Ionic thermoelectric (i-TE) liquid cells offer an environmentally friendly, cost effective, and easy-operation route to low-grade heat recovery. However, the lowest temperature is limited by the freezing temperature of the aqueous electrolyte. Applying a eutectic solvent strategy, we fabricate a high-performance cryo-temperature i-TE liquid cell. Formamide is used as a chaotic organic solvent that destroys the hydrogen bond network between water molecules, forming a deep eutectic solvent that enables the cell to operate near cryo temperatures (down to -35 °C). After synergistic optimization of the electrode and cell structure, the as-fabricated liquid i-TE cell with cold (-35 °C) and hot (70 °C) ends achieve a high power density (17.5 W m-2) and a large two-hour energy density (27 kJ m-2). In a prototype 25-cell module, the open-circuit voltage and short-circuit current are 6.9 V and 68 mA, respectively, and the maximum power is 131 mW. The anti-freezing ability and high output performance of the as-fabricated i-TE liquid cell system are requisites for applications in frigid regions.
Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge, in spite of the success seen with molecular doping strategies. However, the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance. Here, we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS (poly(3,4-ethylenedioxythiophene)-poly(4-styrenesulfonate)) thin film by using photochromic diarylethene (DAE) dopants coupled with UV-light modulation. With a 10-fold enhancement of the thermopower from 13.5 µV K-1 to 135.4 µV K-1 and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 µW m-1 K-2 from an original value of 6.78 µW m-1 K-2. The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature, indicating resonant coupling between the planar closed DAE molecule and PEDOT. Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling. Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.
The traditional quality gain-loss function(QGLF) considers the case that the primary term loss cannot be ignored, does not consider the cubic term loss, but in practice the cubic term loss should not be ignored. In this paper, based on the existing QGLF model, the Taylor expansion is reserved to the third order, the determination of the quality loss coefficient is discussed and analyzed under the condition that the compensation quantity is constant, and the asymmetric cubic QGLF model is established, and uses an example of concrete mixture out of the machine slump during the dam concrete construction to analyze and discuss the relationship between the proposed model and the traditional quadratic QGLF, which verifies the rationality of the proposed model.
Ferroelectric polymers have great potential applications in mechanical/thermal sensing, but their sensitivity and detection limit are still not outstanding. We propose interface engineering to improve the charge collection in a ferroelectric poly(vinylidene fluoride-co-trifluoroethylene) copolymer (P(VDF-TrFE)) thin film via cross-linking with poly(3,4-ethylenedioxythiophene) doped with polystyrenesulfonate (PEDOT:PSS) layer. The as-fabricated P(VDF-TrFE)/PEDOT:PSS composite film exhibits an ultrasensitive and linear mechanical/thermal response, showing sensitivities of 2.2 V kPa-1 in the pressure range of 0.025-100 kPa and 6.4 V K-1 in the temperature change range of 0.05-10 K. A corresponding piezoelectric coefficient of -86 pC N-1 and a pyroelectric coefficient of 95 µC m-2 K-1 are achieved because more charge is collected by the network interconnection interface between PEDOT:PSS and P(VDF-TrFE), related to the increase in the dielectric properties. Our work shines a light on a device-level technique route for boosting the sensitivity of ferroelectric polymer sensors through electrode interface engineering.
Engineering , Motion Pictures , Electrodes , Poly A , Polymers
Diffusion is a key kinetic factor determining chemical mixing and phase formation in liquids. In multicomponent systems, the presence of different elements makes it experimentally challenging to measure diffusivities and understand their mechanisms. Using a molecular dynamics simulation, we obtain the diffusion constants and the atomic process of a model Cantor alloy liquid made of five equimolar components. We show that the diffusivities conform remarkably well to the Arrhenius law in a wide range of temperature covering both the equilibrium and undercooled liquid regions. The activation energies for all the alloy elements with different bonding energies and atomic sizes are close to each other. The results suggest that the diffusivity in the multicomponent liquid tends to be homogenized by the components with marginal differences. This finding allows us to treat the different elements as a single type of atom, the pseudo-atom, for diffusional and maybe structural and physical properties in multicomponent liquids.
Artificial intelligence (AI) methods for the automatic detection and quantification of COVID-19 lesions in chest computed tomography (CT) might play an important role in the monitoring and management of the disease. We organized an international challenge and competition for the development and comparison of AI algorithms for this task, which we supported with public data and state-of-the-art benchmark methods. Board Certified Radiologists annotated 295 public images from two sources (A and B) for algorithms training (n=199, source A), validation (n=50, source A) and testing (n=23, source A; n=23, source B). There were 1,096 registered teams of which 225 and 98 completed the validation and testing phases, respectively. The challenge showed that AI models could be rapidly designed by diverse teams with the potential to measure disease or facilitate timely and patient-specific interventions. This paper provides an overview and the major outcomes of the COVID-19 Lung CT Lesion Segmentation Challenge - 2020.
COVID-19 , Pandemics , Humans , COVID-19/diagnostic imaging , Artificial Intelligence , Tomography, X-Ray Computed/methods , Lung/diagnostic imaging
Poly(3,4-ethylene dioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) thermoelectric thin films have attracted significant interest due to their solution-processable manufacturing. However, molecular-level tuning or doping is still a challenge to synergistically boost their thermoelectric performance and mechanically stretchable capabilities. In this work, we report a counterion exchange between ionic liquid bis(x-fluorosulfonyl) amide lithium (Li:nFSI, n = 1, 3, 5) with different sizes of anions and a PEDOT:PSS-induced bipolaron network, which significantly boosted the thermoelectric power factor from 0.8 to 157 µW m K-2 at 235 °C and the maximum tensile strain from 3% to over 30%. The π-π* stacking of the PEDOT polymer chains was fine-tuned by the hydrophobic anions of nFSI-, providing a technical route for constructing a bipolaron network and inducing the transition from hopping transport to band-like transport. Furthermore, we found that the stretchable capabilities, that is, εmax, were connected to the gelation time of the PEDOT:PSS-Li:nFSI aqueous solution. Thus, more fluorine-containing groups resulted in longer gelation times and higher εmax values, which significantly improved the processability of the solution-derived films.
It is a challenge to spontaneously harvest multiple clean sources from the environment for upgraded energy-converting systems. The ubiquitous moisture and sunlight in nature are attractive for sustainable power generation especially. A high-performance light-coordinated "moist-electric generator" (LMEG) based on the rational combination of a polyelectrolyte and a phytochrome is herein developed. By spontaneous adsorption of gaseous water molecules and simultaneous exposure to sunlight, a piece of 1 cm2 composite film offers an open-circuit voltage of 0.92 V and a considerable short-circuit current density of up to 1.55 mA cm-2 . This record-high current density is about two orders of magnitude improvement over that of most conventional moisture-enabled systems, which is caused by moisture-induced charge separation accompanied with photoexcited carrier migration, as confirmed by a dynamic Monte Carlo device simulation. Flexible devices with customizable size are available for large-scale integration to effectively work under a wide range of relative humidity (about 20-100%), temperature (10-80 °C), and light intensity (30-200 mW cm-2 ). The wearable and portable LMEGs provide ample power supply in natural conditions for indoor and outdoor electricity-consuming systems. This work opens a novel avenue to develop sustainable power generation through collecting multiple types of natural energy by a single hybrid harvester.
Organic molecules with thermally activated delayed fluorescence (TADF) and aggregation induced emission (AIE) properties have attracted increasing research interest due to their great potential applications in organic light emitting diodes (OLEDs), especially for those with multicolor mechanochromic luminescence (MCL) features. Theoretical research on the luminescence characteristics of organic TADF emitters based on the aggregation states is highly desired to quantify the relationship between the TADF properties and aggregation states. In this work, we study the 4,4'-(6-(9,9-dimethylacridine-10(9H)-yl)quinoline-2,3-dibenzonitrile (DMAC-CNQ) emitter with TADF and AIE properties, and calculate the photophysical properties in gas, solid and amorphous states by using the quantum mechanics and molecular mechanics (QM/MM) method. Our simulations demonstrate that the aggregation states enhance obviously the reverse intersystem crossing rates and transition dipole moments of the DMAC-CNQ emitter, and suppress the non-radiative rates from the lowest excited singlet state (S1) to ground state (S0). Specifically, the molecular stacking of DMAC-CNQ in solid phases can mainly restrict the geometric torsion of the DMAC moiety for decreasing non-radiative decay rates, and the torsion of the CNQ moiety for increasing the reverse intersystem crossing rates. As a result, the calculated fluorescence efficiencies of the DMAC-CNQ emitter in the crystal and amorphous states are 67% and 26% respectively, and in good agreement with the experimental results.
Although magnetorheological finishing (MRF) is being widely utilized to achieve ultra-smooth optical surfaces, the mechanisms for obtaining such extremely low roughness after the MRF process are not fully understood, especially the impact of finishing stresses. Herein we carefully investigated the relationship between the stresses and surface roughness. Normal stress shows stronger impacts on the surface roughness of fused silica (FS) when compared with the shear stress. In addition, normal stress in the polishing zone was found to be sensitive to the immersion depth of the magnetorheological (MR) fluid. Based on the above, a fine tuning of surface roughness (RMS: 0.22 nm) was obtained. This work fills gaps in understanding about the stresses that influence surface roughness during MRF.
The inherently small temperature difference in air environment restricts the applications of thermoelectric generation in the field of Internet of Things and wearable electronics. Here, a leaf-inspired flexible thermoelectric generator (leaf-TEG) that makes maximum use of temperature difference by vertically aligning poly(3,4-ethylenedioxythiophene) polystyrene sulfonate and constantan thin films is demonstrated. Analytical formulae of the performance scales, i.e., temperature difference utilization ratio (φth) and maximum output power (Pmax), are derived to optimize the leaf-TEG dimensions. In an air duct (substrate: 36 °C, air: 6 °C, air flowing: 1 m s-1), the 10-leaf-TEG shows a φth of 73% and Pmax of 0.38 µW per leaf. A proof-of-concept wearable 100-leaf-TEG (60 cm2) generates 11 µW on an arm at room temperature. Furthermore, the leaf-TEG is flexible and durable that is confirmed by bending and brushing over 1000 times. The proposed leaf-TEG is very appropriate for air convection scenarios with limited temperature differences.
Artificial intelligence (AI) methods for the automatic detection and quantification of COVID-19 lesions in chest computed tomography (CT) might play an important role in the monitoring and management of the disease. We organized an international challenge and competition for the development and comparison of AI algorithms for this task, which we supported with public data and state-of-the-art benchmark methods. Board Certified Radiologists annotated 295 public images from two sources (A and B) for algorithms training (n=199, source A), validation (n=50, source A) and testing (n=23, source A; n=23, source B). There were 1,096 registered teams of which 225 and 98 completed the validation and testing phases, respectively. The challenge showed that AI models could be rapidly designed by diverse teams with the potential to measure disease or facilitate timely and patient-specific interventions. This paper provides an overview and the major outcomes of the COVID-19 Lung CT Lesion Segmentation Challenge - 2020.
The role of dynamic and static disorder has been widely discussed for carrier transport in organic semiconductors. In this work, we apply a multiscale approach by combining molecular dynamics simulations, quantum mechanics calculations and kinetic Monte-Carlo simulations to study the influence of dynamic and static disorder on the hole mobility of four didodecyl[1]benzothieno[3,2-b]benzothiophene (BTBT-C12) isomers. It is found that the dynamic disorder of transfer integral tends to decrease the mobility for quasi-1D (quasi one-dimensional) BTBT1 and BTBT4 isomers and increase the mobility for 2D (two-dimensional) BTBT2 and BTBT3 isomers, while the dynamic disorder of site energy tends to decrease mobility for all the four isomers; however, the reduction in 2D molecules is much less than that in quasi-1D molecules. Results show that trap defects could reduce the mobility for both the quasi-1D and 2D molecular structures significantly, even to several orders of magnitude. In addition, our work also reveals that there might exist two kinds of oxidation defects of the scatter type for the concerned isomers, which thus leads to greater reduction in mobility for the quasi-1D molecular structures than the 2D molecular structures. The study shows that the 2D molecular structures are favored over the quasi-1D or 1D molecular structure, and it is expected that these results could be used to shed light on device design in organic electronics.
In this paper, ReaxFF force field combined with molecular dynamics method was used to study the ignition, deflagration, and detonation of pentaerythritol tetranitrate (PETN) induced by hot spots. The hot spot is 5.6% of the total volume. When the hot spot temperature is 1000 K, the deflagration and detonation of PETN cannot be observed in the simulation time of 200 ps. When the hot spot temperature is 2000 K, it corresponds to the heating time of 20 to 50 ps, deflation and detonation were observed. During hot spot ignition, the products of decomposition of the condensed phase PETN are dominated by NO2 and HONO. The energy required for the C-C bond and C-ONO2 bond cleavage in PETN is high, resulting in only a small amount of CH2O and NO3 during the reaction. Small nitrogen-containing molecules (such as NO2, NO3, HONO, HNO3, etc.) mainly exist during thermal equilibrium, while the number of N2 increases sharply during the thermal runaway stage, and a small amount of NH3 and NH2 are also produced. H2O molecules are formed before CO2 and N2 are produced, and the number always dominates. During the thermal runaway, the entire system can maintain a spontaneous reaction, resulting in a sharp rise in temperature of about 2500 K in 20 ps. During this phase, the catalytic effect of H2O accelerates the formation of CO2 and N2 due to the near Chapman-Jouguet point in the crystal. PETN is a weak oxygen balance explosive that results in a small amount of CO and H2 production during the thermal instability phase. When the reaction is balanced, the relative molecular mass is close to or exceeds that of PETN. The product is only less than 1% of the total mass fraction, while the small molecule product is as high as 78%, and some relative molecular masses are [75,225]. The intermediates account for about 21%. Rapid and complex reaction events make it difficult to accurately predict the structure of these intermediates by existing experiments and calculations, which will be the focus of future research.
The physical and chemical properties of typical nitrate energetic materials under hydrostatic compression and uniaxial compression were studied using the ReaxFF/lg force field combined with the molecular dynamics simulation method. Under hydrostatic compression, the P-V curve and the bulk modulus (B 0) obtained using the VFRS equation of state show that the compressibility of the three crystals is nitroglycerine (NG) > erythritol tetranitrate (ETN) > 2,3-bis-hydroxymethyl-2,3-dinitro-1,4-butanediol tetranitrate (NEST-1). The a- and c-axis of ETN are easy to compress under the action of hydrostatic pressure, but the b-axis is not easy to compress. The b-axis of NEST-1 is the most compressible, while the a- and c-axis can be compressed slightly when the initial pressure increases and then remains unchanged afterward. The a-, b-, and c-axes of NG all have similar compressibilities. By analyzing the change trend of the main bond lengths of the crystals, it can be seen that the most stable of the three crystals is the N-O bond and the largest change is in the O-NO2 bond. The stability of the C-O bond shows that the NO3 produced by nitrates is not from the C-O bond fracture. Under uniaxial compression, the stress tensor component, the average principal stress, and the hydrostatic pressure have similar trends and amplitudes, indicating that the anisotropy behaviors of the three crystals ETN, NEST-1, and NG are weak. There is no significant correlation between maximum shear stress and sensitivity. The maximum shear stresses τ xy and τ yz of the ETN in the [010] direction are 1.5 GPa higher than τ xz . However, the maximum shear stress of NG shows irregularity in different compression directions, indicating that there is no obvious correlation between the maximum shear stress and sensitivity.
Harvesting heat from the environment into electricity has the potential to power Internet-of-things (IoT) sensors, freeing them from cables or batteries and thus making them especially useful for wearable devices. We demonstrate a giant positive thermopower of 17.0 millivolts per degree Kelvin in a flexible, quasi-solid-state, ionic thermoelectric material using synergistic thermodiffusion and thermogalvanic effects. The ionic thermoelectric material is a gelatin matrix modulated with ion providers (KCl, NaCl, and KNO3) for thermodiffusion effect and a redox couple [Fe(CN)6 4-/Fe(CN)6 3-] for thermogalvanic effect. A proof-of-concept wearable device consisting of 25 unipolar elements generated more than 2 volts and a peak power of 5 microwatts using body heat. This ionic gelatin shows promise for environmental heat-to-electric energy conversion using ions as energy carriers.
Articular cartilage injury and degeneration causing pain and loss of quality-of-life has become a serious problem for increasingly aged populations. Given the poor self-renewal of adult human chondrocytes, alternative functional cell sources are needed. Direct reprogramming by small molecules potentially offers an oncogene-free and cost-effective approach to generate chondrocytes, but has yet to be investigated. Here, we directly reprogrammed mouse embryonic fibroblasts into PRG4+ chondrocytes using a 3D system with a chemical cocktail, VCRTc (valproic acid, CHIR98014, Repsox, TTNPB, and celecoxib). Using single-cell transcriptomics, we revealed the inhibition of fibroblast features and activation of chondrogenesis pathways in early reprograming, and the intermediate cellular process resembling cartilage development. The in vivo implantation of chemical-induced chondrocytes at defective articular surfaces promoted defect healing and rescued 63.4% of mechanical function loss. Our approach directly converts fibroblasts into functional cartilaginous cells, and also provides insights into potential pharmacological strategies for future cartilage regeneration.
Embryo, Mammalian/cytology , Fibroblasts/cytology , Fibrocartilage/cytology , Animals , Cellular Reprogramming , Chondrocytes/cytology , Chondrocytes/metabolism , Chondrogenesis , Fibroblasts/metabolism , Mice , Organoids/cytology , Regeneration , Tissue Scaffolds/chemistry , Transcriptome/genetics
The initial reaction mechanism of energetic materials under impact loading and the role of crystal properties in impact initiation and sensitivity are still unclear. In this paper, we report reactive molecular dynamics simulations of shock initiation of 1,3,5-trinitroperhydro-1,3,5-triazine (RDX) crystals containing a cube void. Shock-induced void collapse, hot spots formation and growth, as well as spalling are revealed to be dependent on the shock velocity. The void collapse times are 1.5 and 0.7 ps, for the shock velocity of 2 and 4 km·s-1, respectively. Results indicate that the initial hot spot formation consists of two steps: one is the temperature rise caused by local plastic deformation and the other is the temperature increase resulting from the collision of upstream and downstream particles during the void collapse. Whether hot spots will continue to grow or quench depends on sensitive balance between energy release caused by local physical and chemical reactions and various heat dissipation mechanisms. In our simulations, hot spot would grow for U p = 4 km·s-1; hot spot is weak to some extent for U p = 2 km·s-1. The tensile wave reflected by the shock wave after reaching the free surface causes the spalling, which depends on the initial shock velocity. Typical spalling occurs for the shock velocity 2 km·s-1, while the tensile wave induces the microsplit region in RDX crystals in the case of U p = 4 km·s-1. Chemical reactions are studied for Rankine-Hugoniot shock pressures P s = 14.4, 57.8 GPa. For the weak shock, there is almost no decomposition reaction of the RDX molecules near the spalling region. On the contrary, there are large number of small molecule products, such as H2O, CO2, NO2, and so forth, around the microsplit regions for the strong shock. The ruptures of N-NO2 bond are the main initial reaction mechanisms for the shocked RDX crystal and are not affected by shock strength, while the microsplit slows down the decomposition rate of RDX. The work in this paper can shed light on a thorough understanding of thermal ignition, hot spot growth, and other physical and chemical phenomena of energetic materials containing voids under impact loading.
Deformation of metallic glasses is closely related to their microstructures which depend on the composition, processing method, and the size of the materials. This subtle structure-property relation is fairly complex and remains to be explored. Here, we scrutinize the microstructural evolution in relation to the mechanical properties in metallic glass nanowires with the same composition and size but subtle microstructural differences by controlling the preparing process using molecular dynamics simulations. The results suggest that a structural threshold exists for the transformation of deformation mechanisms in metallic glasses: when the structural feature exceeds the threshold, the deformation changes from homogeneous flow to shear localized deformation.
Characterized by their slow adhering property, skeletal muscle myogenic progenitor cells (MPCs) have been widely utilized in skeletal muscle tissue engineering for muscle regeneration, but with limited efficacy. Skeletal muscle regeneration is regulated by various cell types, including a large number of rapidly adhering cells (RACs) where their functions and mechanisms are still unclear. In this study, we explored the function of RACs by co-culturing them with MPCs in a biomimetic skeletal muscle organoid system. Results showed that RACs promoted the myogenic potential of MPCs in the organoid. Single-cell RNA-Seq was also performed, classifying RACs into 7 cell subtypes, including one newly described cell subtype: teno-muscular cells (TMCs). Connectivity map of RACs and MPCs subpopulations revealed potential growth factors (VEGFA and HBEGF) and extracellular matrix (ECM) proteins involvement in the promotion of myogenesis of MPCs during muscle organoid formation. Finally, trans-well experiments and small molecular inhibitors blocking experiments confirmed the role of RACs in the promotion of myogenic differentiation of MPCs. The RACs reported here revealed complex cell diversity and connectivity with MPCs in the biomimetic skeletal muscle organoid system, which not only offers an attractive alternative for disease modeling and in vitro drug screening but also provides clues for in vivo muscle regeneration.
Muscle Development/genetics , Muscle, Skeletal/metabolism , Myoblasts/metabolism , Organoids/cytology , Animals , Cell Differentiation/genetics , Cell Proliferation/genetics , Cluster Analysis , Extracellular Matrix/genetics , Extracellular Matrix/metabolism , Heparin-binding EGF-like Growth Factor/genetics , Heparin-binding EGF-like Growth Factor/metabolism , Male , Mice , Mice, Inbred C57BL , Muscle, Skeletal/cytology , Myoblasts/cytology , Organoids/ultrastructure , RNA-Seq , Single-Cell Analysis , Transcriptome/genetics , Vascular Endothelial Growth Factor A/genetics , Vascular Endothelial Growth Factor A/metabolism
