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While high‐performance p‐type semiconducting polymers are widely reported, their n‐type counterparts are still rare in terms of quantity and quality. Here, an improved Stille polymerization protocol using chlorobenzene as the solvent and palladium(0)/copper(I) as the catalyst is developed to synthesize high‐quality n‐type polymers with number‐average molecular weight up to 105 g mol?1. Furthermore, by sp2‐nitrogen atoms (sp2‐N) substitution, three new n‐type polymers, namely, pBTTz, pPPT, and pSNT, are synthesized, and the effect of different sp2‐N substitution positions on the device performances is studied for the first time. It is found that the incorporation of sp2‐N into the acceptor units rather than the donor units results in superior crystalline microstructures and higher electron mobilities. Furthermore, an amine‐tailed self‐assembled monolayer (SAM) is smoothly formed on a Si/SiO2 substrate by a simple spin‐coating technique, which can facilitate the accumulation of electrons and lead to more perfect unipolar n‐type transistor performances. Therefore, a remarkably high unipolar electron mobility up to 5.35 cm2 V?1 s?1 with a low threshold voltage (≈1 V) and high on/off current ratio of ≈107 is demonstrated for the pSNT‐based devices, which are among the highest values for unipolar n‐type semiconducting polymers.  相似文献   

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A novel polymer encapsulation strategy to synthesize metal isolated‐single‐atomic‐site (ISAS) catalysts supported by porous nitrogen‐doped carbon nanospheres is reported. First, metal precursors are encapsulated in situ by polymers through polymerization; then, metal ISASs are created within the polymer‐derived p‐CN nanospheres by controlled pyrolysis at high temperature (200–900 °C). Transmission electron microscopy and N2 sorption results reveal this material to exhibit a nanospheric morphology, a high surface area (≈380 m2 g?1), and a porous structure (with micropores and mesopores). Characterization by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure confirms the metal to be present as metal ISASs. This methodology is applicable to both noble and nonprecious metals (M‐ISAS/p‐CN, M = Co, Ni, Cu, Mn, Pd, etc.). In particular, the Co‐ISAS/p‐CN nanospheres obtained using this method show comparable (E1/2 = 0.838 V) electrochemical oxygen reduction activity to commercial Pt/C with 20 wt% Pt loading (E1/2 = 0.834 V) in alkaline media, superior methanol tolerance, and outstanding stability, even after 5000 cycles.  相似文献   

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Metal oxides, as one of the mostly abundant and widely utilized materials, are extensively investigated and applied in environmental remediation and protection, and in energy conversion and storage. Most of these diverse applications are the result of a large diversity of the electronic states of metal oxides. Noticeably, however, many metal oxides present obstacles for applications in catalysis, mainly due to the lack of efficient active sites with desired electronic states. Here, the fabrication of single‐tungsten‐atom‐oxide (STAO) is demonstrated, in which the metal oxide's volume reaches its minimum as a unit cell. The catalytic mechanism in the STAO is determined by a new single‐site physics mechanism, named as quasi‐atom physics. The photogenerated electron transfer process is enabled by an electron in the spin‐up channel excited from the highest occupied molecular orbital to the lowest unoccupied molecular orbital +1 state, which can only occur in STAO with W5+. STAO results in a record‐high and stable sunlight photocatalytic degradation rate of 0.24 s?1, which exceeds the rates of available photocatalysts by two orders of magnitude. The fabrication of STAO and its unique quasi‐atom photocatalytic mechanism lays new ground for achieving novel physical and chemical properties using single‐metal‐atom oxides (SMAO).  相似文献   

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The considerable advances that have been made in the development of organotypic cultures have failed to overcome the challenges of expressing tissue‐specific functions and complexities, especially for organs that require multitasking and complex biological processes, such as the liver. Primary liver cells are ideal biological building blocks for functional organotypic reconstruction, but are limited by their rapid loss of physiological integrity in vitro. Here the concept of lattice growth used in material science is applied to develop a tissue incubator, which provides physiological cues and controls the 3D assembly of primary cells. The cues include a biological growing template, spatial coculture, biomimetic radial flow, and circulation in a scaffold‐free condition. The feasibility of recapitulating a multiscale physiological structural hierarchy, complex drug clearance, and zonal physiology from the cell to tissue level in long‐term cultured liver‐on‐a‐chip is demonstrated. These methods are promising for future applications in pharmacodynamics and personal medicine.  相似文献   

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Plasmonic nanolasers based on wide bandgap semiconductors are presently attracting immense research interests due to the breaking in light diffraction limit and subwavelength mode operation with fast dynamics. However, these plasmonic nanolasers have so far been mostly realized in the visible light ranges, or most are still under optical excitation pumping. In this work, III‐nitride‐based plasmonic nanolasers emitting from the green to the deep‐ultraviolet (UV) region by energetic electron beam injection are reported, and a threshold as low as 8 kW cm?2 is achieved. A fast decay time as short as 123 ps is collected, indicating a strong coupling between excitons and surface plasmon. Both the spatial and temporal coherences are observed, which provide a solid evidence for exciton‐plasmon coupled polariton lasing. Consequently, the achievements in III‐nitride‐based plasmonic nanolaser devices represent a significant step toward practical applications for biological technology, computing systems, and on‐chip optical communication.  相似文献   

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Grinding of ceramic‐metal‐compounds – finite element analysis simulation of the grinding process of hybrid stratified compounds In this paper, the subproject TP 8 “Grinding of ceramic‐metal‐compounds” is been introduced. An adapted grinding strategy should be created for the production of a ceramic‐cemented carbide compound drill. This aim should be obtained with experimental analysis and the use of finite element analysis to simulate the grinding process of ceramic‐cemented carbide compound drill. Furthermore a basic approach for simulating the grinding process of hybrid stratified compounds is been presented, which should be a basis for a finite element analysis simulation of a grinding process of ceramic‐cemented carbide compound drill.  相似文献   

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Oxygen inhibition remains a challenge in photo‐curing technology despite the expenditure of considerable effort in developing a convenient, efficient, and low‐cost prevention method. Here, a novel strategy to prevent oxygen inhibition is presented; it is based on the self‐assembly of multifunctional nano‐photo‐initiators (F2‐POSS‐(SH)4‐TX/EDB) at the interface of air and the liquid monomer. These nano‐photo‐initiators consist of a thiol‐containing polyhedral oligomeric silsesquioxane (POSS) skeleton onto which fluorocarbon chains and thioxanthone and dimethylaminobenzoate (TX/EDB) photo‐initiator moieties are grafted. Real‐time Fourier‐transform infrared spectroscopy (FT‐IR) is used to investigate the photo‐polymerization of various acrylate monomers that are initiated by F2‐POSS‐(SH)4‐TX/EDB and its model analogues in air and in N2. FT‐IR results show that F2‐POSS‐(SH)4‐TX/EDB decreases the effects of oxygen inhibition. X‐ray photo‐electron spectroscopy and atomic force microscopy reveal that the self‐assembly of F2‐POSS‐(SH)4‐TX/EDB at the air/(liquid monomer) interface forms a cross‐linked top layer via thiol–ene polymerization; this layer acts as a physical barrier against the diffusion of oxygen from the surface into the bulk layer. A mismatch in the shrinkage between the top and bulk layers arise as a result of the different types of photo‐cross‐linking reactions. Subsequently, the surface develops a wrinkled pattern with a low surface energy. This strategy exhibits considerable potential for preventing oxygen inhibition, and the wrinkled pattern may prove very useful in photo‐curing technology.  相似文献   

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The role of skin in the human body is indispensable, serving as a barrier, moderating homeostatic balance, and representing a pronounced endpoint for cosmetics and pharmaceuticals. Despite the extensive achievements of in vitro skin models, they do not recapitulate the complexity of human skin; thus, there remains a dependence on animal models during preclinical drug trials, resulting in expensive drug development with high failure rates. By imparting a fine control over the microenvironment and inducing relevant mechanical cues, skin‐on‐a‐chip (SoC) models have circumvented the limitations of conventional cell studies. Enhanced barrier properties, vascularization, and improved phenotypic differentiation have been achieved by SoC models; however, the successful inclusion of appendages such as hair follicles and sweat glands and pigmentation relevance have yet to be realized. The present Review collates the progress of SoC platforms with a focus on their fabrication and the incorporation of mechanical cues, sensors, and blood vessels.  相似文献   

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Wurtzite materials exhibit both semiconductor and piezoelectric properties under strains due to the non‐central symmetric crystal structures. The three‐way coupling of semiconductor properties, piezoelectric polarization and optical excitation in ZnO, GaN, CdS and other piezoelectric semiconductors leads to the emerging field of piezo‐phototronics. This effect can efficiently manipulate the emission intensity of light‐emitting diodes (LEDs) by utilizing the piezo‐polarization charges created at the junction upon straining to modulate the energy band diagrams and the optoelectronic processes, such as generation, separation, recombination and/or transport of charge carriers. Starting from fundamental physics principles, recent progress in piezo‐phototronic‐effect‐enhanced LEDs is reviewed; following their development from single‐nanowire pressure‐sensitive devices to high‐resolution array matrices for pressure‐distribution mapping applications. The piezo‐phototronic effect provides a promising method to enhance the light emission of LEDs based on piezoelectric semiconductors through applying static strains, and may find perspective applications in various optoelectronic devices and integrated systems.  相似文献   

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Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.  相似文献   

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Neutrophil‐to‐lymphocyte ratio (NLR) was introduced as a potential marker to determine inflammation in end‐stage renal disease (ESRD) patients. Recently, platelet‐to‐lymphocyte ratio (PLR) and NLR were found to positively correlated with inflammatory markers including tumor necrosis factor‐α (TNF‐α) and interleukin (IL)‐6 in cardiac and noncardiac patients. Data regarding PLR and its association with inflammation are lacking in hemodialysis (HD) and peritoneal dialysis (PD) patients. Hence, we aimed to determine the relationship between PLR, NLR, and inflammation in ESRD patients. This was a cross‐sectional study involving 62 ESRD patients (29 females, 33 males; mean age, 49.6 ± 14.6 years) receiving PD or HD for ≥6 months in the Dialysis Unit of Necmettin Erbakan University. PLR, NLR, C‐reactive protein, TNF‐α, IL‐6 levels were measured. PLR, NLR, serum high sensitive C‐reactive protein, IL‐6, and TNF‐α levels were significantly higher in PD patients when compared with HD patients. ESRD patients with PLR ≥ 140 had significantly higher NLR, IL‐6, and TNF‐α levels when compared to patients with PLR < 139. In the bivariate correlation analysis, PLR was positively correlated with NLR, IL‐6, and TNF‐α in this population. When we compared the association of PLR and NLR with IL‐6 (r = 0.371, P = 0.003 vs. r = 0.263, P = 0.04, respectively) and TNF‐α (r = 0.334, P = 0.008 vs. r = 0.273, P = 0.032, respectively), PLR was found to be superior to NLR in terms of inflammation in ESRD patients. Simple calculation of PLR can predict inflammation better than NLR in ESRD patients.  相似文献   

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All‐solution‐processing at low temperatures is important and desirable for making printed photovoltaic devices and also offers the possibility of a safe and cost‐effective fabrication environment for the devices. Herein, an all‐solution‐processed flexible organic solar cell (OSC) using poly(3,4‐ethylenedioxythiophene):poly‐(styrenesulfonate) electrodes is reported. The all‐solution‐processed flexible devices yield the highest power conversion efficiency of 10.12% with high fill factor of over 70%, which is the highest value for metal‐oxide‐free flexible OSCs reported so far. The enhanced performance is attributed to the newly developed gentle acid treatment at room temperature that enables a high‐performance PEDOT:PSS/plastic underlying substrate with a matched work function (≈4.91 eV), and the interface engineering that endows the devices with better interface contacts and improved hole mobility. Furthermore, the flexible devices exhibit an excellent mechanical flexibility, as indicated by a high retention (≈94%) of the initial efficiency after 1000 bending cycles. This work provides a simple route to fabricate high‐performance all‐solution‐processed flexible OSCs, which is important for the development of printing, blading, and roll‐to‐roll technologies.  相似文献   

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