A dissymmetric backbone and selenophene substitution on the central core was used for the synthesis of symmetric or dissymmetric A‐DA′D‐A type non‐fullerene small molecular acceptors (NF‐SMAs) with ...different numbers of selenophene. From S‐YSS‐Cl to A‐WSSe‐Cl and to S‐WSeSe‐Cl, a gradually red‐shifted absorption and a gradually larger electron mobility and crystallinity in neat thin film was observed. A‐WSSe‐Cl and S‐WSeSe‐Cl exhibit stronger and tighter intermolecular π–π stacking interactions, extra S⋅⋅⋅N non‐covalent intermolecular interactions from central benzothiadiazole, better ordered 3D interpenetrating charge‐transfer networks in comparison with thiophene‐based S‐YSS‐Cl. The dissymmetric A‐WSSe‐Cl‐based device has a PCE of 17.51 %, which is the highest value for selenophene‐based NF‐SMAs in binary polymer solar cells. The combination of dissymmetric core and precise replacement of selenophene on the central core is effective to improve Jsc and FF without sacrificing Voc.
A dissymmetric backbone and selenophene substitution on the central core was employed to synthesize dissymmetric A‐DA′D‐A NF‐SMAs. Their detailed single‐crystal packing were revealed successfully. The dissymmetric A‐WSSe‐Cl:PM6 device presented an impressive PCE of 17.51 %, which is the highest values for selenophene‐based and the dissymmetric NF‐SMAs in binary PSCs.
Integrating desirable light absorption, energy levels, and morphology in one matrix is always the aspiration to construct high‐performance organic solar cells (OSCs). Herein, an asymmetric acceptor ...Y6‐1O is incorporated into the binary blends of acceptor Y7‐BO and donor PM6 to prepare ternary OSCs. Two isogenous asymmetric–symmetric acceptors with similar chemical skeletons tend to form alloy‐like state in blends due to their good compatibility, which contributes to optimizing the morphology for efficient charge generation and extraction. The complementary absorption of two acceptors helps to improve the photon harvesting of ternary blends, and the higher lowest unoccupied molecular orbital (LUMO) energy level of Y6‐1O offers the chance to uplift the mixed LUMO energy levels of acceptors. Combining the aforesaid benefits, the ternary OSCs with 10 wt% Y6‐1O produce a top‐ranked power conversion efficiency (PCE) of 18.11% with simultaneously elevated short‐circuit current density, open‐circuit voltage, and fill factor in comparison to Y7‐BO‐based binary devices. Furthermore, the optimized ternary OSCs with ≈300 nm active layers obtain a champion PCE of 16.61%, which is the highest value for thick‐film devices reported so far. This work puts forward an avenue for further boosting the performance of OSCs with two isogenous acceptors but different asymmetric structures.
The synergistically optimized light absorption, energy levels, and morphology, by incorporating an asymmetric isogenous acceptor Y6‐1O in PM6:Y7‐BO‐based ternary organic solar cells (OSCs), is demonstrated. The optimized ternary OSCs produce a top‐ranked power conversion efficiency (PCE) of 18.11% and with ≈300 nm active layers obtain a champion PCE of 16.61%, which is the highest value for thick‐film devices reported so far.
Herein, we synthesized new hetero‐halogenated end groups with well‐determined fluorinated and chlorinated substitutions (o‐FCl‐IC and FClF‐IC), and synthesized regioisomer‐free small molecular ...acceptors (SMAs) Y‐Cl, Y‐FCl, and Y‐FClF with distinct hetero‐halogenated terminals, respectively. The single‐crystal structures and theoretical calculations indicate that Y‐FClF exhibits more compact three‐dimensional network packing and more significant π‐π electronic coupling compared to Y‐FCl. From Y‐Cl to Y‐FCl to Y‐FClF, the neat films exhibit a narrower optical band gap and gradually enhanced electron mobility and crystallinity. The PM6 : Y‐FClF blend film exhibits the strongest crystallinity with preferential face‐on molecular packing, desirable fibrous morphology with suitable phase segregation, and the highest and balanced charge mobilities among three blend films. Overall, the PM6 : Y‐FClF organic solar cells (OSCs) deliver a remarkable efficiency of 17.65 %, outperforming the PM6 : Y‐FCl and PM6 : Y‐Cl, which is the best PCE for reported hetero‐halogens‐based SMAs in binary OSCs. Our results demonstrate that difluoro‐monochloro hetero‐terminal is a superior regio‐regular unit for enhancing the intermolecular crystal packing and photovoltaic performance of hetero‐halogenated SMAs.
New fluorine/chlorine regio‐regular hetero‐trihalogenated terminal was firstly synthesized and systematically employed to enhance single‐crystal packing, improve film morphology, and boost device performance of the hetero‐halogenated SMAs. The PM6 : Y‐FClF achieved a remarkable PCE of 17.65 %, which is far better than that of Y‐Cl and Y‐FCl and is the highest efficiency for the hetero‐halogenated SMAs‐based binary OSCs.
The control effect of various intelligent terminals is affected by the data sensing precision. The filtering method has been the typical soft computing method used to promote the sensing level. Due ...to the difficult recognition of the practical system and the empirical parameter estimation in the traditional Kalman filter, a neuron-based Kalman filter was proposed in the paper. Firstly, the framework of the improved Kalman filter was designed, in which the neuro units were introduced. Secondly, the functions of the neuro units were excavated with the nonlinear autoregressive model. The neuro units optimized the filtering process to reduce the effect of the unpractical system model and hypothetical parameters. Thirdly, the adaptive filtering algorithm was proposed based on the new Kalman filter. Finally, the filter was verified with the simulation signals and practical measurements. The results proved that the filter was effective in noise elimination within the soft computing solution.
The evaluation of the hydraulic properties evolution of granular sandstones in relation with groundwater inrush within faults is an important issue for mining engineering applications. This paper ...presents the results of an experimental investigation of small particle migration from granular sandstone samples under different original porosities, particle size compositions and water flow pressures. A new rock testing system has been setup to carry out the tests. Based on the results, it is observed that the overall permeability evolution during the tests can be divided into four different phases, including i) re-arrangement of large rock fragments, ii) water inrush with substantial particle migration, iii) continued moderate particles seepage, and iv) steady state water flow. The crushing of edges and corners of large rock fragments, and the evolution of the fracture network has mainly been observed in the first two phases of the tests. The results indicate that the migration of small particles has an essential effect on permeability and porosity increase during water inrush through fractured sandstone. The samples with higher original porosity, higher percentage of fine particles in their formation and under higher water flow pressures, achieve higher permeability and porosity values when the test is complete. Furthermore, using the measured data, the performances of a number of empirical models, for permeability evolution in fractured porous media, have been studied. The prediction results indicate that not all of the fractures in a sample domain contribute in small particle migration. There are parts of the fracture network that are not effective in particle flow, a sample with less original porosity, more fine particles and under lower water pressure shows less ineffective fractures. Therefore, using the concept of the effective porosity (fracture) is sufficient enough for the flow calculation.
•The permeability evolution within granular sandstones under water inrush can be divided into four different phases.•Particle migration has an essential effect on permeability increase during water inrush.•Parts of the fracture network within the granular media are not effective for water and particle flow.
Since their discovery in 1960
, metallic glasses based on a wide range of elements have been developed
. However, the theoretical prediction of glass-forming compositions is challenging and the ...discovery of alloys with specific properties has so far largely been the result of trial and error
. Bulk metallic glasses can exhibit strength and elasticity surpassing those of conventional structural alloys
, but the mechanical properties of these glasses are critically dependent on the glass transition temperature. At temperatures approaching the glass transition, bulk metallic glasses undergo plastic flow, resulting in a substantial decrease in quasi-static strength. Bulk metallic glasses with glass transition temperatures greater than 1,000 kelvin have been developed, but the supercooled liquid region (between the glass transition and the crystallization temperature) is narrow, resulting in very little thermoplastic formability, which limits their practical applicability. Here we report the design of iridium/nickel/tantalum metallic glasses (and others also containing boron) with a glass transition temperature of up to 1,162 kelvin and a supercooled liquid region of 136 kelvin that is wider than that of most existing metallic glasses
. Our Ir-Ni-Ta-(B) glasses exhibit high strength at high temperatures compared to existing alloys: 3.7 gigapascals at 1,000 kelvin
. Their glass-forming ability is characterized by a critical casting thickness of three millimetres, suggesting that small-scale components for applications at high temperatures or in harsh environments can readily be obtained by thermoplastic forming
. To identify alloys of interest, we used a simplified combinatorial approach
harnessing a previously reported correlation between glass-forming ability and electrical resistivity
. This method is non-destructive, allowing subsequent testing of a range of physical properties on the same library of samples. The practicality of our design and discovery approach, exemplified by the identification of high-strength, high-temperature bulk metallic glasses, bodes well for enabling the discovery of other glassy alloys with exciting properties.
All‐small‐molecule organic solar cells (ASM‐OSCs) are challenging for their inadequate efficiency and device stability due to their more susceptive morphology. Herein, a family of isomeric small ...molecule donors (SMDs) is synthesized based on the benzodithiophene–terthiophene core with linear, 1st carbon, and 2nd carbon position branched butyl‐based rhodanine for ASM‐OSCs, respectively. The single crystal of thiophene‐substituted model T‐s‐Bu forms a more compact intermolecular packing with herringbone structure than slip‐layered packing‐based T‐n‐Bu and T‐i‐Bu. SM‐i‐Bu and SM‐s‐Bu show slightly blue‐shifted absorption and deepened HOMO levels in the neat film compared to SM‐n‐Bu. SM‐s‐Bu:BO‐4Cl blend films have distinct face‐on packing orientations and suitable fibrous phase separation along with more apparent microcrystals. Finally, SM‐s‐Bu:BO‐4Cl‐based device yields an improved power conversion efficiency of 16.06% compared to 15.12% and 8.22% for SM‐n‐Bu:BO‐4Cl and SM‐i‐Bu:BO‐4Cl, which is one of the top‐ranked results for BTR‐series SMDs in binary ASM‐OSCs. More importantly, the excellent storage stability with a T80 lifetime of over 1700 h and decent thermal stability is realized in SM‐s‐Bu:BO‐4Cl. This work highlights that the isomeric terminal alkyl with a branching point directly connected to the backbone for SMDs is a promising strategy for improving the crystal packing and film morphology and achieving highly efficient and stable ASM‐OSCs.
A family of isomeric small molecule donors based on benzodithiophene–terthiophene core with linear, the 1st carbon and 2nd carbon position branched butyl‐based rhodanine are synthesized. SM‐s‐Bu:BO‐4Cl‐based ASM‐OSCs show an impressive power conversion efficiency with over 16% and excellent storage stability with a T80 of over 1700 h, which is one of the top‐level results among BTR‐series small molecule donors in binary all‐small‐molecule organic solar cells.
Acute kidney injury (AKI), as a common oxidative stress‐related renal disease, causes high mortality in clinics annually, and many other clinical diseases, including the pandemic COVID‐19, have a ...high potential to cause AKI, yet only rehydration, renal dialysis, and other supportive therapies are available for AKI in the clinics. Nanotechnology‐mediated antioxidant therapy represents a promising therapeutic strategy for AKI treatment. However, current enzyme‐mimicking nanoantioxidants show poor biocompatibility and biodegradability, as well as non‐specific ROS level regulation, further potentially causing deleterious adverse effects. Herein, the authors report a novel non‐enzymatic antioxidant strategy based on ultrathin Ti3C2‐PVP nanosheets (TPNS) with excellent biocompatibility and great chemical reactivity toward multiple ROS for AKI treatment. These TPNS nanosheets exhibit enzyme/ROS‐triggered biodegradability and broad‐spectrum ROS scavenging ability through the readily occurring redox reaction between Ti3C2 and various ROS, as verified by theoretical calculations. Furthermore, both in vivo and in vitro experiments demonstrate that TPNS can serve as efficient antioxidant platforms to scavenge the overexpressed ROS and subsequently suppress oxidative stress‐induced inflammatory response through inhibition of NF‐κB signal pathway for AKI treatment. This study highlights a new type of therapeutic agent, that is, the redox‐mediated non‐enzymatic antioxidant MXene nanoplatforms in treatment of AKI and other ROS‐associated diseases.
A novel non‐enzymatic antioxidant MXene nanoplatform with excellent biocompatibility and great chemical reactivity toward multiple ROS is developed to potentially scavenge the overexpressed ROS and subsequently suppress oxidative stress‐induced inflammatory response through the inhibition of NF‐κB signaling pathway in the prevention and treatment of AKI and other ROS‐related diseases.
MicroRNAs can function as key tumor suppressors or oncogenes and act as biomarkers for cancer diagnosis or prognosis. Although high-throughput assays have revealed many miRNA biomarkers for ...pancreatic ductal adenocarcinoma (PDAC), only a few have been validated in independent populations or investigated for functional significance in PDAC pathogenesis. In this study, we correlated the expression of 36 potentially prognostic miRNAs within PDAC tissue with clinico-pathological features and survival in 151 Chinese patients. We then analyzed the functional roles and target genes of two miRNAs in PDAC development. We found that high expression of miR-186 and miR-326 predict poor and improved survival, respectively. miR-186 was over-expressed in PDAC patients compared with controls, especially in patients with large tumors (>2 cm), lymph node metastasis, or short-term survival (< 24 months). In contrast, miR-326 was down-regulated in patients compared with controls and displayed relatively increased expression in the patients with long-term survival or without venous invasion. Functional experiments revealed that PDAC cell proliferation and migration was decreased following inhibition and enhanced following over-expression of miR-186. In contrast, it was enhanced following inhibition and decreased after over-expression of miR-326. A luciferase assay indicated that miR-186 can bind directly to the 3'-UTR of NR5A2 to repress gene expression. These findings suggest that miR-186 over-expression contributes to the invasive potential of PDAC, likely via suppression of NR5A2, thereby leading to a poor prognosis; high miR-326 expression prolongs survival likely via the decreasing invasive potential of PDAC cells. These two miRNAs can be used as markers for clinical diagnosis and prognosis, and they represent therapeutic targets for PDAC.
Acute kidney injury (AKI) is the most common cause of organ failure in multiple organ dysfunction syndrome (MODS) and is associated with increased mortality. This study aimed at determining the ...efficacy of sequential organ failure assessment (SOFA), and acute physiology and chronic health evaluation II (APACHE-II) scoring systems in assessing the prognosis of critically ill patients with AKI undergoing continuous renal replacement therapy (CRRT). At present, APACHE-II score and SOFA score were also used to evaluate and predict the prognosis of critically ill patients with AKI.
The predictive value of SOFA and APACHE-II scores for 28- and 90-d mortality in patients with AKI undergoing CRRT were determined by multivariate analysis, sensitivity analysis, and curve-fitting analysis.
A total of 836 cases were included in this study. Multivariate Cox logistic regression analysis showed that SOFA scores were associated with 28- and 90-d mortality in patients with AKI undergoing CRRT. The adjusted HR of SOFA for 28-d mortality were 1.18 (1.14, 1.21), 1.24 (1.18, 1.31), and 1.19 (1.13, 1.24) in the three models, respectively, and the adjusted HR of SOFA for 90-d mortality was 1.12 (1.09, 1.16), 1.15 (1.10, 1.19), and 1.15 (1.10, 1.19), respectively. The subgroup analysis showed that the SOFA score was associated with 28-d and 90-d mortality in patients with AKI undergoing CRRT. APACHE-II score was not associated with 28- and 90-d mortality patients with AKI undergoing CRRT. Curve fitting analysis showed that SOFA scores increased had a higher prediction accuracy for 28- and 90-d than APACHE-II.
The SOFA score showed a higher accuracy of mortality prediction in critically ill patients with AKI undergoing CRRT than the APACHE-II score.