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Organic electrode molecules hold significant potential as the next generation of cathode materials for Li-ion batteries. In this study, we have introduced a multi-objective active learning framework that leverages Bayesian optimization and non-dominated sorting genetic algorithms-II. This framework enables the selection of organic molecules characterized by high theoretical energy density and low gap (LUMO-HOMO) (LUMO, lowest unoccupied molecular orbital; HOMO, highest occupied molecular orbital). Remarkably, after only two cycles of active learning, the determination of coefficient can reach 0.962 for theoretical energy density and 0.920 for the gap with a modest dataset of 300 molecules, showcasing superior predictive capabilities. The 2,3,5,6-tetrafluorocyclohexa-2,5-diene-1,4-dione, selected by non-dominated sorting genetic algorithms-II, has been successfully applied to Li-ion batteries as cathode materials, demonstrating a high capacity of 288 mAh g−1and a long cycle life of 1,000 cycles. This outcome underscores the high reliability of our framework. Furthermore, we have also validated the universality and transferability of our framework by applying it to two additional databases, the QM9 and OMEAD. When the training dataset of the model includes at least 500 molecules, the determination of coefficient essentially reaches approximately 0.900 for four targets: gap, reduction potential, LUMO, and HOMO. Therefore, the universal framework in our work provides innovative insights applicable to other domains to expedite the screening process for target materials.

Recent decades have witnessed remarkable progress in ligand-promoted C–H activation with palladium catalysts. While a number of transformations have been achieved with a fairly broad substrate scope, the general requirements for high palladium loadings and enormous challenges in catalyst recycling severely limit the practical applications of C–H activation methodologies in organic synthesis. Herein, we incorporate N,C-ligand-chelated palladacycles into rigid, porous, and crystalline covalent organic frameworks for the C–H arylation of indole and pyrrole derivatives. These heterogeneous palladium catalysts exhibit superior stability and recyclability compared to their homogeneous counterparts. We not only produce several highly reactive palladacycles embedded on new framework supports to facilitate C–H activation/C–C bond-forming reactions but also reassign heterogenized palladium species on frameworks containing a benzaldehyde-derived imine moiety as imine-based palladacycles via comprehensive characterization. Our findings provide guidance for the rational design of framework-supported metallacycles in the development of heterogeneous transition-metal catalysis.

Demand-responsive transit (DRT) with smartphone-based applications is emerging as a flexible and sustainable mobility service, transforming urban transportation. Nevertheless, to satisfy the real-time and inconsistent demand, it is becoming increasingly important to capture the decision-making psychology of order cancellations. In this study, a two-phase optimization framework is presented in response to real-time disruptions, including order cancellations and the insertion of new real-time passengers. In contrast to random real-time demand, this paper is more concerned about the impacts of the feedback information on order cancellations. Bounded rationality is incorporated into the model to discuss the decision-making process of cancellation behaviors. With regard to the soft window, a compensation strategy is proposed to promote the profit while encouraging passengers for a long-term use. Additionally, solution algorithm based on variable neighborhood search (VNS) and rolling horizon is constructed to approach the Pareto solutions set. To testify the validity of the proposed algorithm, small-scale experiments in simplified Sioux Falls network are investigated for multiple runs. Meanwhile, a real-world case study in Beijing is explored to evaluate the system performance considering real-time disruptions. The results indicate that the dynamic DRT service can substantially improve the system profit but increase the penalty cost. The profit presents a significant improvement to 940 (renminbi) RMB as a result of the insert of real-time passengers. This study, therefore, not only provides a deeper insight into the analysis of passenger cancellation behavior but also contributes to construct a more flexible DRT service.

A novel and unique approach for the construction of polysubstituted pyrimido[4,5-b]indoles from 2-(indol-3-yl)naphthoquinones and benzamidines is described. Our strategy, promoted by an inorganic base, involves the ring opening and recyclization of naphthoquinone and produces three nitrogen heterocyclic rings via multiple C–N bond formations in one pot under transition-metal-free conditions.

The incorporation of gem-difluoromethylene units into organic molecules remains a formidable challenge. Conventional methodologies for constructing aryldifluoromethyl derivatives relied on the use of high-functional fluorinating regents under harsh conditions. Herein, we report general and efficient photoredox catalytic systems for defluoroalkylation of readily available trifluoromethylarenes through selective C–F cleavage to deliver gem-difluoromethyl radicals which proceed through reductive addition to both electron-donating and withdrawing alkenes under transition-metal free conditions. Mechanistic studies reveal that thiol serves as both photocatalyst and HAT reagent under visible light irradiation. This synergistic photocatalysis and HAT catalysis protocol exhibits ample and salient features such as high chemo- and regioselectivity, broad substrate scope, amenable gram-scale synthesis and late-stage modification of bioactive molecules.

A convenient protocol for synthesis of unsymmetrical 2-methylpyridines from acetyl ketones, ammonium salts and tertiary amines is described. The construction of two C–C bonds and two C–N bonds via [2 + 2 + 1 + 1] four-component domino cyclization reaction is achieved using Cu(OTf) as catalyst in one pot. This cyclization reaction shows good selectivity and produces multisubstituted 2-methylpyridine derivatives in good yields with various functional groups.

The aim of this study was to evaluate the preclinical efficacy of [89Zr]Zr-DFO-Ab253 as a novel positron emission tomography (PET) tracer for CD146-positive malignant melanoma imaging. Considering the high expression of CD146 in malignant melanoma, this study investigated the effect of different CD146 expression levels on the tumor uptake of [89Zr]Zr-DFO-Ab253. CD146 selectivity was investigated by using the CD146-positive human melanoma cell A375 and the CD146-negative human alveolar epithelial cell A549. The cell uptake of [89Zr]Zr-DFO-Ab253 tracers was investigated, and receptor-binding affinities were measured by radioactive enzyme-linked immunosorbent assay. Biodistribution studies and micro-PET imaging of the radiotracers were performed on mice bearing A375 and A549 xenografts under baseline and blocking conditions. An immunohistochemical test was performed using A375 and A549 tissue sections for CD146 expression level analysis. [89Zr]Zr-DFO-Ab253 was obtained with a high radiochemical yield (87.86 ± 4.66%) and a satisfactory radiochemical purity (>98.0%). The specificity and affinity of [89Zr]Zr-DFO-Ab253 were confirmed in melanoma A375 cells and in vivo PET imaging of A375 tumor models. [89Zr]Zr-DFO-IgG and A549 lung tumors were prepared as control radiotracers and negative models to verify the specificity of [89Zr]Zr-DFO-Ab253 on CD146. [89Zr]Zr-DFO-Ab253 has a Kdof 4.01 ± 0.50 nM. PET imaging and biodistribution showed a higher uptake of [89Zr]Zr-DFO-Ab253 in A375 melanomas than that in A549 tumors (42.1 ± 4.04% vs 7.87 ± 1.30% ID/g at 120 h, P< 0.05). A low tumor uptake of [89Zr]Zr-DFO-IgG was observed with uptakes of 1.91 ± 0.41 and 2.80 ± 0.14 ID%/g when blocked at 120 h. The radiation-absorbed dose was calculated to be 0.13 mSv/MBq. This study demonstrates the synthesis and preclinical evaluation of [89Zr]Zr-DFO-Ab253 and indicates that the novel tracer has promising applications in malignant melanoma-specific PET imaging because of its high uptake and long-time retention in malignant melanoma. It also provides feasibility for the development of integrated molecular probes for diagnosis and treatment based on the CD146 target.

In this study, the contact effects between mesophile bacteria and minerals were observed to enhance the bioleaching kinetics, which demonstrated that the adsorption of bacteria to mineral surfaces could improve the dissolution of arsenic and copper. The microstructure results also demonstrated that after the contact bioleaching, residue surfaces were rougher and with more corrosion bars and pits. Compared to contact oxidation approach, ferric ions, acting as the only oxidants in the non-contact bioleaching process, play a more important role in the copper extraction and arsenic dissolution, which is consistent with the previous works about indirect leaching mechanism. Due to the presence of various mesophiles in the contact oxidation, their activities and corresponding preferences for energy sources influenced by temperature were observed, causing differences in the sulfides’ dissolution: ferrous ions were inclined to be oxidized biologically at 30 °C, whereas sulfide minerals, including enargite, were preferentially oxidized at 45 °C.

The main challenge for fine-grained few-shot image classification is to learn feature representations with higher inter-class and lower intra-class variations, with a mere few labelled samples. Conventional few-shot learning methods however cannot be naively adopted for this fine-grained setting – a quick pilot study reveals that they in fact push for the opposite (i.e., lower inter-class variations and higher intra-class variations). To alleviate this problem, prior works predominately use a support set to reconstruct the query image and then utilize metric learning to determine its category. Upon careful inspection, we further reveal that such unidirectional reconstruction methods only help to increase inter-class variations and are not effective in tackling intra-class variations. In this paper, we introduce a bi-reconstruction mechanism that can simultaneously accommodate for inter-class and intra-class variations. In addition to using the support set to reconstruct the query set for increasing inter-class variations, we further use the query set to reconstruct the support set for reducing intra-class variations. This design effectively helps the model to explore more subtle and discriminative features which is key for the fine-grained problem in hand. Furthermore, we also construct a self-reconstruction module to work alongside the bi-directional module to make the features even more discriminative. We introduce the snapshot ensemble method in the episodic learning strategy – a simple trick to further improve model performance without increasing training costs. Experimental results on three widely used fine-grained image classification datasets, as well as general and cross-domain few-shot image datasets, consistently show considerable improvements compared with other methods.

• A cyano-modified g-C3N4/TiO2 heterojunction film was successfully constructed;. • The heterojunction film could effectively degrade NOR over different reaction parameters;. • The possible photocatalytic degradation pathway of NOR was investigated;. • S-scheme mechanism was investigated via DFT and selective photo-deposition experiment. Developing highly efficient and recyclable photocatalysts has been regarded as an attractive strategy to solve antibiotic contaminants. Herein, we designed and fabricated Cy-C 3 N 4 /TiO 2 S-scheme heterojunction film with boosted charge transfer and a highly hydrophilic surface. The as-prepared heterojunction exhibited outstanding removal efficiency on tetracyclines and fluoroquinolone antibiotics (more than 80 % within 90 min). The removal rate of 300-Cy-C 3 N 4 /TiO 2 on norfloxacin (NOR) was 2.12, and 1.59 times higher than that of pristine TiO 2 , C 3 N 4 /TiO 2 , respectively. The excellent photocatalytic performance of 300-Cy-C 3 N 4 /TiO 2 was attributed to the highly hydrophilic surface and effective transfer and separation of carriers. Moreover, the NOR degradation pathways were proposed based on the results of density functional theory (DFT), and liquid chromatography-mass spectrometry. The toxicity assessment indicated the toxicity of intermediates can be remarkably alleviated. The DFT calculation and selective photo-deposition experiment demonstrated that an internal electric field was formed at the heterojunction interface, and the charge carriers migrated between Cy-C 3 N 4 and TiO 2 following an S-scheme transfer pathway. This research not only provides a promising method for tracking charge distribution on thin-film heterojunction photocatalysts but also helps us to design high-efficiency, and recyclable heterojunctions to solve antibiotic contaminants. Novel S-scheme heterojunction of cyano-modified C 3 N 4 /TiO 2 film for efficient photocatalytic norfloxacin degradation [Display omitted] [ABSTRACT FROM AUTHOR]

Graphical Abstract:

A visible-light-induced photoredox three-component carbocyclization reaction of 1,7-enynes with sulfoxonium ylides and water is reported. The protocol provides a facile entry to structurally valuable highly functionalized cyclopenta[c]quinoline scaffolds in a highly chemoselective and stereoselective manner. Salient features of this method include facile redox-neutral conditions, no requirement of base or other additive, and good functional-group tolerance.

Synthetic α-galactosylceramide (αGalCer) and its analogues as powerful agonists for natural killer T (NKT) cell manipulation have received significant attention in immunotherapy and adjuvant development. However, identifying new potent NKT cell agonists, especially those with Th1 selectivity that promote anticancer effects, remains a challenging task. In this work, we introduced a sulfonamide group into the acyl chain of αGalCer to form additional hydrogen bonds to intensify the glycolipid/CD1d interaction. Two compounds GCS-11and GCS-12demonstrated remarkable potency while exhibiting different cytokine induction patterns. Compared to αGalCer, the Th1-biased GCS-11exhibited a 6-fold increase in IFN-γ but not IL-4, while the Th1/2-balanced GCS-12elicited 7- and 5-fold increase in IFN-γ and IL-4, respectively, in vivo. These findings place them among the most potent NKT cell agonists, with superior antitumor effects. Therefore, hydrogen-bond-involved derivatization could be a powerful strategy to develop potent and polarized NKT cell agonists for various immunotherapies.

A copper-catalyzed three-component coupling reaction of styrene oxide, aryl iodide, and carbon disulfide for the construction of β-hydroxysulfides has been developed. In this process, readily available CS2was used as the sulfur source to construct C–S bonds for the synthesis of phenyl-β-hydroxysulfides and (benzo[d]thiazol)-β-hydroxysulfides. This process features mild reaction conditions, simple operation, and wide substrate scope (>50 examples).

Anti-Program-Death-1 (PD-1) is a standard adjuvant therapy for patients with resected melanoma. We hypothesized that there are discrepancies in survival, recurrence pattern and toxicity to adjuvant PD-1 between different ethnicities and melanoma subtypes.

Iron metabolism plays a crucial role in cell viability, but its relationship with adult stem cells and cancer stem cells is not fully understood. The ferritin complex, responsible for intracellular iron storage, is important in this process. We report that conditional deletion of ferritin heavy chain 1 (Fth1) in the hematopoietic system reduced the number and repopulation capacity of hematopoietic stem cells (HSCs). These effects were associated with a decrease in cellular iron level, leading to impaired mitochondrial function and the initiation of apoptosis. Iron supplementation, antioxidant, and apoptosis inhibitors reversed the reduced cell viability of Fth1-deleted hematopoietic stem and progenitor cells (HSPCs). Importantly, leukemic stem cells (LSCs) derived from MLL-AF9-induced acute myeloid leukemia (AML) mice exhibited reduced Fth1expression, rendering them more susceptible to apoptosis induced by the iron chelation compared to normal HSPCs. Modulating FTH1 expression using mono-methyl fumarate increased LSCs resistance to iron chelator-induced apoptosis. Additionally, iron supplementation, antioxidant, and apoptosis inhibitors protected LSCs from iron chelator-induced cell death. Fth1deletion also extended the survival of AML mice. These findings unveil a novel mechanism by which ferritin-mediated iron homeostasis regulates the survival of both HSCs and LSCs, suggesting potential therapeutic strategies for blood cancer with iron dysregulation.

A strategy for the synthesis of α-carboline derivatives from indole-3-carboxaldehydes and 3-aminocyclohex-2-enones under metal-free conditions has been developed. The combination use of phenyliodine (III) diacetate (PIDA) and benzoic acid could significantly facilitate the corresponding [3 ​+ ​3] annulation process. This newly developed strategy featured unextraordinary chemoselectivity, good functional group tolerance and the preservation of the carbonyl group of the ketone substrates, which offers the possibility for further transformation of the products.

Weak antigens represented by MUC1 are poorly immunogenic, which greatly constrains the development of relevant vaccines. Herein, we developed a multifunctional lipidated protein as a carrier, in which the TLR1/2 agonist Pam3CSK4was conjugated to the N-terminus of MUC1-loaded carrier protein BSA through pyridoxal 5'-phosphate-mediated transamination reaction. The resulting Pam3CSK4–BSA-MUC1 conjugate was subsequently incorporated into liposomes, which biomimics the membrane structure of tumor cells. The results indicated that this lipidated protein carrier significantly enhanced antigen uptake by APCs and obviously augmented the retention of the vaccine at the injection site. Compared with the BSA-MUC1 and BSA-MUC1 + Pam3CSK4groups, Pam3CSK4–BSA-MUC1 evoked 22- and 11-fold increases in MUC1-specific IgG titers. Importantly, Pam3CSK4–BSA-MUC1 elicited robust cellular immunity and significantly inhibited tumor growth. This is the first time that lipidated protein was constructed to enhance antigen immunogenicity, and this universal carrier platform exhibits promise for utilization in various vaccines, holding the potential for further clinical application.

A selective three-component 1,2-sulfonyl etherification of aryl 1,3-dienes enabled by copper catalysis to afford biologically interesting alkenyl 1,2-sulfone ether derivatives through C–S and C–O bond formation is described. The protocol proceeds with the sulfonyl chloride and alcohols under simple, mild, and base-free conditions, providing a straightforward route to sulfonylated allyl ether compounds with broad functional group tolerance and excellent chemo- and regioselectivity. Mechanistic studies indicate that the selective alkene difunctionalization includes a key copper-mediated single-electron transfer process.

The relationship between support and surrounding rock is of great significance to the control of surrounding rock in mining process. In view of the fact that most of the existing numerical simulation methods construct virtual elements and stress servo control to approximately replace the hydraulic support problem, this paper establishes a new numerical model of hydraulic support with the same working characteristics as the actual hydraulic support by integrating numerical simulation software Rhino, Griddle and FLAC3D, which can realize the simulation of different working conditions. Based on this model, the influence mechanism of the supporting strength of hydraulic support on surrounding rock stress regulation and coal stability in front of the top coal caving face in extra thick coal seam were researched. Firstly, under different support intensity, the abutment pressure of the bearing coal and the coal in front of it presents the “three-stage” evolution characteristics. The influence range of support intensity is 15%–30%. Secondly, 1.5 MPa is the upper limit of impact that the support strength can have on the front coal failure area. Thirdly, within a displacement range of 2.76 m from the coal wall, a support strength of 1.5 MPa provides optimal control of the horizontal displacement of the coal.

Byline: Qiang. Shen, Neng. Wang, Pan-pan. Wu, Bi-bo. Tan, Guo-jun. Qian Purpose: To compare the therapeutic efficacy and safety of percutaneous microwave ablation (MWA) with those of percutaneous radiofrequency ablation [...]

ABSTRACT High strain hardening UHPC was expected to be self-healing due to its multiple micro-cracks in tension and the low water-to-binder ratio. The direct tensile tests with the acoustic emission [...]

Estrogen receptor α (ERα) is an important biomarker in breast cancer diagnosis and treatment. Sensitive and accurate detection of ERα protein expression is crucial in guiding selection of an appropriate therapeutic strategy to improve the effectiveness and prognosis of breast cancer treatment. Herein, we report a liquid-gated graphene field-effect transistor (FET) biosensor that enables rapid, sensitive, and label-free detection of the ERα protein by employing a novel drug molecule as a capture probe. The drug molecule was synthesized and subsequently immobilized onto the sensing surface of the fabricated graphene FET, which was able to distinguish the ERα-positive from the ERα-negative protein. The developed sensor not only demonstrated a low detection limit (LOD: 2.62 fM) but also achieved a fast response to ERα protein samples within 30 min. Moreover, depending on the relationship between the change of dirac point and the ERα protein concentrations, the dissociation constant (Kd) was estimated to be 7.35 ± 0.06 pM, indicating that the drug probe-modified graphene FET had a good affinity with ERα protein. The nanosensor was able to analyze ERα proteins from 36 cell samples lysates. These results show that the graphene FET sensor was able to differentiate between ERα-positive and ERα-negative cells, indicating a promising biosensor for the ultrasensitive and rapid detection of ERα protein without antibody labeling.

An acetic acid-promoted C(sp3)-H functionalization of 2-methyl quinoline, enaminoesters and elemental sulfur for the synthesis of 3,4,5-trisubstituted isothiazoles under metal-free conditions has been developed. This approach provides viable access to various 5-(quinolin-2-yl)isothiazoles in moderate to good yields with good functional group tolerance. Moreover, the success of the gram-scale reaction gives this reaction a great potential application.

The asymptotic model is applied to analyze the high-frequency electromagnetic coupling problem of the multiconductor transmission lines (MTLs). To efficiently calculate the current of MTLs in the nonuniform electromagnetic field, an extended asymptotic model combined with matrix pencil method (MPM) is proposed in this article. In the proposed method, the complicated electric field is analytically expressed using an MPM signal model first. Then, considering the basic theory of the moment of method (MOM), the previous solving process of the asymptotic model is optimized in this article to adapt to the requirements of multiple calculations. Finally, the asymptotic model is extended to calculate the current excited by the equivalent plane wave component of the signal model with a good efficiency and accuracy. Moreover, calculating the transient response by the inverse fast Fourier transform (IFFT), several numerical examples with typical nonuniform electromagnetic fields are presented to validate the reliability of the extended asymptotic model.

Pre-Cenozoic high-Mg andesites (HMAs) are mostly present in continental interiors, but their genetic relationship with continental lithosphere evolution remains unclear because of uncertainties of their mantle source, magmatic processes, and physicochemical conditions of formation. Early Cretaceous high-Mg dioritic rocks (HMDs, analogs of HMAs) of the Jinling complex in the Luxi area are typical intra-plate intrusions of the eastern North China Craton (NCC) and can be subdivided into two groups (Group-I and -II) on the basis of their petrographic and geochemical features. Group-I HMDs show low SiO2contents (52.47–56.10 wt%) and Sr/Y (34.5–39.6) and (La/Yb)N(10.3–13.6) ratios but high contents of MgO (7.86–9.13 wt%), Y (18.3–20.3 ppm), Yb (1.43–1.47 ppm), and compatible elements (Cr = 407–585 ppm; Ni = 117–216 ppm), classifying as sanukitic rocks. Group-II HMDs are characterized by high SiO2contents (63.81–64.87 wt%) and Sr/Y (47.1–63.4) and (La/Yb)N(16.1–17.5) ratios with low MgO (2.90–3.08 wt%), Y (0.88–1.04 ppm), Yb (0.88–1.04 ppm), and compatible elements (Cr = 201–213 ppm; Ni = 55–57 ppm) contents, belonging to adakitic rocks. Group-I and Group-II HMDs of the Jinling complex are closely related in spatial and temporal distribution, and all have enriched Sr-Nd isotopic compositions and arc-like trace element patterns with abundant hydrous minerals. Therefore, the Jinling HMDs should share a common source of ancient sub-continental lithospheric mantle that was metasomatized by aqueous fluids derived from the subducted Paleo-Pacific slab. The Jinling HMDs were not formed from interaction between slab-derived melts and mantle-wedge peridotites but were instead derived from partial melting of hydrous mantle peridotites in the continental interior of the eastern NCC. The distinctly different petrography, geochemistry, and mineralogy of the two groups of rocks resulted mainly from differing magmatic processes at crustal depths. Thus, Pre-Cenozoic intra-plate HMAs/HMDs are genetically distinct from Cenozoic HMAs that were mostly present in arc settings and generally represent juvenile crust growth. In a way, Archean tonalitic-trondhjemiticgranodioritic rocks (TTG) and sanukitoids, geochemically similar to HMAs/HMDs, could also be derived from interaction between slab-derived melts and mantle-wedge peridotites in arc settings or partial melting of hydrous mantle peridotites in continental interiors, and thus might not always be related with continental crustal growth and the onset of plate subduction.

It remains a tremendous challenge to achieve high-efficiency bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) for hydrogen production by water splitting. Herein, a novel hybrid of 0D nickel nanoparticles dispersed on the one-dimensional (1D) molybdenum carbide micropillars embedded in the carbon layers (Ni/Mo2C@C) was successfully prepared on nickel foam by a facile pyrolysis strategy. During the synthesis process, the nickel nanoparticles and molybdenum carbide were simultaneously generated under H2and C2H2mixed atmospheres and conformally encapsulated in the carbon layers. Benefiting from the distinctive 0D/1D heterostructure and the synergistic effect of the biphasic Mo2C and Ni together with the protective effect of the carbon layer, the reduced activation energy barriers and fast catalytic reaction kinetics can be achieved, resulting in a small overpotential of 96 mV for the HER and 266 mV for the OER at the current density of 10 mA cm–2together with excellent durability in 1.0 M KOH electrolyte. In addition, using the developed Ni/Mo2C@C as both the cathode and anode, the constructed electrolyzer exhibits a small voltage of 1.55 V for the overall water splitting. The novel designed Ni/Mo2C@C may give inspiration for the development of efficient bifunctional catalysts with low-cost transition metal elements for water splitting.

Tip leakage flow (TLF) trajectory in a pump with gas entrainment is investigated via visualization experiments and numerical simulations. Starting position of tip leakage vortex (TLV) is determined accurately by numerical simulation. Under high liquid flow rate (Ql) and high inlet gas volume fraction (IGVF) conditions, TLF flows from suction surface to pressure surface near the leading edge of blade, and the direction of TLF gradually changes along the chord which flows from pressure surface to suction surface near the tailing edge. The angle between TLF and blade mean camberline increases progressively as either Qlor IGVF decreases, and starting position of TLV moves towards leading edge direction. As Qlor IGVF decreases, value of vorticity increases and high vorticity region moves towards leading edge. The entropy production rate at blade tip clearance is high, and entropy diffuses from pressure surface to suction surface due to jet flow in blade tip clearance. The greater the amount of accumulated gas there is, the greater the amount of entropy in the area. In addition, when gas is entrained in pump, there are many low frequency fluctuations generated in blade tip clearance.

Phosphonate and phosphate prodrugs are integral to enhancing drug permeability, but the potential toxicity of their metabolites requires careful consideration. This study evaluates the impact of widely used phosphoramidate, bis-amidate, and cycloSal phosph(on)ate prodrug metabolites on BxPC3 pancreatic cancer cells, GL261-Luc glioblastoma cells, and primary cultured mouse astrocytes. 1-Naphthol and 2-naphthol demonstrated the greatest toxicity. Notably, 2-naphthol exhibited an ED50of 21 μM on BxPC3 cells, surpassing 1-naphthol with an ED50of 82 μM. Real-time xCELLigence experiments revealed notable activity for both metabolites at a low concentration of 16 μM. On primary cultured mouse astrocyte cells, all prodrugs exhibited reduced viability at 128 to 256 μM after only 4 hours of exposure. A cell-type-dependent sensitivity to phosph(on)ate prodrug metabolites was evident, with normal cells showing greater susceptibility than corresponding tumour cells. The results suggest it is essential to consider the potential cytotoxicity of phosph(on)ate prodrugs in the drug design and evaluation process.

The N-vehicle exploration problem (NVEP) is a nonlinear discrete scheduling problem, and the complexity status remains open. To our knowledge, there is no literature until now employing mixed integer linear programming (MILP) technology to solve this problem except for Wang (J Oper Res Soc China 3(4):489–498, 2015). However, they did not give numerical experiments since their model existed strictly inequalities and the number of constraints was up to O(n3), which was inefficient to solve practical problems. This paper establishes a more concise MILP model, where the number of constraints is just O(n2). Therefore, the existing efficient MILP algorithms can be used to solve NVEP. Secondly, we provide some properties of N-vehicle problem and give three methods for cutting plane construction, which can increase the solving speed significantly. Finally, a numerical experiment is provided to verify the effectiveness and robustness for different instances and scales of acceleration techniques.

Transmission lines are very important in electrical systems. High-frequency electromagnetic fields can couple to overhead lines. Once the wavelength of the high-frequency electromagnetic field is smaller than the height of the transmission line, the classic transmission line theory is no longer applicable. Although the traditional full-wave numerical algorithm can solve this problem, it is not efficient. Moreover, transmission lines often have multiple vertical ends and complex line layouts. In order to solve these problems, this article proposes a theoretical and effective method to solve the coupling of high-frequency electromagnetic fields with partial discontinuity transmission lines with scatterers in the presence of lossy ground. The asymptotic method with high computational efficiency is adopted, and the concept of scatterer is brought into the asymptotic method to consider more complex circuit structures. Numerical examples verify the accuracy and efficiency of the proposed method.

An approach based on film buckling under simple uniaxial tensile testing was utilized in this paper to quantitatively estimate the interfacial energy of the nanostructured multilayer films (NMFs) adherent to flexible substrates. The interfacial energies of polyimide-supported NMFs are determined to be ~5.0 J/m2for Cu/Cr, ~4.1 J/m2for Cu/Ta, ~2.8 J/m2for Cu/Mo, ~1.1 J/m2for Cu/Nb, and ~1.2 J/m2for Cu/Zr NMFs. Furthermore, a linear relationship between the adhesion energy and the interfacial shear strength is clearly demonstrated for the Cu-based NMFs, which is highly indicative of the applicability and reliability of the modified models.

Federated learning (FL) allows multiple clients to collaboratively learn a globally shared model through cycles of model aggregation and local model training, without the need to share data. Most existing FL methods train local models separately on different clients, and then simply average their parameters to obtain a centralized model on the server side. However, these approaches generally suffer from large aggregation errors and severe local forgetting, which are particularly bad in heterogeneous data settings. To tackle these issues, in this paper, we propose a novel FL framework that uses online Laplace approximation to approximate posteriors on both the client and server side. On the server side, a multivariate Gaussian product mechanism is employed to construct and maximize a global posterior, largely reducing the aggregation errors induced by large discrepancies between local models. On the client side, a prior loss that uses the global posterior probabilistic parameters delivered from the server is designed to guide the local training. Binding such learning constraints from other clients enables our method to mitigate local forgetting. Finally, we achieve state-of-the-art results on several benchmarks, clearly demonstrating the advantages of the proposed method.

Purpose: This study aimed to evaluate the performance of 18F-MD-PSMA PET/CT in patients previously treated for prostate cancer by either surgery or therapy, but later relapsed biochemically.Methods: This retrospective study enrolled 213 patients in sequence previously treated for prostate cancer by either surgery or therapy, but later PSA relapsed. A total of 191 of these 213 patients were included in this analysis. All patients were biochemically relapsed after radical prostatectomy or therapy, had 18F-MD-PSMA PET/CT scan within 1 week, and were off hormonal therapy at the time of the scans. The new tracer was compared directly with 11C-choline in sensitivity.Results: In 3 patients, a side-by-side comparison between 18F-MD-PSMA and 11C-choline was performed, and it was found that the former was about 3 times more sensitive than the latter. The analysis of PET imaging using 18F-MD-PSMA in 191 relapsed patients showed that less than 10% of patients showed the disease limited in the prostate. Among the remote lesions, the number in decreasing order was bone, followed by lymph nodes and other organs. The maximal SUV in lesions in each patient followed an exponential decay, with SUV inclined to the lower end. The Gleason score measured at the diagnosis showed no correlation with the average number of lesions in each patient, the average maximal SUV values among this cohort of patients, and the PSA values measured at the time of PET imaging. The number of lesions observed in each patient has no correlation with the PSA value measured at the time of PET imaging. When PSA value was measured as an independent biomarker at the time of PET imaging, the positivity of PET imaging using 18F-MD-PSMA increased along with an increase in PSA value, but with exceptions where PSMA expression was low or negative. From the PET imaging of this radioligand, the majority of patients showed oligo-metastasis, favoring using local therapy to manage the disease.Conclusion: An 18F-MD-PSMA as a radioligand was found to be superior to 11C-choline in the setting of patients with biochemical relapse after previous treatment. Its PET imaging results matched those of established PSMA radioligands, but its chemical structure was found to have added features to conjugate with other functional molecules, such as those with therapeutic properties. This radioligand lays the foundation for our further work.

Despite great strides made on fine-grained visual classification (FGVC), current methods are still heavily reliant on fully-supervised paradigms where ample expert labels are called for. Semi-supervised learning (SSL) techniques, acquiring knowledge from unlabeled data, provide a considerable means forward and have shown great promise for coarse-grained problems. However, exiting SSL paradigms mostly assume in-category (i.e., category-aligned) unlabeled data, which hinders their effectiveness when re-proposed on FGVC. In this paper, we put forward a novel design specifically aimed at making out-of-category data work for semi-supervised FGVC. We work off an important assumption that all fine-grained categories naturally follow a hierarchical structure (e.g., the phylogenetic tree of “Aves” that covers all bird species). It follows that, instead of operating on individual samples, we can instead predict sample relations within this tree structure as the optimization goal of SSL. Beyond this, we further introduced two strategies uniquely brought by these tree structures to achieve inter-sample consistency regularization and reliable pseudo-relation. Our experimental results reveal that (i) the proposed method yields good robustness against out-of-category data, and (ii) it can be equipped with prior arts, boosting their performance thus yielding state-of-the-art results.

The GRACE satellite mission provides a new approach for monitoring, tracking, and assessing drought conditions by detecting changes in Earth’s gravitational fields and inversing signals of terrestrial water storage anomalies. Existing studies of terrestrial water storage anomalies related droughts paid rare attention to the behind atmospheric physical mechanisms, nor quantified the risk propagation patterns between terrestrial water storage deficits and hydrological or agricultural droughts. In this study, we first extract terrestrial water storage (TWS) droughts, hydrological droughts, and agricultural droughts by using multiple variables including TWS from the GRACE/GRACE-FO satellites, runoff and soil moisture from the ERA5-Land reanalysis dataset. We then identify key atmospheric and oceanic oscillation indices affecting water deficits by employing machine learning technologies. We characterize the joint distributions between drought duration and severity by using the Copula function and quantify the risk propagation of hydrological and agricultural droughts to TWS droughts. The results show that: (1) From 2002 to 2021, there is a significant decrasing trend of TWS in China; the WPIO group atmospheric circulation indices (sea surface temperature index within the Western Pacific and Indian Ocean) contributes the most to TWS. Specifically, the sea surface temperature anomalies within the NINO 3.4 region as well as the Western Pacific Warm Pool area index show significantly positive correlation relationships with TWS in southern China; (2) The northwestern China, the Yangtze River basin, and the downstream of the Pearl River basin are the hotspots of TWS droughts. Besides, the hotspots of hydrological droughts locate in northwestern China and the hotspots of agricultural droughts locate in South China and eastern Tibetan Plateau; (3) The elastic coefficients of hydrological droughts propagating to TWS droughts are higher than those of agricultural droughts, indicating that the TWS droughts are more sensitive to hydrological droughts than to agricultural droughts.

Cu–Al/Al nanostructured metallic multilayers with Al layer thickness hAlvarying from 5 to 100 nm were prepared, and their mechanical properties and deformation behaviors were studied by nanoindentation testing. The results showed that the hardness increased drastically with decreasing hAldown to about 20 nm, whereafter the hardness reached a plateau that approaches the hardness of the alloyed Cu–Al monolithic thin films. The strain rate sensitivity (SRS, m), however, decreased monotonically with reducing hAl. The layer thickness-dependent strengthening mechanisms were discussed, and it was revealed that the alloyed Cu–Al nanolayers dominated at hAl≤ 20 nm, while the crystalline Al nanolayers dominated at hAl> 20 nm. The plastic deformation was mainly related to the ductile Al nanolayers, which was responsible for the monotonic evolution of SRS with hAl. In addition, the hAl-dependent hardness and SRS were quantitatively modeled in light of the strengthening mechanisms at different length scales.

The central dogma of modern biology underscores the pivotal roles proteins play in diverse biological processes, the study of which necessitates advanced methods to produce proteins with precision and versatility. Chemical protein synthesis, a powerful approach utilizing chemical reactions for the de novoconstruction of structurally accurate proteins, has emerged as a transformative tool for studying proteins and generating protein derivatives/mimics inaccessible by natural biological machinery, including post-translationally modified proteins, proteins comprised of unnatural amino acids, as well as mirror-image proteins. This review summarizes recent strides in synthetic method developments for chemical protein synthesis, including innovative techniques in solid-phase peptide synthesis, the challenges presented by difficult sequences in either synthesis or folding and the exploration of novel ligation reactions using both chemical and enzymatic methods. Furthermore, the review also delves into newly developed protocols for site-selective protein modifications and the generation of stapled or macrocyclized peptides/mini-proteins, highlighting the power of chemical methods to make structurally diverse proteins. Recent applications of synthetic proteins in investigating post-translational modifications (phosphorylation, lipidation, glycosylation, ubiquitination, etc.), mirror-image biological processes and drug development are further discussed. Together, these topics provide a comprehensive overview of the current landscape of chemical protein synthesis.

Unsupervised domain adaptation aims to leverage labeled data from a source domain to learn a classifier for an unlabeled target domain. Amongst its many variants, open set domain adaptation (OSDA) is perhaps the most challenging one, as it further assumes the presence of unknown classes in the target domain. In this paper, we study OSDA with a particular focus on enriching its ability to traverse across larger domain gaps, and we show that existing state-of-the-art methods suffer a considerable performance drop in the presence of larger domain gaps, especially on a new dataset (PACS) that we re-purposed for OSDA. Exploring this is pivotal for OSDA as with increasing domain shift, identifying unknown samples in the target domain becomes harder for the model, thus making negative transfer between source and target domains more challenging. Accordingly, we propose a Mutual-to-Separate (MTS) framework to address the larger domain gaps. Essentially we design two networks – (a) Sample Separation Network (SSN): which is trained to learn a hyperplane for separating unknown samples from known ones, and (b) Distribution Matching Network (DMN): which is trained to maximise domain confusion between source and target domains without unknown samples under the guidance of the SSN. The key insight lies in how we exploit the mutually beneficial information between these two networks. On closer observation, we see that SSN can reveal which samples in the target domain belong to the unknown class by instance weighting whereas, DMN pushes apart the samples that most likely belong to the unknown class in the target domain, which in turn reduces the difficulty of SSN in identifying unknown samples. It follows that (a) and (b) will mutually supervise each other and alternate until convergence, which can better align the source and target domains in the shared label space. Extensive experiments on five datasets (Office-31, Office-Home, PACS, VisDA, and $mini$ _DomainNet) demonstrate the efficiency of the proposed method. Detailed ablation experiments also validate the effectiveness of each component and the generality of the proposed framework. Codes are available at: https://github.com/PRIS-CV/Mutual-to-Separate.

In order to achieve ultra-low emissions of SO2and NOx, the oxygen blast furnace with sintering flue gas injection is presented as a promising novel process. The CO2emission was examined, and a cost analysis of the process was conducted. The results show that in the cases when the top gas is not circulated (Cases 1–3), and the volume of injected sintering flue gas per ton of hot metal is below about 1250 m3, the total CO2emissions decrease first and then increase as the oxygen content of the blast increases. When the volume of injected sintering flue gas per ton of hot metal exceeds approximately 1250 m3, the total CO2emissions gradually decrease. When the recirculating top gas and the vacuum pressure swing adsorption are considered, the benefits of recovered gas can make the ironmaking cost close to or even lower than that of the ordinary blast furnace. Furthermore, the implementation of this approach leads to a substantial reduction in total CO2emissions, with reductions of 69.13% (Case 4), 70.60% (Case 5), and 71.07% (Case 6), respectively. By integrating previous research and current findings, the reasonable oxygen blast furnace with sintering flue gas injection can not only realize desulfurization and denitrification, but also achieve the goal of reducing CO2emissions and ironmaking cost.

The use of efficient modification methods determines the wide application potential of zirconium salt coagulants. In this study, zirconium xerogel coagulants were prepared by acetylacetone regulation, and they exhibited application potential in a wider range of pH (pH = 5–9) and higher coagulation performance (residual turbidity < 2 NTU) than ZrCl4and PAC at a dosage of 0.2 mM. In addition, the acetylacetone-regulated xerogel coagulants were insensitive to changes in organic matter and were effective in removing turbidity even at high organic matter concentrations. The interaction mechanism between the zirconium xerogel coagulants and humic acid involving a complexation effect in the acidic environment and a sweeping effect in the alkaline environment has been proposed. The interpretation of this mechanism further revealed the “protective umbrella effect” of acetylacetone, which might work as a hydrolysis inhibitor to reduce the hydrolysis rate, as a chelating ligand to control the release of H+, and as a barrier to prevent organic matter from coming into direct contact with metal ions. These characteristics provide better stability, a higher effluent pH and higher turbidity removal. This study outlines the interaction mechanism of zirconium xerogel coagulants with humic acid and provides evidence for the contribution of acetylacetone in fabricating efficient gel coagulants.

This letter proposes a high-order probabilistic shaped (PS) system for joint source-channel coding (JSCC) using polar codes, which are employed for both source compression and channel coding. The modulation is based on a selection rule derived from the proposed bit classification distribution matching (BCDM) algorithm. An external binary random sequence is used to select and redundantly insert the codeword sequence, which makes the modulation symbol probability approach the Gaussian distribution, instead of being uniformly distributed as in the conventional constellation mapping. At the receiver, a joint belief propagation (JBP) decoder, which consists of a source and a channel BP decoder, is applied. Simulation results demonstrate that the proposed PS joint source-channel polar-coded modulation (PS-JSCPCM) system yields a significant enhancement to the bit error rate (BER) performance compared with the traditional unshaped joint source-channel code-modulation (JSCCM) system.

Background: Sacrococcygeal sinus ulcers are caused by pressure sores, trauma, or surgery. Several surgical techniques have been developed for its treatment; however, studies are ongoing to develop the ideal method. The present study aims to introduce an innovative application of gluteus maximus muscle flaps (GMMFs) packing combined with local random pattern skin flaps (RPSFs) in repairing sacrococcygeal sinus tracts (SSTs). Methods: This was a prospective analysis study conducted on the patients (n= 26) with SSTs underwent an innovative repairing surgery in Qilu Hospital of Shandong University, China between December 2015 and December 2020. The repairing surgery was GMMFs combined with RPSFs. The demographic information and the clinical parameters including operative time, postoperative healing time, and recurrence rate were used to evaluate the efficacy of the operation. Results: Except one case of partial necrosis at the edge of the flap due to severe fibrosis, which was cured after dressing change, all the other cases showed effective healing after the operation. Conclusion: The combined application of GMMFs and RPSFs for the treatment of sacrococcygeal sinus tracts gains the advantages of short operative time, quick postoperative recovery, and low postoperative recurrence rate.

The photoredox/PPh3-mediated cyclization of 2-isocyanobiaryls has been developed. A substantial range of functional-group-rich phenanthridine derivatives were synthesized at room temperature in a highly selective and atom-economic manner. Mechanistic studies suggested that the cyclization process is probably mediated both by Ph3P radical cation with key 1,2-hydride transfer and hydrogen atom generated through O–H bond homolytic cleavage of Ph3P–OH radical intermediate.

Nitrate/nitrite-dependent anaerobic oxidation of methane (n-DAMO) is a recently discovered process, which provides a sustainable perspective for simultaneous nitrogen removal and greenhouse gas emission (GHG) mitigation by using methane as an electron donor for denitrification. However, the engineering roadmap of the n-DAMO process is still unclear. This work constitutes a state-of-the-art review on the classical and most recently discovered metabolic mechanisms of the n-DAMO process. The versatile combinations of the n-DAMO process with nitrification, nitritation, and partial nitritation for nitrogen removal are also clearly presented and discussed. Additionally, the recent advances in bioreactor development are systematically reviewed and evaluated comprehensively in terms of methane supply, biomass retention, membrane requirement, startup time, reactor performance, and limitations. The key issues including enrichment and operation strategy for the scaling up of n-DAMO-based processes are also critically addressed. Moreover, the challenges inherent to implementing the n-DAMO process in practical applications, including application scenario recognition, GHG emission mitigation, and operation under realistic conditions, are highlighted. Finally, prospects as well as opportunities for future research are proposed. Overall, this review provides a roadmap for potential applications and further development of the n-DAMO process in the field of wastewater treatment.