17): e202400254, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38441399

RESUMO

Acting as a passive protective layer, solid-electrolyte interphase (SEI) plays a crucial role in maintaining the stability of the Li-metal anode. Derived from the reductive decomposition of electrolytes (e.g., anion and solvent), the SEI construction presents as an interfacial process accompanied by the dynamic de-solvation process during Li-metal plating. However, typical electrolyte engineering and related SEI modification strategies always ignore the dynamic evolution of electrolyte configuration at the Li/electrolyte interface, which essentially determines the SEI architecture. Herein, by employing advanced electrochemical in situ FT-IR and MRI technologies, we directly visualize the dynamic variations of solvation environments involving Li+-solvent/anion. Remarkably, a weakened Li+-solvent interaction and anion-lean interfacial electrolyte configuration have been synchronously revealed, which is difficult for the fabrication of anion-derived SEI layer. Moreover, as a simple electrochemical regulation strategy, pulse protocol was introduced to effectively restore the interfacial anion concentration, resulting in an enhanced LiF-rich SEI layer and improved Li-metal plating/stripping reversibility.

19.
J Cell Mol Med ; 27(1): 101-112, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36524848

RESUMO

Discordant abundances of different immune cell subtypes is regarded to be an essential feature of tumour tissue. Direct studies in Prostate cancer (PC) of intratumoral immune heterogeneity characterized by immune cell subtype, are still lacking. Using the single sample gene set enrichment analysis (ssGSEA) algorithm, the abundance of 28 immune cells infiltration (ICI) were determined for PC. A NMF was performed to determine tumour-sample clustering based on the abundance of ICI and PFS information. Hub genes of clusters were identified via weighted gene co-expression network analysis (WGCNA). The multivariate dimensionality reduction analysis of hub genes expression matrix was carried out via principal component analysis (PCA) to obtain immune score (IS). We analysed the correlation between clustering, IS and clinical phenotype. We divided the 495 patients into clusterA (n = 193) and clusterB (n = 302) on the basis of ICI and PFS via NMF. The progression-free survival (PFS) were better for clusterA than for clusterB (p < 0.001). Each immune cell subtypes was more abundant in clusterA than in clusterB (p < 0.001). The expression levels of CTAL-4 and PD-L1 were lower in clusterB than in clusterA (p < 0.001 and p = 0.006). We obtained 103 hub genes via WGCNA. In the training and validation cohorts, the prognosis of high IS group was worse than that of the low IS group (p < 0.05). IS had good predictive effect on 5-year PFS. The expression of immune checkpoint genes was higher in the low IS group than in the high IS group (p < 0.01). Patients with low IS and receiving hormone therapy had better prognosis than other groups. The combination of IS and clinical characteristics including lymph node metastasis and gleason score can better differentiate patient outcomes than using it alone. IS was a practical algorithm to predict the prognosis of patients. Advanced PC patients with low IS may be more sensitive to hormone therapy. CXCL10, CXCL5, MMP1, CXCL12, CXCL11, CXCL2, STAT1, IL-6 and TLR2 were hub genes, which may drive the homing of immune cells in tumours and promote immune cell differentiation.


Assuntos
Carcinoma , Neoplasias da Próstata , Humanos , Masculino , Algoritmos , Hormônios , Neoplasias da Próstata/genética
20.
J Am Chem Soc ; 145(42): 22934-22944, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37824191

RESUMO

Knowledge of the magnetic domain is indispensable for understanding the magnetostatic properties of magnets. However, to date, the magnetic domain has not yet been reported in the field of molecule-based magnets. Herein, we study the magnetic domains of molecule-based magnets. Two magnetic films of iron/chromium hexacyanidochromate FexCr1-x[Cr(CN)6]2/3·5H2O (x = 0; Film 1 and x = 0.2; Film 2) were prepared for investigation. The temperature evolution of surface magnetization was measured using magnetic force microscopy. Film 1 showed a magnetic domain below Curie temperature (TC) and its positive-magnetic polarization increased monotonously with decreasing temperature, while Film 2 showed positive magnetic polarization below TC and switches from positive to negative magnetization through a demagnetization state at 146 K. This study originally reports the temperature variation of the magnetization state at the magnetization reversal. The magnetic domains appeared as a maze pattern with an approximate domain size of one-to-several micrometers. This work shows that research on molecule-based magnets can be expanded from magnetochemistry to the magnetostatic engineering of bulk magnets, molecule-based magnetostatic engineering.

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