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1.
Artigo em Inglês | MEDLINE | ID: mdl-31794181

RESUMO

Precise spatiotemporal control of surface bubble movement can benefit a wide range of applications like high-throughput drug screening, combinatorial material development, microfluidic logic, colloidal and molecular assembly, and so forth. In this work, we demonstrate that surface bubbles on a solid surface are directed by a laser to move at high speeds (>1.8 mm/s), and we elucidate the mechanism to be the depinning of the three-phase contact line (TPCL) by rapid plasmonic heating of nanoparticles (NPs) deposited in situ during bubble movement. On the basis of our observations, we deduce a stick-slip mechanism based on asymmetric fore-aft plasmonic heating: local evaporation at the front TPCL due to plasmonic heating depins and extends the front TPCL, followed by the advancement of the trailing TPCL to resume a spherical bubble shape to minimize surface energy. The continuous TPCL drying during bubble movement also enables well-defined contact line deposition of NP clusters along the moving path. Our finding is beneficial to various microfluidics and pattern writing applications.

2.
Reprod Biol Endocrinol ; 17(1): 112, 2019 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-31881887

RESUMO

BACKGROUND: Gestational diabetes mellitus (GDM) has a high prevalence in the period of pregnancy. However, the lack of gold standards in current screening and diagnostic methods posed the biggest limitation. Regulation of gene expression caused by DNA methylation plays an important role in metabolic diseases. In this study, we aimed to screen GDM diagnostic markers, and establish a diagnostic model for predicting GDM. METHODS: First, we acquired data of DNA methylation and gene expression in GDM samples (N = 41) and normal samples (N = 41) from the Gene Expression Omnibus (GEO) database. After pre-processing the data, linear models were used to identify differentially expressed genes (DEGs). Then we performed pathway enrichment analysis to extract relationships among genes from pathways, construct pathway networks, and further analyzed the relationship between gene expression and methylation of promoter regions. We screened for genes which are significantly negatively correlated with methylation and established mRNA-mRNA-CpGs network. The network topology was further analyzed to screen hub genes which were recognized as robust GDM biomarkers. Finally, the samples were randomly divided into training set (N = 28) and internal verification set (N = 27), and the support vector machine (SVM) ten-fold cross-validation method was used to establish a diagnostic classifier, which verified on internal and external data sets. RESULTS: In this study, we identified 465 significant DEGs. Functional enrichment analysis revealed that these genes were associated with Type I diabetes mellitus and immunization. And we constructed an interactional network including 1091 genes by using the regulatory relationships of all 30 enriched pathways. 184 epigenetics regulated genes were screened by analyzing the relationship between gene expression and promoter regions' methylation in the network. Moreover, the accuracy rate in the training data set was increased up to 96.3, and 82.1% in the internal validation set, and 97.3% in external validation data sets after establishing diagnostic classifiers which were performed by analyzing the gene expression profiles of obtained 10 hub genes from this network, combined with SVM. CONCLUSIONS: This study provided new features for the diagnosis of GDM and may contribute to the diagnosis and personalized treatment of GDM.

3.
Sci Adv ; 5(12): eaax3777, 2019 12.
Artigo em Inglês | MEDLINE | ID: mdl-31853496

RESUMO

In comparison with the advancement of switchable, nonlinear, and active components in electronics, solid-state thermal components for actively controlling heat flow have been extremely rare. We demonstrate a high-contrast and reversible polymer thermal regulator based on the structural phase transition in crystalline polyethylene nanofibers. This structural phase transition represents a dramatic change in morphology from a highly ordered all-trans conformation to a combined trans and gauche conformation with rotational disorder, leading to an abrupt change in phonon transport along the molecular chains. For five nanofiber samples measured here, we observe an average thermal switching ratio of ~8× and maximum switching ratio of ~10×, which occurs in a narrow temperature range of 10 K across the structural phase transition. To the best of our knowledge, the ~10× switching ratio exceeds any reported experimental values for solid-solid and solid-liquid phase transitions of materials. There is no thermal hysteresis observed upon heating/cooling cycles.

4.
Nucleic Acids Res ; 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31642496

RESUMO

De novo mutations (DNMs) significantly contribute to sporadic diseases, particularly in neuropsychiatric disorders. Whole-exome sequencing (WES) and whole-genome sequencing (WGS) provide effective methods for detecting DNMs and prioritizing candidate genes. However, it remains a challenge for scientists, clinicians, and biologists to conveniently access and analyse data regarding DNMs and candidate genes from scattered publications. To fill the unmet need, we integrated 580 799 DNMs, including 30 060 coding DNMs detected by WES/WGS from 23 951 individuals across 24 phenotypes and prioritized a list of candidate genes with different degrees of statistical evidence, including 346 genes with false discovery rates <0.05. We then developed a database called Gene4Denovo (http://www.genemed.tech/gene4denovo/), which allowed these genetic data to be conveniently catalogued, searched, browsed, and analysed. In addition, Gene4Denovo integrated data from >60 genomic sources to provide comprehensive variant-level and gene-level annotation and information regarding the DNMs and candidate genes. Furthermore, Gene4Denovo provides end-users with limited bioinformatics skills to analyse their own genetic data, perform comprehensive annotation, and prioritize candidate genes using custom parameters. In conclusion, Gene4Denovo conveniently allows for the accelerated interpretation of DNM pathogenicity and the clinical implication of DNMs in humans.

5.
ACS Nano ; 13(11): 13027-13036, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31660731

RESUMO

Oil spills remain a worldwide challenge and need emergency "spill-SOS" actions when they occur. Conventional methods suffer from complex processes and high cost. Here, we demonstrate a solar-heating siphon-capillary oil skimmer (S-SOS) that harvests solar energy, gravitational potential energy, and solid surface energy to enable efficient oil spill recovery in a self-pumping manner. The S-SOS is assembled by an inverted U-shape porous architecture combining solar-heating, siphon, and capillary effects, and works without any external power or manual interventions. Importantly, solid surface energy is used by capillary adsorption to enable the self-starting behavior, gravitational potential energy is utilized by siphon transport to drive the oil flow, and solar energy is harvested by solar-thermal conversion to facilitate the transport speed. In the proof-of-concept work, an all-carbon hierarchical architecture (VG/GF) is fabricated by growing vertically oriented graphene nanosheets (VGs) on a monolith of graphite felt (GF) via a plasma-enhanced method to serve as the U-shape architecture. Consequently, an oil-recovery rate of 35.2 L m-2 h-1 is obtained at ambient condition. When exposed to normal solar irradiation, the oil-recovery rate dramatically increases to 123.3 L m-2 h-1. Meanwhile, the solar-thermal energy efficiency is calculated to be 75.3%. Moreover, the S-SOS system presents excellent stability without obvious performance-degradation over 60 h. The outstanding performance is ascribed to the enhanced siphon action, capillary action, photonic absorption, and interfacial heating in the plasma-made graphene nanostructures. Multiple merits make the current S-SOS design and the VG/GF nanostructures promising for efficient oil recovery and transport of energy stored in chemical bonds.

6.
ACS Appl Mater Interfaces ; 11(35): 32481-32488, 2019 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-31408315

RESUMO

Water slip at solid surfaces is important for a wide range of micro-/nanofluidic applications. While it is known that water slip behavior depends on surface functionalization, how it impacts the molecular level dynamics and mass transport at the interface is still not thoroughly understood. In this paper, we use nonequilibrium molecular dynamics simulations to investigate the slip behavior of water confined between gold surfaces functionalized by self-assembled monolayer (SAM) molecules with different polar functional groups. We observe a positive-to-negative slip transition from hydrophobic to hydrophilic SAM functionalizations, which is found to be related to the stronger interfacial interaction between water molecules and more hydrophilic SAM molecules. The stronger interaction increases the surface friction and local viscosity, making water slip more difficult. More hydrophilic functionalization also slows down the interfacial water relaxation and leads to more pronounced water trapping inside the SAM layer, both of which impede water slip. The results from this work will provide useful insights into the understanding of the water slip at functionalized surfaces and design guidelines for various applications.

7.
Phys Chem Chem Phys ; 21(31): 17029-17035, 2019 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-31353367

RESUMO

Thermal transport across solid interfaces is of great importance for applications like power electronics. In this work, we perform non-equilibrium molecular dynamics simulations to study the effect of light atoms on the thermal transport across SiC/GaN interfaces, where light atoms refer to substitutional or interstitial defect atoms lighter than those in the pristine lattice. Various light atom doping features, such as the light atom concentration, mass of the light atom, and skin depth of the doped region, have been investigated. It is found that substituting Ga atoms in the GaN lattice with lighter atoms (e.g. boron atoms) with 50% concentration near the interface can increase the thermal boundary conductance (TBC) by up to 50%. If light atoms are introduced interstitially, a similar increase in TBC is observed. Spectral analysis of interfacial heat transfer reveals that the enhanced TBC can be attributed to the stronger coupling of mid- and high-frequency phonons after introducing light atoms. We have also further included quantum correction, which reduces the amount of enhancement, but it still exists. These results may provide a route to improve TBC across solid interfaces as light atoms can be introduced during material growth.

8.
Phys Chem Chem Phys ; 21(28): 15523-15530, 2019 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-31263807

RESUMO

The physics of thermal transport in polymers is important in many applications, such as in heat exchangers and electronics packaging. Even though thermal conductivity models for amorphous polymers have been reported since the 1970s, none of the published models included the chain conformation and chain stiffness effects. In this study, we use molecular dynamics (MD) simulations to study the chain length effect on thermal conductivity of amorphous polyethylene (PE), and the number of repeating C2H4 units ranges from 5 to 200. The total thermal conductivity is decomposed into its contributions from energy convection (k-convection), and heat transfer through nonbonding (k-nonbonding) and bonding (k-bonding) interactions. Each part of the contributions is fitted empirically by using a scaling relationship: k-convection (Einstein's diffusion coefficient model), k-nonbonding ∝ n (Choy's model) and k-bonding (from this study), where Rg is the radius of gyration, n is the number density, and ξ is the persistence length. Summarizing these three components, we emphasize the chain conformation (Rg) and chain stiffness (ξ) effects on thermal conductivity, and we propose a structure-property relation model for amorphous polymers. Our empirical model is compared with Hansen's experimental data [D. Hansen, R. Kantayya and C. Ho, Polym. Eng. Sci., 1966, 6, 260-262] and with our MD results. Our empirical model relies on realistic structural properties to enable accurate predictions. We believe that our model has captured some key structure-property relations in amorphous polymers.

9.
J Chem Inf Model ; 59(7): 3110-3119, 2019 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-31268306

RESUMO

Machine learning techniques are being applied in quantifying structure-property relationships for a wide variety of materials, where the properly represented materials play key roles. Although algorithms for representation learning are extensively studied, their applications to domain-specific areas, such as polymers, are limited largely due to the lack of benchmark databases. In this work, we investigate different types of polymer representations, including Morgan fingerprint (MF), molecular embedding (ME), and molecular graph (MG), based on the benchmark database from a subset of the well-known web-based polymer databases, PolyInfo. We evaluate the quality of different polymer representations via quantifying the relationships between the representations and polymer properties, including density, melting temperature, and glass transition temperature. Different representation learning schemes for MEs, such as supervised learning, semisupervised learning, and transfer learning, are investigated. In supervised learning, only labeled molecules in our benchmark database are used for representation learning, in semisupervised learning, both labeled and unlabeled molecules in our benchmark database are used, and in transfer learning, molecules from an external database that is different from the benchmark database are used for representation learning. It is found that ME (with the R2 of 0.724 in the density case, 0.684 in the melting temperature case, and 0.865 in the glass transition temperature case) outperforms the other representations for structure-property relationship quantification in all cases studied, and MG (with the R2 of 0.260 in the density case, -0.149 in the melting temperature case, and 0.711 in the glass transition case) is shown to be much inferior to ME and MF (with the R2 of 0.562 in the density case, 0.645 in the melting temperature case, and 0.849 in the glass transition case), likely due to the relatively small volumes of training data available. For MEs, it is found that the similarities of substructure MEs under different learning schemes (e.g., SL, SSL, and TL) are differently estimated, thus leading to different performance scores in structure-property relation quantification. Combinations of MEs show little effect on predictive performance when comparing to the single MEs in the corresponding regression tasks, proving no information gain in mixing MEs.

11.
ACS Nano ; 13(2): 1097-1106, 2019 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-30633498

RESUMO

Polymers with superior mechanical properties are desirable in many applications. In this work, polyethylene (PE) films reinforced with exfoliated thermally reduced graphene oxide (TrGO) fabricated using a roll-to-roll hot-drawing process are shown to have outstanding mechanical properties. The specific ultimate tensile strength and Young's modulus of PE/TrGO films increased monotonically with the drawing ratio and TrGO filler fraction, reaching up to 3.2 ± 0.5 and 109.3 ± 12.7 GPa, respectively, with a drawing ratio of 60× and a very low TrGO weight fraction of 1%. These values represent by far the highest reported to date for a polymer/graphene composite. Experimental characterizations indicate that as the polymer films are drawn, TrGO fillers are exfoliated, which is further confirmed by molecular dynamics (MD) simulations. Exfoliation increases the specific area of the TrGO fillers in contact with the PE matrix molecules. Molecular dynamics simulations show that the PE-TrGO interaction is stronger than the PE-PE intermolecular van der Waals interaction, which enhances load transfer from PE to TrGO and leverages the ultrahigh mechanical properties of TrGO.

12.
Nano Lett ; 18(12): 7469-7477, 2018 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-30412411

RESUMO

We present experimental measurements of the thermal boundary conductance (TBC) from 78-500 K across isolated heteroepitaxially grown ZnO films on GaN substrates. This data provides an assessment of the underlying assumptions driving phonon gas-based models, such as the diffuse mismatch model (DMM), and atomistic Green's function (AGF) formalisms used to predict TBC. Our measurements, when compared to previous experimental data, suggest that TBC can be influenced by long wavelength, zone center modes in a material on one side of the interface as opposed to the '"vibrational mismatch"' concept assumed in the DMM; this disagreement is pronounced at high temperatures. At room temperature, we measure the ZnO/GaN TBC as 490[+150,-110] MW m-2 K-1. The disagreement among the DMM and AGF, and the experimental data at elevated temperatures, suggests a non-negligible contribution from other types of modes that are not accounted for in the fundamental assumptions of these harmonic based formalisms, which may rely on anharmonicity. Given the high quality of these ZnO/GaN interfaces, these results provide an invaluable, critical, and quantitative assessment of the accuracy of assumptions in the current state of the art computational approaches used to predict phonon TBC across interfaces.

13.
ACS Appl Mater Interfaces ; 10(40): 34690-34698, 2018 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-30209944

RESUMO

Enhancing thermal energy transport across solid interfaces is of critical importance to a wide variety of applications ranging from energy systems and lighting devices to electronics. Nanoscale surface roughness is usually considered detrimental to interfacial thermal transport because of its role in phonon scattering. In this study, however, we demonstrate significant thermal conductance enhancements across metal-semiconductor interfaces by as much as 90% higher than that of the planar interfaces using engineered nanostructures fabricated by Au nanoparticle (NP)-assisted lithography, where self-assembled Au NPs are used as an efficient etching mask to pattern solid substrates over large surface areas. The enlarged interfacial contact area due to the presence of nanostructures is the main reason for the significantly enhanced thermal transport. It is further demonstrated that the conductance can be systematically tuned over a wide range through the use of the Au NP self-assembly process that is regulated by a sacrificial Sb layer whose thickness determines the size and density of the nanostructures produced. This strategy is tested on two technologically important semiconductors, Si and GaN, and their interfacial thermal conductance with Al being measured using the time-domain thermoreflectance technique. Moreover, the nanostructured interfaces can maintain the enhanced conductance for a temperature range of 30-110 °C-the operating temperatures commonly experienced by energy, lighting, and electronic devices. Our results could provide a wafer-scale and low-cost strategy for improving the thermal management of these devices.

14.
Phys Chem Chem Phys ; 20(31): 20534-20539, 2018 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-30046783

RESUMO

Block copolymers have a wide range of applications, such as battery electrolytes and nanoscale pattern generation. The thermal conductivity is a critical parameter in many of these applications (e.g., batteries), which is strongly related to the molecular conformation. In this work, the thermal transport in a representative diblock copolymer, polyethylene (PE)-polypropylene (PP), at different PE to PP block ratios is studied using molecular dynamics (MD) simulations. Our results show that the thermal conductivity of the PE-PP diblock copolymer can be tuned continuously by the block ratio, and it is strongly related to the molecular conformation, characterized by the radius of gyration (Rg). It is found that increasing the PP portion results in an overall decreasing trend in the thermal conductivity since the PP block has a more flexible backbone, which leads to a smaller spatial extension of the whole PE-PP copolymer molecule. Thermal conductivity decomposition shows that the bonding contribution is dominant in both the PE and PP portions of the block copolymer. The findings from this study can help understand thermal transport in general block copolymers.

15.
ACS Appl Mater Interfaces ; 10(33): 28159-28165, 2018 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-30056700

RESUMO

Thermal transport across solid-water interfaces is critical for a wide range of applications such as solar thermal evaporation, nanoparticle-assisted hyperthermia therapeutics, and nanofluids. Surface functionalization using self-assembled monolayers (SAMs) to change the hydrophilicity of the solid surface is a common strategy to improve the thermal conductance of solid-water interfaces. Although it is known that hydrophilic interfaces increase the interfacial bonding, how it impacts the molecular level energy transport across the interface is still not clear. In this paper, we perform molecular dynamics simulations to calculate the thermal conductance of differently functionalized gold (Au)-water interfaces. Combining the heat flux decomposition to different interatomic interactions across interfaces and analyses of water structures close to the functionalized surfaces, we found that there is a collaborative effect from the electrostatic interactions and the Lennard-Jones (L-J) interactions (especially the repulsive part). The electrostatic interactions, which are between the polar functional groups of SAMs and water, will attract water molecules closer to the SAM surface, leading both the electrostatic and L-J interactions to have larger effective forces across the interfaces. This increases the power exchanged between solid and water atoms, enhancing the thermal energy transport. The results from this work will provide new insights to the understanding of thermal transport across solid-water interfaces.

16.
Phys Rev E ; 97(3-1): 033106, 2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29776103

RESUMO

We investigate the nature of vapor bubble formation near a nanoscale-curved convex liquid-solid interface using two models: an equilibrium Gibbs model for homogenous nucleation, and a nonequilibrium dynamic van der Waals-diffuse-interface model for phase change in an initially cool liquid. Vapor bubble formation is shown to occur for sufficiently large radius of curvature and is suppressed for smaller radii. Solid-fluid interactions are accounted for and it is shown that liquid-vapor interfacial energy, and hence Laplace pressure, has limited influence over bubble formation. The dominant factor is the energetic cost of creating the solid-vapor interface from the existing solid-liquid interface, as demonstrated via both equilibrium and nonequilibrium arguments.

17.
Nat Commun ; 9(1): 1664, 2018 04 25.
Artigo em Inglês | MEDLINE | ID: mdl-29695754

RESUMO

Polymers are widely used in daily life, but exhibit low strength and low thermal conductivity as compared to most structural materials. In this work, we develop crystalline polymer nanofibers that exhibit a superb combination of ultra-high strength (11 GPa) and thermal conductivity, exceeding any existing soft materials. Specifically, we demonstrate unique low-dimensionality phonon physics for thermal transport in the nanofibers by measuring their thermal conductivity in a broad temperature range from 20 to 320 K, where the thermal conductivity increases with increasing temperature following an unusual ~T1 trend below 100 K and eventually peaks around 130-150 K reaching a metal-like value of 90 W m-1 K-1, and then decays as 1/T. The polymer nanofibers are purely electrically insulating and bio-compatible. Combined with their remarkable lightweight-thermal-mechanical concurrent functionality, unique applications in electronics and biology emerge.

18.
ACS Omega ; 3(10): 12530-12534, 2018 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-31457986

RESUMO

Understanding the role of fillers in the thermal transport of composite materials is of great importance to engineering better materials. The filler induces material interfaces within the composite, which influence the thermal transport between the matrix and themselves. The filler can also alter the molecular arrangement of the matrix in its vicinity, which may also impact the thermal transport ability. In this paper, molecular dynamics simulations are performed to study the thermal transport across the matrix-filler interfaces in hexagonal boron nitride (h-BN)-organic molecule composites. Four different organic molecules are studied as the matrixes. They include hexane (C6H14), hexanamine (C6H13NH2), hexanol (C6H13OH), and hexanoic acid (C5H11COOH), which feature the same molecular backbone but increasingly different polar functional groups. The nominal local thermal conductivities of the hexane matrix with varying distances to the interface are calculated to demonstrate the influence of the filler on the thermal transport properties of the matrix. It is found that a more polar matrix exhibits a higher density in the near-interface region and a higher nominal local thermal conductivity, suggesting that the interfacial interaction can impact the local heat transfer ability of the matrix. In addition, the more polar matrix also leads to a larger interfacial thermal conductance with h-BN (hexane: 90.47 ± 14.49 MW/m2 K, hexanamine: 113.38 ± 17.72 MW/m2 K, hexanol: 136.16 ± 25.12 MW/m2 K, and hexanoic acid: 155.17 ± 24.89 MW/m2 K) because of the higher matrix density near the interface and thus more atoms exchanging energy with the filler. The results of this study may provide useful information for designing composite materials for heat transfer applications.

19.
Phys Chem Chem Phys ; 19(44): 29855-29861, 2017 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-29104997

RESUMO

In this work, the droplet size in a water-in-oil emulsion obtained by supersaturation is studied. The emulsion is obtained by cooling down a saturated water/oil solution by a certain temperature difference. The effects of the cooling rate and temperature difference on the produced droplet size are experimentally investigated. The average size of water droplets in the emulsion is found to be proportional to the square root of the cooling rate. By analyzing the time scales of three different steps, including nucleation, droplet growth due to diffusion and coarsening, involved in the emulsification process, it is found that the time scales of nucleation and droplet growth due to mass diffusion are much smaller than the cooling time constant, which is much shorter than the coarsening time scale. A mechanism that links the cooling rate and supersaturation temperature to droplet size is proposed: the cooling rate influences the nucleation and thus droplet density, while the temperature difference, which is linearly proportional to the total volume of precipitated water from the saturated water-in-oil solution, determines the size of each droplet. The droplet size data were found to support this proposed mechanism well. The results obtained from this work may provide useful guidance on controlling the droplet size in the supersaturation-based emulsification process, which has a lot of practical relevance to many applications.

20.
ACS Appl Mater Interfaces ; 9(39): 33740-33748, 2017 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-28885818

RESUMO

Thermal transport across hard-soft interfaces is critical to many modern applications, such as composite materials, thermal management in microelectronics, solar-thermal phase transition, and nanoparticle-assisted hyperthermia therapeutics. In this study, we use equilibrium molecular dynamics (EMD) simulations combined with the Green-Kubo method to study how molecularly heterogeneous structures of the self-assembled monolayer (SAM) affect the thermal transport across the interfaces between the SAM-functionalized gold and organic liquids (hexylamine, propylamine and hexane). We focus on a practically synthesizable heterogeneous SAM featuring alternating short and long molecular chains. Such a structure is found to improve the thermal conductance across the hard-soft interface by 46-68% compared to a homogeneous nonpolar SAM. Through a series of further simulations and analyses, it is found that the root reason for this enhancement is the penetration of the liquid molecules into the spaces between the long SAM molecule chains, which increase the effective contact area. Such an effect is similar to the fins used in macroscopic heat exchanger. This "molecular fin" structure from the heterogeneous SAM studied in this work provides a new general route for enhancing thermal transport across hard-soft material interfaces.

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