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Alternating copolymers are crucial for diverse applications. While dispersity (Æ, also known as molecular weight distribution, MWD) influences the properties of polymers, achieving low dispersities in alternating copolymers poses a notable challenge via free radical polymerizations (FRPs). In this work, we demonstrated an unexpected discovery that dispersities are affected by the participation of charge transfer complexes (CTCs) formed between monomer pairs during free radical alternating copolymerization, which have inspired the successful synthesis of various alternating copolymers with low dispersities (>30 examples, Æ = 1.13-1.39) under visible-light irradiation. The synthetic method is compatible with binary, ternary and quaternary alternating copolymerizations and is expandable for both fluorinated and non-fluorinated monomer pairs. DFT calculations combined with model experiments indicated that CTC-absent reaction exhibits higher propagation rates and affords fewer radical terminations, which could contribute to low dispersities. Based on the integration of Monte Carlo simulation and Bayesian optimization, we established the relationship map between FRP parameter space and dispersity, further suggested the correlation between low dispersities and higher propagation rates. Our research sheds light on dispersity control via FRPs and creates a novel platform to investigate polymer dispersity through machine learning.
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This study aimed to quantitively profile the S-nitrosylation in beef semimembranosus (SM) with different treatments (nitric oxide donor or nitric oxide synthase inhibitor) by applying iodoTMT-based nitrosoproteomics. Results showed that 2096 S-nitrosylated cysteine sites in 368 proteins were detected in beef SM. Besides, differential SNO-modified proteins were screened, some of which were involved in crucial biochemical pathways, including calcium-releasing-related proteins, energy metabolic enzymes, myofibrils, and cytoskeletal proteins. GO analysis indicated that differential proteins were localized in a wide range of cellular compartments, such as cytoplasm, organelle, and mitochondrion, providing a prerequisite for S-nitrosylation exerting broad roles in post-mortem muscles. Furthermore, KEGG analysis validated that these proteins participated in the regulation of diverse post-mortem metabolic processes, especially glycolysis. To conclude, changes of S-nitrosylation levels in post-mortem muscles could impact the structure and function of crucial muscle proteins, which lead to different levels of muscle metabolism and ultimately affect beef quality.
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Proteínas Musculares , Músculo Esquelético , Proteômica , Carne Vermelha , Bovinos , Animais , Carne Vermelha/análise , Músculo Esquelético/química , Músculo Esquelético/metabolismo , Proteínas Musculares/metabolismo , Cisteína/metabolismo , Óxido Nítrico/metabolismo , Doadores de Óxido Nítrico/farmacologiaRESUMO
Garnet oxide is one of the most promising solid electrolytes for solid-state lithium metal batteries. However, the traditional interface modification layers cannot completely block electron migrating from the current collector to the interior of the solid-state electrolyte, which promotes the penetration of lithium dendrites. In this work, a highly electron-blocking interlayer composed of potassium fluoride (KF) is deposited on garnet oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO). After reacting with melted lithium metal, KF in-situ transforms to KF/LiF interlayer, which can block the electron leakage and inhibit lithium dendrite growth. The Li symmetric cells using the interlayer show a long cycle life of ~3000 hours at 0.2 mA cm-2 and over 350 hours at 0.5 mA cm-2 respectively. Moreover, an ionic liquid of LiTFSI in C4mim-TFSI is screened to wet the LLZTO|LiNi0.8Co0.1Mn0.1O2 (NCM) positive electrode interfaces. The Li|KF-LLZTO | NCM cells present a specific capacity of 109.3 mAh g-1, long lifespan of 3500 cycles and capacity retention of 72.5% at 25 °C and 2 C (380 mA g-1) with an average coulombic efficiency of 99.99%. This work provides a simple and integrated strategy on high-performance quasi-solid-state lithium metal batteries.
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[This corrects the article DOI: 10.1371/journal.pone.0103022.].
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PURPOSE: Oral Squamous Cell Carcinoma (OSCC) is the 6th most common cancer worldwide. It is generally aggressive and closely associated with chemoresistance and poor survival. There is accumulating evidence for the involvement of inhibitors of apoptosis proteins (IAPs), including IAP1 and XIAP, in mediating chemotherapy resistance in OSCC. Various strategies for targeting IAPs have been designed and tested in recent years and several small molecule IAP inhibitors are in clinical trials as monotherapies as well as in combination with radiotherapy and chemotherapy. The purpose of this study was to evaluate and compare the efficacy and biological activity of three IAP inhibitors both as stand-alone and sensitising agents to cisplatin in a preclinical model of squamous cell carcinoma of the tongue. METHODS: Cisplatin-sensitive SCC4 and -resistant SCC4cisR cells were utilised in this study. Apoptosis was evaluated by flow cytometric analysis of Annexin V/Propidium Iodide-stained cells. Expression of IAP proteins was determined by western blotting and knockdown of cIAP1, livin and XIAP was conducted by transfection of cells with siRNA. RESULTS: We establish for the first time the therapeutic efficacy of the Smac mimetic, BV6 and the XIAP inhibitor Embelin, for OSCC. Both of these IAP targeting agents synergistically enhanced cisplatin-mediated apoptotic cell death in resistant cells which was mediated in part by depletion of XIAP. In addition, knockdown of XIAP using siRNA enhanced cisplatin-mediated cell death, demonstrating the importance of targeting XIAP in this sensitisation. CONCLUSION: These findings provide pre-clinical evidence that IAP inhibition may be a valuable therapeutic option in OSCC.
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Carcinoma de Células Escamosas , Neoplasias Bucais , Humanos , Cisplatino/farmacologia , Carcinoma de Células Escamosas/tratamento farmacológico , Proteínas Inibidoras de Apoptose Ligadas ao Cromossomo X/genética , Proteínas Inibidoras de Apoptose Ligadas ao Cromossomo X/metabolismo , Linhagem Celular Tumoral , Neoplasias Bucais/tratamento farmacológico , Proteínas Inibidoras de Apoptose/genética , Proteínas Inibidoras de Apoptose/metabolismo , Apoptose/fisiologia , Proteínas de Transporte , RNA Interferente PequenoRESUMO
OBJECTIVE: This study aimed to investigate whether virtual monoenergetic images (VMIs) can aid radiologists and surgeons in better identifying the arc of Riolan (AOR) and to determine the optimal kilo electron volt (keV) level. METHODS: Thirty-three patients were included. Conventional images (CIs) and VMI (40-100 keV) were reconstructed using arterial phase spectral-based images. The computed tomography (CT) attenuation and noise of the AOR, the CT attenuation of the erector spinal muscle, and the background noise on VMI and CI were measured, respectively. The signal-to-noise ratio, contrast-to-noise ratio (CNR), and signal intensity ratio were calculated. The image quality of the AOR was evaluated according to a 4-point Likert grade. RESULTS: The CT attenuation, noise, CNR, and signal intensity ratio of the AOR were significantly higher in VMI at 40 and 50 keV compared with CI ( P < 0.001); VMI at 40 keV was significantly higher than 50 keV ( P < 0.05). No significant difference in signal-to-noise ratio, background noise, and CT attenuation of the spinal erector muscle was observed between VMI and CI ( P > 0.05). virtual monoenergetic image at 40 keV produced the best subjective scores. CONCLUSIONS: Virtual monoenergetic image at 40 keV makes it easier to observe the AOR with optimized subjective and objective image quality. This may prompt radiologists and surgeons to actively search for it and encourage surgeons to preserve it during splenic flexure takedown.
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Tomografia Computadorizada por Raios X , Humanos , Masculino , Feminino , Pessoa de Meia-Idade , Adulto , Tomografia Computadorizada por Raios X/métodos , Idoso , Razão Sinal-Ruído , Baço/diagnóstico por imagem , Estudos Retrospectivos , Interpretação de Imagem Radiográfica Assistida por Computador/métodos , Idoso de 80 Anos ou maisRESUMO
PURPOSE: The objective of this study was to investigate the efficacy of an artificial intelligence-assisted 3D planning system (AIHIP) in total hip arthroplasty by direct anterior approach and assess the reliability of the AIHIP preoperative program in terms of both interobserver and intraobserver agreement. METHODS: A retrospective analysis was conducted on patients who underwent unilateral primary THA via direct anterior approach from June 2019 to March 2022. Participants were randomly assigned to receive either the AIHIP system (n = 220) or the 2D template (control group) (n = 220) for preoperative planning. The primary outcome aimed to evaluate the correspondence between the prosthesis selected intro-operation and the one planned preoperatively, as well as to calculate the intraclass correlation coefficient (ICC). Secondary outcomes included operation time, intraoperative blood loss, fluoroscopy times, Harris hip score (HHS), lower limb length difference (LLD), femoral offset (FO), and bilateral femoral offset difference. RESULTS: No significant differences were observed in gender, age, body mass index (BMI), aetiology, and American Society of Anesthesiologists (ASA) score between the two groups. Both planning methods exhibited good intraobserver agreement for component planning (ICC: 0.941-0.976). Interobserver agreement for component planning was comparable between the two methods (ICC: 0.882-0.929). In the AIHIP group, the accuracy of acetabular cup and femoral stem prosthetics planning significantly improved, with accuracies within the size range of ± 0 and ± 1 being 76.8% and 90.5% and 79.5% and 95.5%, respectively. All differences between two groups were statistically significant (p < 0.05). Patients receiving AIHIP preoperative planning experienced shorter operation times, reduced intraoperative blood loss, fewer fluoroscopy times, and lower leg length discrepancy (LLD) (p < 0.05). Moreover, they demonstrated a higher Harris hip score (HHS) at three days post-surgery (p < 0.05). However, no significant differences were found in femoral offset (FO), difference of bilateral femoral offsets, and HHS at 1 month after the operation. CONCLUSION: Utilizing AIHIP for preoperative planning of direct anterior approach THA can significantly enhance the accuracy of prosthetic sizing with good reliability, decrease operation time, reduce intraoperative blood loss, and more effectively restore the length of both lower limbs. This approach has greater clinical application value.
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Artroplastia de Quadril , Prótese de Quadril , Humanos , Artroplastia de Quadril/efeitos adversos , Artroplastia de Quadril/métodos , Inteligência Artificial , Estudos Retrospectivos , Reprodutibilidade dos Testes , Perda Sanguínea Cirúrgica , Desigualdade de Membros Inferiores , Resultado do TratamentoRESUMO
This study explored the utility of quantitative real-time panfungal PCR assay in diagnosing invasive pulmonary fungal diseases (IPFD) in non-neutropenic patients. Panfungal PCR assay was performed on respiratory tract specimens from patients whose clinical signs could not exclude fungal infection. At the same time, the samples were subjected to bacterial and fungal culture, microscopic examination and galactomannan antigen (GM) test in order to find the sensitivity, specificity, positive predictive value (PPV) and negative predictive value (NPV) of the 4 diagnostic methods in proven and probable cases. 518 specimens were collected while 63 respiratory tract specimens tested by PCR had positive results. According to diagnostic criteria, 40 patients were diagnosed with IPFD, with 12 proven, 20 probable and 8 possible cases. Among these, 33 patients of PCR results were positive, most of which were from BALF samples (44.12%). 23 cases were caused by Aspergillus species, with Aspergillus fumigatus was the major cause. Other Aspergillus species, including Aspergillus flavus, Aspergillus terreus and Aspergillus nidulans were found in 1 sample respectively. Candida species were found in 5 samples, Pneumocystis jeroveci pneumonia (PJP) in 4 samples and Mucormycosis in 1 sample. An analysis of proven/probable diagnosis showed a sensitivity of 78.13%, specificity of 92.18%, PPV of 39.68% and NPV of 98.46% for PCR and 50%, 85.27%, 35.7%, 95.65% for GM test respectively. The Ct value difference between proven/probable and possible cases had no statistical significance (Pâ =â .824). Fungal culture showed a sensitivity of 17.5% while microscopic examination sensitivity of 32.5%. Through stratified analysis, no apparent correlation was found between the Ct value of the PCR assay and GM value (r: 0.223, Pâ =â .294). But a conjunction of the 2 tests raised the PPV of Aspergillus to 90%. As shown in this study, the panfungal RT-PCR assay has high sensitivity and consistency with serological test and culture. Its high PPV in the detection of Aspergillus and PJP were also evident.
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Infecções Fúngicas Invasivas , Pneumopatias Fúngicas , Humanos , Sensibilidade e Especificidade , Infecções Fúngicas Invasivas/diagnóstico , Pulmão , Reação em Cadeia da Polimerase em Tempo RealRESUMO
Two-dimensional membranes have shown promising potential for ion-selective separation due to their well-defined interlayer channels. However, the typical "trade-off" effect of throughput and selectivity limits their developments. Herein, we report a precise tailoring of monovalent cation sieving technology with enhanced water throughput via the intercalation of graphene-oxide membranes with selective crown ethers. By tuning the lamellar spacing of graphene oxide, a critical interlayer distance (â¼11.04 Å) is revealed to maximize water flux (53.4 mol m-2 h-2 bar-1) without sacrificing ion selectivity. As a result, the elaborately enlarged interlayer distance offers improved water permeance. Meanwhile, various specific cations with remarkably high selectivity can be separated in mixed solutions because of the strong chelation with crown ethers. This work opens up a new avenue for high-throughput and precise regulation of ion separations for various application scenarios.
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We investigate the mechanics of crack propagation in architected adhesive joints whose adherends are inspired to the base plate of the barnacle Amphibalanus (=Balanus) amphitrite, and feature an array of buried hollow cylindrical channels located perpendicularly to the direction of crack growth. Selective laser sintering is used to obtain the adherends that are subsequently bonded in the double cantilever beam configuration to ascertain the mechanics of crack growth. Finite element (FE) simulations are deployed to determine the strain energy release rate (ERR) and to elucidate the salient features of the fracture process. It is shown that the channels induce a modulation of the ERR and enable a crack tip shielding mechanism. Besides, FE simulations based on a cohesive zone approach indicate the occurrence of crack pinning/depinning cycles that are validated via experiments. A highlight of the present study is the use of a mechanoluminescent (ML) coating to unravel the evolution of the transient stress field in the crack tip region. The coating comprises an optical epoxy resin loaded with doped strontium aluminate phosphors (SrAl2O4/Eu2+) and converts mechanical energy into light emission with intensity proportional to the magnitude of mechanical stress. By combining the ML emission patterns with the stress distribution obtained from FEA, we unveil interesting details of snap-through cracking in architected bio-inspired adhesive joints.
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Background: Numerous studies have confirmed that inflammation promotes the occurrence, development and prognosis of colorectal cancer (CRC). Objective: This study focuses on the potentially prognostic value of the platelet-to-lymphocyte ratio (PLR) in CRC patients. Data Sources: This study was registered at PROSPERO (ID: CRD42020219215). Relative studies were searched on PubMed, Cochrane Library, Embase, Web of Science, and clinical trial databases by two back-to-back reviewers. Study Selection and Intervention: Studies were screened according to the predetermined inclusion and exclusion criteria, comparing prognosis differences between low PLR levels and high PLR levels for CRC patients. Main Outcome Measures: Studies were integrated and compared to analyze the value of PLR in predicting overall survival (OS), progression-free survival (PFS), cancer-specific survival (CSS), disease-free survival (DFS) and recurrence-free survival (RFS) of CRC. Results: Outcomes were compared using Review Manager (version 5.4) software from Cochrane Collaboration. A total of 27 literary works, including 13,330 patients, were incorporated into our study. The final results showed that higher PLR levels had worse OS (hazard ratio [HR] = 1.40, 95% confidence interval [CI] = 1.21-1.62, P < 0.00001), DFS (HR = 1.44, 95% CI = 1.09-1.90, P = 0.01) and RFS (HR = 1.48, 95% CI = 1.13-1.94, P = 0.005) than lower PLR levels, respectively. However, there was no evidence of significance for PFS (HR = 1.14, 95% CI = 0.84-1.54, P = 0.40) and CSS (HR = 1.16, 95% CI = 0.88-1.53, P = 0.28) in the final meta-analysis. Limitations: Our study has the following limitations. First of all, we only included literature published in English, which means that some publication bias may be inevitable. In addition, our study used aggregate data, not individual data; furthermore, we did not define the exact cut-off value representing the PLR level. Conclusion: An elevated PLR seems to be an adverse prognostic factor affecting survival outcomes in patients with CRC. Meanwhile, more prospective studies are required to confirm our conclusion.PROSPERO ID: CRD42020219215.
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Traditional lithium-ion batteries cannot meet the ever-increasing energy demands due to the unsatisfied graphite anode with sluggish electrochemical kinetics. Recently, the perovskite material family as anode attracts growing attention due to their advantages on specific capacity, rate capability, lifetime, and safety. Herein, a double perovskite La2 MnNiO6 synthesized by solid-state reaction method as a high-performance anode material for LIBs is reported. La2 MnNiO6 with an average operating potential of <0.8 V versus Li+ /Li exhibits a good rate capability. Besides, the Li|La2 MnNiO6 cells perform long cycle life without decay after 1000 cycles at 1C and a high cycling retention of 93% is observed after 3000 cycles at 6C. It reveals that this material maintains stable perovskite structure with cycling. Theoretical calculations further demonstrate the high electronic conductivity, low diffusion energy barrier, and structural stability of the lithiated La2 MnNiO6 . This study highlights the double perovskite type material as a promising anode for next-generation batteries.
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Compostos de Cálcio , Lítio , Condutividade Elétrica , EletrodosRESUMO
In order to finish a bloodmeal successfully, hematophagous organisms often stored a variety of anticoagulant proteins in their salivary glands, such as proteins that inhibit platelet aggregation. When they ingest a bloodmeal, these proteins are injected into the host to prevent the blood from clotting. As one of the origins of leeches used in traditional Chinese medicine, H. nipponia was proved to be clinically effective in treatment of cardiovascular and cerebrovascular diseases. This study cloned the sequence of HnSaratin cDNA derived from salivary glands of H. nipponia. The sequence contains an open reading frame of 387 bp, encoding a protein of 128 amino acids containing a signal peptide of 21 amino acids. After removal of the signal peptide, the molecular mass of mature HnSaratin was 12.37 kDa, with a theoretical isoelectric point (pI) of 3.89. The N-terminal of mature HnSaratin was folded into a globular structure, in which 3 disulfide bonds, a ßßαßßß topology and 2 Glu residues that binds collagenous Lys2 were located, and the C-terminal formed a flexible region. The fusion HnSaratin protein was obtained by a prokaryotic expression system. The protein showed anti-platelet aggregation activity, and was observed to prevent blood clotting in rats. The significant high expression of HnSaratin mRNA in salivary glands was induced by bloodmeal ingestion of H. nipponia. Briefly, our work provides theoretical basis for further development and utilization of H. nipponia.
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Sanguessugas , Animais , Ratos , Clonagem Molecular , Proteínas/genética , DNA Complementar/genética , DNA Complementar/metabolismo , Sinais Direcionadores de Proteínas/genética , Aminoácidos/genéticaRESUMO
In this work, nitrogen-doped graphene quantum dots (N-GQDs) were synthesized by an efficient one-step hydrothermal using hydrated citric acid and urea as the carbon and nitrogen sources, respectively. The fluorescent quantum yield of the N-GQDs was up to 88.20 %, and the fluorescence lifetime was 12.29 ns. Based on the excellent fluorescence property, water-soluble and low cytotoxicity of N-GQDs, a novel fluorescent probe was fabricated and used for simultaneous detection of l-glutamic acid (l-Glu) and l-aspartic acid (l-Asp). Herein, Al3+ was used as a chelant agent for l-Glu shielding. The sensitive response of the probe towards l-Glu and l-Asp presented a wide concentration range with a low detection limit (S/N = 3). The fluorescent probe showed good selectivity, high stability and acceptable reproducibility in the application of l-Glu/l-Asp simultaneous detection in chicken soup. Meanwhile, the detection results of the fluorescent probe were correlated well with those obtained by amino acid analyzer.
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Grafite , Pontos Quânticos , Pontos Quânticos/química , Grafite/química , Corantes Fluorescentes/química , Nitrogênio/química , Aminoácidos , Reprodutibilidade dos Testes , Espectrometria de Fluorescência/métodosRESUMO
Two-dimensional electron gas (2DEG) at the interface of amorphous Al2O3/SrTiO3 (aAO/STO) heterostructures has received considerable attention owing to its convenience of fabrication and relatively high mobility. The integration of these 2DEG heterostructures on a silicon wafer is highly desired for electronic applications but remains challanging up to date. Here, conductive aAO/STO heterostructures have been synthesized on a silicon wafer via a growth-and-transfer method. A scanning transmission electron microscopy image shows flat and close contact between STO membranes and a Si wafer. Electron energy loss spectroscopic measurements reveal the interfacial Ti valence state evolution, which identifies the formation of 2D charge carriers confined at the interface of aAO/STO. This work provides a feasible strategy for the integration of 2DEG on a silicon wafer and other desired substrates for potential functional and flexible electronic devices.
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Brain-computer interfaces (BCIs) based on motor imagery (MI) utilizing multi-channel electroencephalogram (EEG) data are commonly used to improve motor function of people with motor disabilities. EEG channel selection can enhance MI classification accuracy by selecting informative channels, accordingly reducing redundant information. The sequential backward floating search (SBFS) approach has been considered as one of the best feature selection methods. In this paper, SBFS is first implemented to select the optimal EEG channels in MI-BCI. Further, to reduce the time complexity of SBFS, the modified SBFS is proposed and applied to left and right hand MI tasks. In the modified SBFS, based on the map of EEG channels at the scalp, the symmetrical channels are selected as channel pairs and acceleration is thus realized by removing or adding multiple channels in each iteration. Extensive experiments were conducted on four public BCI datasets. Experimental results show that the SBFS achieves significantly higher classification accuracy (p < 0.001) than using all channels and conventional MI channels (i.e., C3, C4, and Cz). Moreover, the proposed method outperforms the state-of-the-art selection methods.
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To characterize species of viral mRNA transcripts generated during respiratory syncytial virus (RSV) infection, human fibroblast-like MRC-5 lung cells were infected with subgroup A RSV for 6, 16 and 24 hours. In addition, we characterised the viral transcriptome in infected Calu-3 lung epithelial cells at 48 hours post infection. Total RNA was harvested and polyadenylated mRNA was enriched and sequenced by direct RNA sequencing using an Oxford nanopore device. This platform yielded over 450,000 direct mRNA transcript reads which were mapped to the viral genome and analysed to determine the relative mRNA levels of viral genes using our in-house ORF-centric pipeline. We examined the frequency of polycistronic readthrough mRNAs were generated and assessed the length of the polyadenylated tails for each group of transcripts. We show a general but non-linear decline in gene transcript abundance across the viral genome, as predicted by the model of RSV gene transcription. However, the decline in transcript abundance is not uniform. The polyadenylate tails generated by the viral polymerase are similar in length to those generated by the host polyadenylation machinery and broadly declined in length for most transcripts as the infection progressed. Finally, we observed that the steady state abundance of transcripts with very short polyadenylate tails less than 20 nucleotides is less for N, SH and G transcripts in both cell lines compared to NS1, NS2, P, M, F and M2 which may reflect differences in mRNA stability and/or translation rates within and between the cell lines.
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Infecções por Vírus Respiratório Sincicial , Vírus Sincicial Respiratório Humano , Humanos , RNA Mensageiro/genética , RNA Viral/genética , Vírus Sincicial Respiratório Humano/genética , Infecções por Vírus Respiratório Sincicial/genética , Análise de Sequência de RNARESUMO
Here, we report a two-dimension (2D) superlattice-like membrane composed of periodic MoS2 and GO nanosheets, which delivers enhanced salt rejection capability, high water flux, and Li ion selectivity. It opens a new perspective in assembling 2D membranes and can be utilized as a green and low-cost approach for desalination.
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Ferroelectric domain wall memories have been proposed as a promising candidate for nonvolatile memories, given their intriguing advantages including low energy consumption and high-density integration. Perovskite oxides possess superior ferroelectric prosperities but perovskite-based domain wall memory integrated on silicon has rarely been reported due to the technical challenges in the sample preparation. Here, we demonstrate a domain wall memory prototype utilizing freestanding BaTiO3 membranes transferred onto silicon. While as-grown BaTiO3 films on (001) SrTiO3 substrate are purely c-axis polarized, we find they exhibit distinct in-plane multidomain structures after released from the substrate and integrated onto silicon due to the collective effects from depolarizing field and strain relaxation. Based on the strong in-plane ferroelectricity, conductive domain walls with reading currents up to nanoampere are observed and can be both created and erased artificially, highlighting the great potential of the integration of perovskite oxides with silicon for ferroelectric domain wall memories.
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[This retracts the article DOI: 10.1016/j.omtn.2020.09.036.].