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Short nanopores find extensive applications, capitalizing on their high throughput and detection resolution. Ionic behaviors through long nanopores are mainly determined by charged inner-pore walls. When pore lengths decrease to sub-200 nm, charged exterior surfaces provide considerable modulation to ion current. We find that the charge status of inner-pore walls affects the modulation of ion current from charged exterior surfaces. For 50-nm-long nanopores with neutral inner-pore walls, the charged exterior surfaces on the voltage (surfaceV) and ground (surfaceG) sides enhance and inhibit the ion transport by forming ion enrichment and depletion zones inside nanopores, respectively. For nanopores with both charged inner-pore and exterior surfaces, continuous electric double layers enhance the ion transport through nanopores significantly. The charged surfaceV results in higher ion current by simultaneously weakening the ion depletion at pore entrances and enhancing the intra-pore ion enrichment. The charged surfaceG expedites the exit of ions from nanopores, resulting in a decrease in ion enrichment at pore exits. Through adjustment in the width of charged-ring regions near pore boundaries, the effective charged width of the charged exterior is explored at â¼20 nm. Our results may provide a theoretical guide for further optimizing the performance of nanopore-based applications, such as seawater desalination, biosensing, and osmotic energy conversion.
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Additive engineering has emerged as one of the most promising strategies to improve the performance of perovskite solar cells (PSCs). Among additives, perovskite nanocrystals (NCs) have a similar chemical composition and matched lattice structure with the perovskite matrix, which can effectively enhance the efficiency and stability of PSCs. However, relevant studies remain limited, and most of them focus on bromide-involved perovskite NCs, which may undergo dissolution and ion exchange within the FAPbI3 host, potentially resulting in an enlarged band gap. In this work, we employ butylamine-capped CsPbI3 NCs (BPNCs) as additives in PSCs, which can be well maintained and serve as seeds for regulating the crystallization and growth of perovskite films. The resultant perovskite film exhibits larger domain sizes and fewer grain boundaries without compromising the band gap. Moreover, BPNCs can alleviate lattice strain and reduce defect densities within the active layer. The PSCs incorporating BPNCs show a champion power conversion efficiency (PCE) of up to 25.41 %, well over both Control of 22.09 % and oleic acid/oleylamine capped CsPbI3 NC (PNC)-based devices of 23.11 %. This work illustrates the key role of nanosized seed surfaces in achieving high-performance photovoltaic devices.
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Microfluidic chips have been widely applied in biology and medical research for stably generating uniform droplets that can be solidified into hydrogel microspheres. However, issues such as low microsphere yield, lengthy experimental processes, and susceptibility to environmental interference need to be addressed. In this work, a simple and effective method was developed to modify microfluidic chips at room temperature to improve the production performance of hydrogel microspheres. Numerical simulation-assisted experiments were conducted to comprehensively understand the effect of solution viscosity, hydrophilicity, and flow rate ratio on droplet formation during microsphere production. Chitosan was selected as the main component and combined with poly(ethylene glycol) diacrylate to prepare photocurable hydrogel microspheres as a demonstration. As a result, grafting fluoro-silane (FOTS) increased the contact angle of the channel from 90 to approximately 110°, which led to a 12.2% increase in droplet yield. Additionally, FOTS-modification attenuated the impact of the flow rate ratio on droplet yield by 19.1%. Alternatively, depositing dopamine decreased the channel's contact angle from 90 to 60°, resulting in a 21.4% increase in particle size and enabling the chip to adjust droplet size over a wider range. Further study demonstrates that the obtained hydrogel microspheres can be modified with layers of aldehyde, which can potentially be used for controlled drug release. Overall, this study proposed a facile method for adjusting the yield and droplet size through surface treatment of microfluidic chips while also enhancing the understanding of the synergistic effects of multiple factors in microfluidics-based microsphere production.
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All-inorganic lead halide perovskite (CsPbX3 , X = Cl, Br, I, or their mixture) nanocrystals (NCs) have achieved inspiring advancements in optoelectronic fields but still suffer from poor durability when exposed to environmental stimuli such as water, irradiation and heat. Herein, a strategy of employing pyrophosphate as the inert shell for CsPbX3 NCs is reported. The strong binding between pyrophosphate and CsPbBr3 surface can stabilize the perovskite structure well. The as-obtained core@shell CsPbBr3 @NH4 AlP2 O7 NCs exhibit impressive stability against water and maintain the initial optical properties with negligible change in 400 days. Furthermore, significant improvement of irradiation/thermal resistance is realized due to the protecting role of pyrophosphate. The NCs can retain 100% and ≈90% of the original PL after hundreds of heating/cooling cycles and several hundred hours of UV light irradiation, respectively. As a result, the core@shell products can be directly used for high-resolution inkjet printing, enabling the printed fluorescent information to be resistant under harsh environmental conditions. This work provides a promising way for the synthesis of highly stable encapsulated perovskite NCs and demonstrates a great potential in practical applications.
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Nanopartículas , Agua , Difosfatos , Nanopartículas/químicaRESUMEN
As an important property of porous membranes, the surface charge property determines many ionic behaviors of nanopores, such as ionic conductance and selectivity. Based on the dependence of electric double layers on bulk concentrations, ionic conductance through nanopores at high and low concentrations is governed by the bulk conductance and surface charge density, respectively. Here, through the investigation of ionic conductance inside track-etched single polyethylene terephthalate (PET) nanopores under various concentrations, the surface charge density of PET membranes is extracted as â¼-0.021 C/m2 at pH 10 over measurements with 40 PET nanopores. Simulations show that surface roughness can cause underestimation in surface charge density due to the inhibited electroosmotic flow. Then, the averaged pore size and porosity of track-etched multipore PET membranes are characterized by the developed ionic conductance method. Through coupled theoretical predictions in ionic conductance under high and low concentrations, the averaged pore size and porosity of porous membranes can be obtained simultaneously. Our method provides a simple and precise way to characterize the pore size and porosity of multipore membranes, especially for those with sub-100 nm pores and low porosities.
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Nanoporos , Polímeros , Porosidad , Propiedades de Superficie , Iones/química , Tereftalatos Polietilenos/químicaRESUMEN
Besides the dominant NaCl, natural seawater/river water contains trace multivalent ions, which can provide effective screening of surface charges. Here, in both negatively and positively charged nanopores, influences from divalent ions as counterions and co-ions have been investigated with respect to the performance of osmotic energy conversion (OEC) under natural salt gradients. As counterions, trace Ca2+ ions can suppress the electric power and conversion efficiency significantly. The reduced OEC performance is due to the bivalence and low diffusion coefficient of Ca2+ ions instead of the uphill transport of divalent ions discovered in the previous work. Effectively screened charged surfaces by Ca2+ ions induce an enhanced diffusion of Cl- ions which simultaneously decreases the net ion penetration and ionic selectivity of the nanopore. As co-ions, Ca2+ ions have weak effects on the OEC performance. The promotion from charged exterior surfaces in OEC processes for ultrashort nanopores is also studied, with an effective region of â¼200 nm in width beyond pore boundaries independent of the presence of Ca2+ ions. Our results shed light on the physical details of the nanofluidic OEC process under natural seawater/river water conditions, which can provide a useful guide for high-performance osmotic energy harvesting.
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Ríos , Cloruro de Sodio , Iones , Agua de Mar , AguaRESUMEN
Electrochemical processes occurring at solid/solid and solid/membrane interfaces govern the behavior of a variety of energy storage devices, including electrocatalytic reactions at electrode/membrane interfaces in fuel cells and ion insertion at electrode/electrolyte interfaces in solid-state batteries. Due to the heterogeneity of these systems, interrogation of interfacial activity at nanometer length scales is desired to understand system performance, yet the buried nature of the interfaces makes localized activity inaccessible to conventional electrochemical techniques. Herein, we demonstrate nanoscale electrochemical imaging of hydrogen evolution at individual Pt nanoparticles (PtNPs) positioned at a buried interface using scanning electrochemical cell microscopy (SECCM). Specifically, we image the hydrogen evolution reaction (HER) at individual carbon-supported PtNP electrocatalysts covered by a 100 to 800 nm thick layer of the proton exchange membrane Nafion. The rate of hydrogen evolution at PtNP at this buried interface is shown to be a function of Nafion thickness, with the highest activity observed for â¼200 nm thick films.
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Nanopores that exhibit ionic current rectification (ICR) behave like diodes such that they transport ions more efficiently in one direction than in the other. Conical nanopores have been shown to rectify ionic current, but only those with at least 500 nm in length exhibit significant ICR. Here, through the finite element method, we show how ICR of conical nanopores with lengths below 200 nm can be tuned by controlling individual charged surfaces, that is, the inner pore surface (surfaceinner) and exterior pore surfaces on the tip and base side (surfacetip and surfacebase). The charged surfaceinner and surfacetip can induce obvious ICR individually, while the effects of the charged surfacebase on ICR can be ignored. The fully charged surfaceinner alone could render the nanopore counterion-selective and induces significant ion concentration polarization in the tip region, which causes reverse ICR compared to nanopores with all surfaces charged. In addition, the direction and degree of rectification can be further tuned by the depth of the charged surfaceinner. When considering the exterior membrane surface only, the charged surfacetip causes intrapore ionic enrichment and depletion under opposite biases, which results in significant ICR. Its effective region is within â¼40 nm beyond the tip orifice. We also found that individual charged parts of the pore system contributed to ICR in an additive way because of the additive effect on the ion concentration regulation along the pore axis. With various combinations of fully/partially charged surfaceinner and surfacetip, diverse ICR ratios from â¼2 to â¼170 can be achieved. Our findings shed light on the mechanism of ICR in ultrashort conical nanopores and provide a useful guide to the design and modification of ultrashort conical nanopores in ionic circuits and nanofluidic sensors.
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The electrochemical reduction of deuterons (2D+ + 2e- â D2) at Pt nanodisk electrodes (radius = 15-100 nm) in D2O solutions containing deuterium chloride (DCl) results in the formation of a single gas nanobubble at the electrode surface. Analogous to that previously observed for the electrochemical generation of H2 nanobubbles, the nucleation and growth of a stable D2 nanobubble is characterized in voltammetric experiments by a highly reproducible and well-resolved sudden drop in the faradaic current, a consequence of restricted mass transport of D+ to the electrode surface following the liquid-to-gas phase transition. D2 nanobubbles are stable under potential control due to a dynamic equilibrium existing between D2 gas dissolution and electrochemical generation of D2 at the circumference of the Pt nanodisk electrode. Remarkably, within the error of the experimental measurement (<6%), the electrochemical current required to nucleate a D2 gas phase in a D2O solution is identical to that for the H2 gas phase in a H2O solutions, indicating that the concentration required for nucleating a D2 nanobubble in D2O (0.29 M) is â¼1.25 times larger than that for a H2 nanobubble (0.23 M), while the supersaturation is â¼300 in each case. We further demonstrate that individual nanobubbles can be electrogenerated in mixed D2O/H2O solutions containing both D+ and H+ at respective individual concentrations well below those required to nucleate a gas phase containing either pure D2 or H2. This latter finding indicates that the resulting nanobubbles comprise a mixture of D2, H2, and HD molecules with the chemical composition of a nanobubble determined by the concentrations and diffusivities of D+ and H+ in the mixed D2O/H2O solutions.
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A large number of SNPs significant for osteoporosis (OP) had been identified by genome-wide association studies. However, the underlying association mechanisms were largely unknown. From the perspective of protein phosphorylation, gene expression regulation, and bone cell activity, this study aims to illustrate association mechanisms for representative SNPs of interest. We utilized public databases and bioinformatics tool to identify OP-associated SNPs which potentially influence protein phosphorylation (phosSNPs). Associations with hip/spine BMD, as well as fracture risk, in human populations for one significant phosSNP, that is, rs227584 (major/minor allele: C/A, EAS population) located in C17orf53 gene, were suggested in prior meta-analyses. Specifically, carriers of allele C had significant higher BMD and lower risk of low-trauma fractures than carriers of A. We pursued to test the molecular and cellular functions of rs227584 in bone through osteoblastic cell culture and multiple assays. We identified five phosSNPs significant for OP (P < 0.01). The osteoblastic cells, which was transfected with wild-type C17orf53 (allele C at rs227584, P126), demonstrated specific interaction with NEK2 kinase, increased expression levels of osteoblastic genes significantly (OPN, OCN, COL1A1, P < 0.05), and promoted osteoblast growth and ALP activity, in contrast to those transfected with mutant C17orf53 (allele A at rs227584, T126). In the light of the consistent evidences between the present functional study in human bone cells and the prior association studies in human populations, we conclude that the SNP rs227584, via altering protein-kinase interaction, regulates osteoblastic gene expression, influences osteoblast growth and activity, hence to affect BMD and fracture risk in humans.
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Densidad Ósea/genética , Proteínas de Unión al ADN/genética , Fracturas Óseas/genética , Osteoblastos/metabolismo , Osteoporosis/genética , Polimorfismo de Nucleótido Simple , Procesamiento Proteico-Postraduccional , Fosfatasa Alcalina/genética , Fosfatasa Alcalina/metabolismo , Alelos , Línea Celular , Colágeno Tipo I/genética , Colágeno Tipo I/metabolismo , Cadena alfa 1 del Colágeno Tipo I , Biología Computacional/métodos , Proteínas de Unión al ADN/metabolismo , Fracturas Óseas/diagnóstico , Fracturas Óseas/metabolismo , Fracturas Óseas/patología , Regulación de la Expresión Génica , Frecuencia de los Genes , Estudio de Asociación del Genoma Completo , Cadera/patología , Humanos , Quinasas Relacionadas con NIMA/genética , Quinasas Relacionadas con NIMA/metabolismo , Osteoblastos/patología , Osteocalcina/genética , Osteocalcina/metabolismo , Osteopontina/genética , Osteopontina/metabolismo , Osteoporosis/diagnóstico , Osteoporosis/metabolismo , Osteoporosis/patología , Fosforilación , Riesgo , Columna Vertebral/metabolismo , Columna Vertebral/patologíaRESUMEN
Ion transport through nanopores is a process of fundamental significance in nature and in engineering practice. Over the past decade, it has been found that the ion conductivity in nanopores could be drastically enhanced, and different mechanisms have been proposed to explain this observation. To date, most reported studies have been carried out with relatively dilute electrolytes, while ion transport in nanopores under high electrolyte concentrations (>1 M) has been rarely explored. Through systematic experimental and atomistic simulation studies with NaCl solutions, here we show that at high electrolyte concentrations, ion mobility in small nanopores could be significantly reduced from the corresponding bulk value. Subsequent molecular dynamics studies indicate that in addition to the low mobility of surface-bound ions in the Stern layer, enhanced pairing and collisions between partially dehydrated ions of opposite charges also make important contributions to the reduced ion mobility. Furthermore, we show that the extent of mobility reduction depends on the association constant between cations and anions in different electrolytes with a more drastic reduction for a larger association constant.
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Cloruros/química , Difusión , Nanoporos , Sodio/química , Simulación de Dinámica Molecular , Cloruro de Sodio/químicaRESUMEN
Single nanopores have attracted much scientific interest because of their versatile applications. The majority of experiments have been performed with nanopores being in contact with the same electrolyte on both sides of the membrane, although solution gradients across semipermeable membranes are omnipresent in natural systems. In this manuscript, we studied ionic and fluidic movement through thin nanopores under viscosity gradients both experimentally and using simulations. Ionic-current rectification was observed under these conditions because solutions with different conductivities filled across the pore under different biases caused by electroosmotic flow. We found that a pore filled with high-viscosity solutions exhibited a current increase with applied voltage in a steeper slope beyond a threshold voltage, which abnormally reduced the current-rectification ratio. Through simulations, we found that reversed electroosmotic flow, which filled the pore with aqueous solutions of lower viscosities, was responsible for this behavior. The reversed electroosmotic flow could be explained by slower depletion of co-ions than of counterions along the pore. By increasing the surface charge density of pore surfaces, current-rectification ratio could reach the value of the viscosity gradient across thin nanopores. Our findings shed light on fundamental aspects to be considered when performing experiments with viscosity gradients across nanopores and nanofluidic channels.
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Electroósmosis , Nanoporos , Conductividad Eléctrica , Electrólitos , Iones/química , ViscosidadRESUMEN
OBJECTIVES: To identify novel DNA methylation sites significant for rheumatoid arthritis (RA) and comprehensively understand their underlying pathological mechanism. METHODS: We performed (1) genome-wide DNA methylation and mRNA expression profiling in peripheral blood mononuclear cells from RA patients and health controls; (2) correlation analysis and causal inference tests for DNA methylation and mRNA expression data; (3) differential methylation genes regulatory network construction; (4) validation tests of 10 differential methylation positions (DMPs) of interest and corresponding gene expressions; (5) correlation between PARP9 methylation and its mRNA expression level in Jurkat cells and T cells from patients with RA; (6) testing the pathological functions of PARP9 in Jurkat cells. RESULTS: A total of 1046 DNA methylation positions were associated with RA. The identified DMPs have regulatory effects on mRNA expressions. Causal inference tests identified six DNA methylation-mRNA-RA regulatory chains (eg, cg00959259-PARP9-RA). The identified DMPs and genes formed an interferon-inducible gene interaction network (eg, MX1, IFI44L, DTX3L and PARP9). Key DMPs and corresponding genes were validated their differences in additional samples. Methylation of PARP9 was correlated with mRNA level in Jurkat cells and T lymphocytes isolated from patients with RA. The PARP9 gene exerted significant effects on Jurkat cells (eg, cell cycle, cell proliferation, cell activation and expression of inflammatory factor IL-2). CONCLUSIONS: This multistage study identified an interferon-inducible gene interaction network associated with RA and highlighted the importance of PARP9 gene in RA pathogenesis. The results enhanced our understanding of the important role of DNA methylation in pathology of RA.
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Artritis Reumatoide/genética , Metilación de ADN/genética , Leucocitos Mononucleares/metabolismo , ARN Mensajero/metabolismo , Artritis Reumatoide/sangre , Estudios de Casos y Controles , Femenino , Perfilación de la Expresión Génica , Redes Reguladoras de Genes/genética , Humanos , Células Jurkat/metabolismo , Masculino , Persona de Mediana Edad , Proteínas de Neoplasias/metabolismo , Poli(ADP-Ribosa) Polimerasas/metabolismo , Linfocitos T/metabolismoRESUMEN
The poor stability of CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) has severely impeded their practical applications. Although there are some successful examples on encapsulating multiple CsPbX3 NCs into an oxide or polymer matrix, it has remained a serious challenge for the surface modification/encapsulation using oxides or polymers at a single particle level. In this work, monodisperse CsPbX3/SiO2 and CsPbBr3/Ta2O5 Janus nanoparticles were successfully prepared by combining a water-triggered transformation process and a sol-gel method. The CsPbBr3/SiO2 NCs exhibited a photoluminescence quantum yield of 80% and a lifetime of 19.8 ns. The product showed dramatically improved stability against destruction by air, water, and light irradiation. Upon continuous irradiation by intense UV light for 10 h, a film of the CsPbBr3/SiO2 Janus NCs showed only a slight drop (2%) in the PL intensity, while a control sample of unmodified CsPbBr3 NCs displayed a 35% drop. We further highlighted the advantageous features of the CsPbBr3/SiO2 NCs in practical applications by using them as the green light source for the fabrication of a prototype white light emitting diode, and demonstrated a wide color gamut covering up to 138% of the National Television System Committee standard. This work not only provides a novel approach for the surface modification of individual CsPbX3 NCs but also helps to address the challenging stability issue; therefore, it has an important implication toward their practical applications.
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MicroRNAs (miRNAs) can regulate gene expression through binding to complementary sites in the 3'-untranslated regions of target mRNAs, which will lead to existence of correlation in expression between miRNA and mRNA. However, the miRNA-mRNA correlation patterns are complex and remain largely unclear yet. To establish the global correlation patterns in human peripheral blood mononuclear cells (PBMCs), multiple miRNA-mRNA correlation analyses and expression quantitative trait locus (eQTL) analysis were conducted in this study. We predicted and achieved 861 miRNA-mRNA pairs (65 miRNAs, 412 mRNAs) using multiple bioinformatics programs, and found global negative miRNA-mRNA correlations in PBMC from all 46 study subjects. Among the 861 pairs of correlations, 19.5% were significant (P < 0.05) and ~70% were negative. The correlation network was complex and highlighted key miRNAs/genes in PBMC. Some miRNAs, such as hsa-miR-29a, hsa-miR-148a, regulate a cluster of target genes. Some genes, e.g., TNRC6A, are regulated by multiple miRNAs. The identified genes tend to be enriched in molecular functions of DNA and RNA binding, and biological processes such as protein transport, regulation of translation and chromatin modification. The results provided a global view of the miRNA-mRNA expression correlation profile in human PBMCs, which would facilitate in-depth investigation of biological functions of key miRNAs/mRNAs and better understanding of the pathogenesis underlying PBMC-related diseases.
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Regulación de la Expresión Génica/genética , Redes Reguladoras de Genes/genética , MicroARNs/genética , Autoantígenos/genética , Ensamble y Desensamble de Cromatina/genética , Biología Computacional , Humanos , Leucocitos Mononucleares/metabolismo , Leucocitos Mononucleares/patología , Sitios de Carácter Cuantitativo/genética , ARN Mensajero/genética , Proteínas de Unión al ARN/genéticaRESUMEN
The resistive-pulse technique provides a fast and label-free method for nanoparticle detection. To achieve higher sensitivity, thin nanopores such as silicon nitride nanopores are usually considered. In this study, nanoparticle detection has been mimicked with simulations. We found that the surface charges of particles can significantly affect current blockade in short pores, particularly under high electric fields. For particles with surface charge densities higher than -0.02 C m-2, current blockade ratios depend closely on the applied voltage. From our simulation results, an optimal voltage can be found for particle detection, at which the current blockade ratio does not depend on the surface charge density of the particle. This optimal voltage was obtained from the balance of current increase and decrease caused by cations and anions, respectively, due to negative surface charges of the particles. From this systematic study, the optimal voltage was found to represent a property of the system that only depends on the electrolyte type. We think our findings can provide some help for accurate particle detection in experiments.
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Extensive molecular dynamics simulations are employed to optimize nanopore size and surface charge density in order to obtain high ionic selectivity and high water throughput for seawater desalination systems. It is demonstrated that with the help of surface charge exclusion, nanopores with diameter as large as 3.5 nm still have high ionic selectivity. The mechanism of the salt rejection in a surface-charged nanopore is mainly attributed to the ion concentration difference between the cations and anions induced by the surface charges. Increasing surface charge density is beneficial to enhance ionic selectivity. However, there exists a critical value for the surface charge density. Once the surface charge density exceeds the critical value, charge inversion occurs inside a nanopore. Further increasing the surface charge density will deteriorate the ionic selectivity because the highly charged nanopore surface will allow more coions to enter the nanopore in order to keep the whole system in charge neutrality. Besides the surface charge density, the nanopore length also affects the ionic selectivity. Based on our systematic simulations, nanopores with surface charge density between -0.09 C/m2 and -0.12 C/m2, diameters smaller than 3.5 nm, and membrane thickness ranging between 8 and 10 graphene layers show an excellent performance for the ionic selectivity.
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Long non-coding RNAs (lncRNAs) serve as important controller of cellular functions via regulating RNA transcription, degradation and translation. However, what are the regulation patterns of lncRNAs on downstream mRNA and how the upstream genetic variants regulate lncRNAs are largely unknown. We first performed a comprehensive expression quantitative trait locus (eQTL) analysis (MatrixeQTL package, R) using genome-wide lncRNA expression and SNP genotype data from human peripheral blood mononuclear cells (PBMCs) of 43 unrelated individuals. Subsequently, multi-omics integrative network analysis was applied to construct SNP-lncRNA-mRNA (SLM) interaction networks. The causal inference test (CIT) was used to identify lncRNA-mediated (epi-) genetic regulation on mRNA expressions. Our eQTL analysis detected 707 pairs of cis-effect associations (p < 5.64E-06) and 6657 trans-effect associations (p < 3.51E-08), respectively. We also found that top significant cis-eSNPs were enriched around the lncRNA transcription start site regions, and that enrichment patterns of cis-eSNPs differs among different lncRNA sizes (small, medium and large).The constructed SLM interaction networks (1 primary networks and four small separate networks) showed various complex interaction patterns. Especially, the in-depth CIT detected 50 significant lncRNA-mediated SLM trios, and some hotspots (e.g., SNPs: rs926370, rs7716167 and rs16880521; lncRNAs: HIT000061975 and ENST00000579057.1). This study represents the first effort of dissecting the SLM interaction patterns in PBMCs by multi-omics integrative network analysis and causal inference test for clearing the regulation chain. The results provide novel insights into the regulation patterns of lncRNA, and may facilitate investigations of PBMC-related immune physiological process and immunological diseases in the future.
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Monocitos/metabolismo , Polimorfismo de Nucleótido Simple , ARN Largo no Codificante/genética , ARN Mensajero/genética , Transcriptoma , Femenino , Humanos , Sitios de Carácter CuantitativoRESUMEN
Conically shaped pores such as glass pipets as well as asymmetric pores in polymers became an important analytics tool used for the detection of molecules, viruses, and particles. Electrokinetic or pressure driven passage of single particles through a single pore causes a transient change of the transmembrane current, called a resistive-pulse, whose amplitude is the measure of the particle volume. The shape of the pulse reflects the pore topography, and in a conical pore, resistive pulses have a shape of a tick point. Passage of particles in both directions was reported to produce pulses of the same amplitude and shapes that are mirror images of each other. In this manuscript we identify conditions at which the amplitude of resistive-pulses in a conical mesopore is direction dependent. Neutral particles entering the pore from the larger entrance of a conical pore, called the base, block the current to a larger extent than the particles traveling in the opposite direction. Negatively charged particles on the other hand size larger when being transported in the direction from tip to base. The findings are explained via voltage-regulated ionic concentrations in the pore such that for one voltage polarity a weak depletion zone is formed, which increases the current blockage caused by a particle. For the opposite polarity, an enhancement of ionic concentrations was predicted. The findings reported here are of crucial importance for the resistive-pulse technique, which relates the current blockage with the size of the passing object.
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Through molecular dynamics simulations considering thermal vibration of surface atoms, ionic behaviors in concentrated NaCl solutions confined between discretely charged silicon surfaces have been investigated. The electric double layer structure was found to be sensitive to the density and distribution of surface charges. Due to the discreteness of the surface charge, a slight charge inversion appeared which depended on the surface charge density, bulk concentration, and confinement. In the nanoconfined NaCl solutions concentrated from 0.2 to 4.0 M, the locations of accumulation layers for Na(+) and Cl(-) ions remained stable, but their peak values increased. The higher the concentration was, the more obvious the charge inversion appeared. In 4.0 M NaCl solution, Na(+) and Cl(-) ions show obvious alternating layered distributions which may correspond to the solidification found in experiments. By changing surface separation, the confinement had a large effect on the ionic distribution. As both surfaces approached each other, many ions and water molecules were squeezed out of the confined space. Two adjacent layers in ion or water distribution profiles can be forced closer to each other and merge together. From ionic hydration analysis, the coordination number of Na(+) ions in highly confined space was much lower than that in the bulk.