Heterostructured metal—organic framework (MOF)‐on‐MOF thin films have the potential to cascade the various properties of different MOF layers in a sequence to produce functions that cannot be ...achieved by single MOF layers. An integration method that relies on van der Waals interactions, and which overcomes the lattice‐matching limits of reported methods, has been developed. The method deposits molecular sieving Cu‐TCPP (TCPP=5,10,15,20‐tetrakis(4‐carboxyphenyl)porphyrin) layers onto semiconductive Cu‐HHTP (HHTP=2,3,6,7,10,11‐hexahydrotriphenylene) layers to obtain highly oriented MOF‐on‐MOF thin films. For the first time, the properties in different MOF layers were cascaded in sequence to synergistically produce an enhanced device function. Cu‐TCPP‐on‐Cu‐HHTP demonstrated excellent selectivity and the highest response to benzene of the reported recoverable chemiresistive sensing materials that are active at room temperature. This method allows integration of MOFs with cascading properties into advanced functional materials.
MOF‐on‐MOF thin films were prepared from Cu‐HHTP (HHTP=hexahydrotriphenylene) and Cu‐TCPP (TCPP=tetrakis(4‐carboxyphenyl)porphyrin frameworks). The properties of the MOF layers cascade to produce functionality not achieved by a single layer. The MOF‐on‐MOF films demonstrate excellent selectivity and the highest response to benzene among reported recoverable chemiresistive sensing materials active at room temperature.
Circularly polarized thermally activated delayed fluorescence (CP‐TADF) and multiple‐resonance thermally activated delayed fluorescence (MR‐TADF), which exhibit novel circularly polarized ...luminescence and excellent color fidelity, respectively, have gained immense popularity. In this study, integrated CP‐TADF and MR‐TADF (CPMR‐TADF) are prepared by strategic design and synthesis of asymmetrical peripherally locked enantiomers, which are separated and denoted as (P,P″,P″)‐/(M,M″,M″)‐BN4 and (P,P″,P″)‐/(M,M″,M″)‐BN5 and exhibit TADF and circularly polarized light (CPL) properties. As the entire molecular frame participates in the frontier molecular orbitals, the resulting helical chirality of (+)/(−)‐BN4‐ and (+)/(−)‐BN5‐based solution‐processed organic light‐emitting diodes (OLEDs) helps in achieving a narrow full width at half maximum (FWHM) of 49/49 and 48/48 nm and a high maximum external quantum efficiency (EQE) of 20.6%/19.0% and 22.0%/26.5%, respectively. Importantly, unambiguous circularly polarized electroluminescence signals with dissymmetry factors (gEL) of +3.7 × 10−3/−3.1 × 10−3 (BN4) and +1.9 × 10−3/−1.6 × 10−3 (BN5) are obtained. The results indicate successful exploitation of CPMR‐TADF‐emitter‐based OLEDs to exhibit three characteristics: high efficiency, color purity, and circularly polarized light.
Circularly polarized thermally activated delayed fluorescence (CP‐TADF) and multiple‐resonance thermally activated delayed fluorescence (MR‐TADF) properties are integrated into a new advanced material, a CPMR‐TADF material. OLEDs based on these CPMR‐TADF emitters show excellent performance, attaining a three‐in‐one advantage: high efficiency, color purity, and circular polarized light simultaneously.
Background
Biopsy Gleason score (GS) is crucial for prostate cancer (PCa) treatment decision‐making. Upgrading in GS from biopsy to radical prostatectomy (RP) puts a proportion of patients at risk of ...undertreatment.
Purpose
To develop and validate a radiomics model based on multiparametric magnetic resonance imaging (mp‐MRI) to predict PCa upgrading.
Study Type
Retrospective, radiomics.
Population
A total of 166 RP‐confirmed PCa patients (training cohort, n = 116; validation cohort, n = 50) were included.
Field Strength/Sequence
3.0T/T2‐weighted (T2W), apparent diffusion coefficient (ADC), and dynamic contrast enhancement (DCE) sequences.
Assessment
PI‐RADSv2 score for each tumor was recorded. Radiomic features were extracted from T2W, ADC, and DCE sequences and Mutual Information Maximization criterion was used to identify the optimal features on each sequence. Multivariate logistic regression analysis was used to develop predictive models and a radiomics nomogram and their performance was evaluated.
Statistical Tests
Student's t or chi‐square were used to assess the differences in clinicopathologic data between the training and validation cohorts. Receiver operating characteristic (ROC) curve analysis was performed and the area under the curve (AUC) was calculated.
Results
In PI‐RADSv2 assessment, 67 lesions scored 5, 70 lesions scored 4, and 29 lesions scored 3. For each sequence, 4404 features were extracted and the top 20 best features were selected. The radiomics model incorporating signatures from the three sequences achieved better performance than any single sequence (AUC: radiomics model 0.868, T2W 0.700, ADC 0.759, DCE 0.726). The combined mode incorporating radiomics signature, clinical stage, and time from biopsy to RP outperformed the clinical model and radiomics model (AUC: combined model 0.910, clinical model 0.646, radiomics model 0.868). The nomogram showed good performance (AUC 0.910) and calibration (P‐values: training cohort 0.624, validation cohort 0.294).
Data Conclusion
Radiomics based on mp‐MRI has potential to predict upgrading of PCa from biopsy to RP.
Level of Evidence
3
Technical Efficacy
Stage 5 J. Magn. Reson. Imaging 2020;52:1239–1248.
Hyperglycemia in diabetic mothers enhances the risk of fetal cardiac hypertrophy during gestation. However, the mechanism of high-glucose-induced cardiac hypertrophy is not largely understood. In ...this study, we first demonstrated that the incidence rate of cardiac hypertrophy dramatically increased in fetuses of diabetic mothers using color ultrasound examination. In addition, human fetal cardiac hypertrophy was successfully mimicked in a streptozotocin (STZ)-induced diabetes mouse model, in which mouse cardiac hypertrophy was diagnosed using type-M ultrasound and a histological assay. PH3 immunofluorescent staining of mouse fetal hearts and in vitro-cultured H9c2 cells indicated that cell proliferation decreased in E18.5, E15.5 and E13.5 mice, and cell apoptosis in H9c2 cells increased in the presence of high glucose in a dose-dependent manner. Next, we found that the individual cardiomyocyte size increased in pre-gestational diabetes mellitus mice and in response to high glucose exposure. Meanwhile, the expression of β-MHC and BMP-10 was up-regulated. Nkx2.5 immunofluorescent staining showed that the expression of Nkx2.5, a crucial cardiac transcription factor, was suppressed in the ventricular septum, left ventricular wall and right ventricular wall of E18.5, E15.5 and E13.5 mouse hearts. However, cardiac hypertrophy did not morphologically occur in E13.5 mouse hearts. In cultured H9c2 cells exposed to high glucose, Nkx2.5 expression decreased, as detected by both immunostaining and western blotting, and the expression of KCNE1 and Cx43 was also restricted. Taken together, alterations in cell size rather than cell proliferation or apoptosis are responsible for hyperglycemia-induced fetal cardiac hypertrophy. The aberrant expression of Nkx2.5 and its regulatory target genes in the presence of high glucose could be a principal component of pathogenesis in the development of fetal cardiac hypertrophy.
Recently, the newest Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 6.1 (C6.1) aerosol optical depth (AOD) products were available with various refinements and improvements made to ...both the radiation calibration and Dark Target (DT) and Deep Blue (DB) algorithms. A combined DT and DB dataset (DTB) was also added based on piecewise fixed thresholds using the Normalized Difference Vegetation Index (NDVI) for taking advantage of one's merits. This study provides a cross-comparison and evaluation of these Terra MODIS aerosol products with reference to the enhanced ground-based AOD measurements by the Aerosol Robotic Network (AERONET) Level 3 Version 2.0 data at 384 ground stations. Their absolute and relative performance are evaluated in the period of 2013–2017 among the products, as well as between the current (C6.1) and previous (C6) releases. In general, the C6.1 aerosol products are found to be superior over the C6 products for three datasets from all scales, but the differences and improvements are rather non-uniform that varies with region. Overall, the DB AOD products show the best performance in most regions at about half of the sites, especially in Europe and North America. Meanwhile, besides bright surfaces (i.e., deserts and arid/semi-arid areas), DB products match more closely with the AERONET AODs than that of DT over medium or densely vegetated areas. The dependences of retrieval errors illustrate that the performance of three datasets deteriorates as surface reflectance, elevation and aerosol loading increase. However, the DB algorithm remains relatively more stable and less affected by changes in atmospheric and surface conditions. While the merged product using NDVI has some improvements over individual ones in general, worse performance is also shown in many cases. A more optimal method is thus wanting.
•The latest MODIS C6.1 DT, DB and DTB AOD products are improved than the C6 release.•Higher accuracy is found for the DB product in more places than just over the bright surfaces.•Generation of the merged products based on NDVI may not lead to optimal results.•Retrieval uncertainties on six main independent factors are comprehensively analyzed.
Pores in a solid can effectively reduce thermal conduction, but they are not favored in thermoelectric materials due to simultaneous deterioration of electrical conductivity. Conceivably, creating a ...porous structure may endow thermoelectric performance enhancement provided that overwhelming reduction of electrical conductivity can be suppressed. This work demonstrates such an example, in which a porous structure is formed leading to a significant enhancement in the thermoelectric figure of merit (zT). By a unique BiI3 sublimation technique, pore networks can be introduced into tetrahedrite Cu12Sb4S13‐based materials, accompanied by changes in their hierarchical structures. The addition of a small quantity of BiI3 (0.7 vol%) results in a ≈72% reduction in the lattice thermal conductivity, whereas the electrical conductivity is improved due to unexpected enhanced carrier mobility. As a result, an enhanced zT of 1.15 at 723 K in porous tetrahedrite and a high conversion efficiency of 6% at ΔT = 419 K in a fabricated segmented single‐leg based on this porous material are achieved. This work offers an effective way to concurrently modulate the electrical and thermal properties during the synthesis of high‐performance porous thermoelectric materials.
A porous network structure with excellent electrical properties can enhance the thermoelectric performance of solid materials. This work demonstrates that a porous structure can be introduced into tetrahedrite‐based synthetic minerals by a unique BiI3 sublimation technique. The multiscale architectures simultaneously disrupt phonon transport and trigger energy‐dependent scattering of holes, leading to a superior zT value of 1.15 at 723 K.
Lithium–sulfur (Li–S) batteries are highly regarded as the next‐generation energy‐storage devices because of their ultrahigh theoretical energy density of 2600 Wh kg−1. Sulfurized polyacrylonitrile ...(SPAN) is considered a promising sulfur cathode to substitute carbon/sulfur (C/S) composites to afford higher Coulombic efficiency, improved cycling stability, and potential high‐energy‐density Li–SPAN batteries. However, the instability of the Li‐metal anode threatens the performances of Li–SPAN batteries bringing limited lifespan and safety hazards. Li‐metal can react with most kinds of electrolyte to generate a protective solid electrolyte interphase (SEI), electrolyte regulation is a widely accepted strategy to protect Li‐metal anodes in rechargeable batteries. Herein, the basic principles and current challenges of Li–SPAN batteries are addressed. Recent advances on electrolyte regulation towards stable Li‐metal anodes in Li–SPAN batteries are summarized to suggest design strategies of solvents, lithium salts, additives, and gel electrolyte. Finally, prospects for future electrolyte design and Li anode protection in Li–SPAN batteries are discussed.
Increased attention SPAN: Recent advances in electrolyte regulation towards stable lithium‐metal anodes for Li‐sulfurized polyacrylonitrile (SPAN) batteries are summarized to afford design strategies of solvents, lithium salts, additives, and gel electrolyte.
Spherical mesoporous Fe-N-C single-atom nanozyme with excellent peroxidase-like activity and photothermal property is developed via a soft-template method. Light irradiation can not only improve the ...catalytic activity of nanozyme via the increasement of reaction temperature, but also be used to kill bacteria via photothermal treatment. The synergistic effect can effectively accelerate the wound healing in vivo.
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Nanozyme has been regarded as an efficient antibiotic to kill bacteria using the reactive oxygen species (ROS) generated by Fenton-like reaction. However, its activity is still unsatisfied and requires large amount of hydrogen peroxide with side effects toward normal tissues. Herein, spherical mesoporous Fe-N-C single-atom nanozyme (SAzyme) is designed for antibacterial therapy via photothermal treatment enhanced Fenton-like catalysis process. Due to the large pore size (4.0 nm), high specific surface area (413.9 m2 g−1) and uniform diameter (100 nm), the catalytic performance of Fe-N-C SAzyme is greatly improved. The Michaelis-Menten constant (Km) is 4.84 mmol L−1, which is similar with that of horseradish peroxidase (3.7 mmol L−1). Moreover, mesoporous Fe-N-C SAzyme shows high photothermal conversion efficiency (23.3 %) owing to the carbon framework. The catalytic activity can be enhanced under light irradiation due to the elevated reaction temperature. The bacteria can also be killed via physical heat effect. Due to the synergistic effect of nanozyme catalysis and photothermal treatment, the antibacterial performance is much higher than that using single antibacterial method. This work provides an alternative for combined antibacterial treatment via photothermal treatment assisted catalytic process using spherical mesoporous single-atom nanozyme as an antibiotic.
Squalene, a valuable acyclic triterpene, can be used as a chemical commodity for pharmacology, flavor, and biofuel industries. Microbial production of squalene has been of great interest due to its ...limited availability, and increasing prices extracted from animal and plant tissues. Here we report genetic perturbations that synergistically improve squalene production in Saccharomyces cerevisiae. As reported previously, overexpression of a truncated HMG‐CoA reductase 1 (tHMG1) led to the accumulation 20‐fold higher squalene than a parental strain. In order to further increase squalene accumulation in the tHMG1 overexpressing yeast, we introduced genetic perturbations—known to increase lipid contents in yeast—to enhance squalene accumulation as lipid body is a potential storage of squalene. Specifically, DGA1 coding for diacylglycerol acyltranferase was overexpressed to enhance lipid biosynthesis, and POX1 and PXA2 coding for acyl‐CoA oxidase and a subunit of peroxisomal ABC transporter were deleted to reduce lipid β‐oxidation. Simultaneous overexpression of tHMG1 and DGA1 coding for rate‐limiting enzymes in the mevalonate and lipid biosynthesis pathways led to over 250‐fold higher squalene accumulation than a control strain. However, deletion of POX1 and PXA2 in the tHMG1 overexpressing yeast did not improve squalene accumulation additionally. Fed‐batch fermentation of the tHMG1 and DGA1 co‐overexpressing yeast strain resulted in the production of squalene at a titer of 445.6 mg/L in a nitrogen‐limited minimal medium. This report demonstrates that increasing storage capacity for hydrophobic compounds can enhance squalene production, suggesting that increasing lipid content is an effective strategy to overproduce a hydrophobic molecule in yeast.
This study focused on the genetic perturbations eliciting improved lipid production and enhanced squalene accumulation in Saccharomyces cerevisiae. The engineered strains, with simultaneous overexpression of tHMG1 and DGA1 coding for rate‐limiting enzymes in the mevalonate and lipid biosynthesis pathways, showed over 250‐fold higher squalene accumulation than a control strain. The results indicated that increasing storage capacity for hydrophobic compounds enhances squalene production.
Mg3(Sb,Bi)2 is a potential nearly‐room temperature thermoelectric compound composed of earth‐abundant elements. However, complex defect tuning and exceptional microstructural control are required. ...Prior studies have confirmed the detrimental effect of Mg vacancies (VMg) in Mg3(Sb,Bi)2. This study proposes an approach to mitigating the negative scattering effect of VMg by Bi deficiency, synergistically modulating the electrical and thermal transport properties to enhance the thermoelectric performance. Positron annihilation spectrometry and Cs‐corrected scanning transmission electron microscopy analyses indicated that the VMg tends to coalesce due to the introduced Bi vacancies (VBi). The defects created by Bi deficiency effectively weaken the scattering of electrons from the intrinsic VMg and enhance phonon scattering. A peak zT of 1.82 at 773 K and high conversion efficiency of 11.3% at ∆T = 473 K are achieved in the optimized composition of Mg3(Sb,Bi)2 by tuning the defect combination. This work demonstrates a feasible and effective approach to improving the performance of Mg3(Sb,Bi)2 as an emerging thermoelectric material.
The formation and tuning of complex defects can effectively enhance the thermoelectric performance of Mg3(Sb,Bi)2. This work proposes an approach to mitigate the negative scattering effect of Mg vacancies by Bi deficiency. The heterovalent vacancies provide a strong phonon scattering, leading to a significant reduction of the lattice thermal conductivity and a superior zT.
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