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The characteristics and heterogeneity of coal pores are crucial for understanding the production mechanism of coalbed methane (CBM). In this study, coal samples with varying degrees of metamorphism (0.58% ≤ RO, max ≤ 3.44%) were collected. The characteristics of pore development and the heterogeneous properties of pores were revealed through low-temperature nitrogen adsorption (LTNA) and low-field nuclear magnetic resonance (NMR) experiments. The results indicate that pores with varying diameters exhibit favorable development in low-rank coals, along with favorable pores connectivity. The micropores composition of middle-rank coals was found to be 73.56%, however, the connectivity among transitional, meso, and macropores was observed to be poor. In high-rank coals, the proportion of micropores was 92.74%, with numerous micropores being closed or semi-closed. This resulted in inferior connectivity between micropores and transitional pores. As coal metamorphism progressed, the DL1 (characterizing the roughness of adsorption pores (AP) surface, ranging from 2.13 to 2.45) and DL2 (characterizing the complexity of AP structure, ranging from 2.56 to 2.77) initially decreased and then increased, whereas the DN (characterizing the heterogeneity of seepage pores (SP), ranging from 2.92 to 2.95) consistently improved. Furthermore, the roughness of pore surface and the complexity of pore structure in AP increased as the specific surface area and volume of pores increased. On the contrary, as the SP content increased, the uniformity of the pore structure improved. When the volume of SP remained constant, the complexity of the pore structure decreased due to increased pore connectivity.
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Traditional semiconductors are known to exhibit excellent electrical properties but oversized lattice thermal conductivities, thus limiting their thermoelectric performance. Herein, we have discovered a low-energy allotrope of those traditional semiconductors. Compared with the wurtzite structure, the lattice thermal conductivity is reduced by more than five times in the haeckelite structure. This is attributed to the softening of acoustic phonon modes and concurrently enhanced anharmonicity in the haeckelite structure. Benefiting from the suppressed lattice thermal conductivity while retaining the excellent electrical properties of wurtzite structure, haeckelite compounds have been proven to be a novel category of high-performance thermoelectric materials. As an excellent representative, haeckelite CdTe exhibits a peak figure of merit approaching 1.3 at n-type doping and high temperature, which experiences a 3-fold improvement compared with its wurtzite counterpart. This work provides an alternative pathway of engineering the lattice thermal conductivities of traditional semiconductors toward superior thermoelectric properties.
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Hampered by their susceptibility to nucleophilic attack and chemical bleaching, electron-deficient squaraine dyes have long been considered unsuitable for biological imaging. This study unveils a surprising twist: in aqueous environments, bleaching is not irreversible but rather a reversible spontaneous quenching process. Leveraging this new discovery, we introduce a novel deep-red squaraine probe tailored for live-cell super-resolution imaging. This probe enables single-molecule localization microscopy (SMLM) under physiological conditions without harmful additives or intense lasers and exhibits spontaneous blinking orchestrated by biological nucleophiles, such as glutathione or hydroxide anion. With a low duty cycle (â¼0.1%) and high-emission rate (â¼6 × 104 photons/s under 400 W/cm2), the squaraine probe surpasses the benchmark Cy5 dye by 4-fold and Si-rhodamine by a factor of 1.7 times. Live-cell SMLM with the probe reveals intricate structural details of cell membranes, which demonstrates the high potential of squaraine dyes for next-generation super-resolution imaging.
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Fluorescent probes are essential for single-molecule imaging. However, their application in biological systems is often limited by the short photobleaching lifetime. To overcome this, we developed a novel thiolation strategy for squaraine dyes. By introducing thiolation of the central cyclobutene of squaraine (thio-squaraine), we observed a ≈5-fold increase in photobleaching lifetime. Our single-molecule data analysis attributes this improvement to improved photostability resulting from thiolation. Interestingly, bulk measurements show rapid oxidation of thio-squaraine to its oxo-analogue under irradiation, giving the perception of inferior photostability. This discrepancy between bulk and single-molecule environments can be ascribed to the factors in the latter, including larger intermolecular distances and restricted mobility, which reduce the interactions between a fluorophore and reactive oxygen species produced by other fluorophores, ultimately impacting photobleaching and photoconversion rate. We demonstrate the remarkable performance of thio-squaraine probes in various imaging buffers, such as glucose oxidase with catalase (GLOX) and GLOX+trolox. We successfully employed these photostable probes for single-molecule tracking of CD56 membrane protein and monitoring mitochondria movements in live neurons. CD56 tracking revealed distinct motion states and the corresponding protein fractions. This investigation is expected to propel the development of single-molecule imaging probes, particularly in scenarios where bulk measurements show suboptimal performance.
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Ciclobutanos , Corantes Fluorescentes , Fotodegradação , Fenóis , IonóforosRESUMO
The 6-Degree-of-Freedom (6-DoF) robotic grasping is a fundamental task in robot manipulation, aimed at detecting graspable points and corresponding parameters in a 3D space, i.e affordance learning, and then a robot executes grasp actions with the detected affordances. Existing research works on affordance learning predominantly focus on learning local features directly for each grid in a voxel scene or each point in a point cloud scene, subsequently filtering the most promising candidate for execution. Contrarily, cognitive models of grasping highlight the significance of global descriptors, such as size, shape, and orientation, in grasping. These global descriptors indicate a grasp path closely tied to actions. Inspired by this, we propose a novel bio-inspired neural network that explicitly incorporates global feature encoding. In particular, our method utilizes a Truncated Signed Distance Function (TSDF) as input, and employs the recently proposed Transformer model to encode the global features of a scene directly. With the effective global representation, we then use deconvolution modules to decode multiple local features to generate graspable candidates. In addition, to integrate global and local features, we propose using a skip-connection module to merge lower-layer global features with higher-layer local features. Our approach, when tested on a recently proposed pile and packed grasping dataset for a decluttering task, surpassed state-of-the-art local feature learning methods by approximately 5% in terms of success and declutter rates. We also evaluated its running time and generalization ability, further demonstrating its superiority. We deployed our model on a Franka Panda robot arm, with real-world results aligning well with simulation data. This underscores our approach's effectiveness for generalization and real-world applications.
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Procedimentos Cirúrgicos Robóticos , Robótica , Aprendizagem , Generalização Psicológica , Simulação por ComputadorRESUMO
Dye-sensitization can enhance lanthanide-based upconversion luminescence, but is hindered by interfacial energy transfer from organic dye to lanthanide ion Yb3+ . To overcome these limitations, modifying coordination sites on dye conjugated structures and minimizing the distance between fluorescence cores and Yb3+ in upconversion nanoparticles (UCNPs) are proposed. The specially designed near-infrared (NIR) dye, disulfo-indocyanine green (disulfo-ICG), acts as the antenna molecule and exhibits a 2413-fold increase in luminescence under 808 nm excitation compared to UCNPs alone using 980 nm irradiation. The significant improvement is attributed to the high energy transfer efficiency of 72.1% from disulfo-ICG to Yb3+ in UCNPs, with majority of energy originating from triplet state (T1 ) of disulfo-ICG. Shortening the distance between the dye and lanthanide ions increases the probability of energy transfer and strengthens the heavy atom effect, leading to enhanced T1 generation and improved dye-triplet sensitization upconversion. Importantly, this approach also applies to 730 nm excitation Cy7-SO3 sensitization system, overcoming the spectral mismatch between Cy7 and Yb3+ and achieving a 52-fold enhancement in luminescence. Furthermore, the enhancement of upconversion at single particle level through dye-sensitization is demonstrated. This strategy expands the range of NIR dyes for sensitization and opens new avenues for highly efficient dye-sensitized upconversion systems.
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The ocean, covering 71% of the Earth's surface, is integral to human life [...].
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Upconversion nanoparticles (UCNPs) doped with lanthanides have limited brightness due to their small absorption cross section to light. However, using organic sensitizers can significantly enhance their light absorption ability. Unfortunately, the practical application of organic sensitizers has been hindered by poor stability and aggregation-caused quenching (ACQ). To address these issues, we developed a novel squaraine-based dye, SQ-739, for sensitizing upconversion luminescence (UCL). This dye has a maximum absorption at 739 nm, and shows 1 order of magnitude and 2-fold improved chemical- and photostability, compared to the commonly used cyanine-based dye IR-806, respectively. When SQ-739 is used to sensitize UCNPs, the resulting SQ-739-UCNPs exhibit excellent photostability and reduced ACQ in the presence of polar solvents. Moreover, at the single particle level, the SQ-739-UCNPs exhibit a 97-fold increase in UCL emission compared to bare UCNPs. This squaraine dye-based system represents a new design strategy for developing highly stable and efficient NIR upconversion probes.
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Atmospheric solids analysis probe-mass spectrometry (ASAP-MS), an ambient mass spectrometry technique, was used to differentiate spring and autumn Tieguanyin teas. Two configurations were used to obtain their chemical fingerprints - ASAP attached to a high-resolution quadrupole time-of-flight mass spectrometer (i.e., ASAP-QTOF) and to a single-quadrupole mass spectrometer (i.e., Radian™ ASAP™ mass spectrometer). Then, orthogonal projections to latent structures-discriminant analysis was conducted to identify features that held promise in differentiating harvest seasons. Four machine learning models - decision tree, linear discriminant analysis, support vector machine, and k-nearest neighbour - were built using these features, and high classification accuracy of up to 100% was achieved. The markers were putatively identified using their accurate masses and MS/MS fragmentation patterns from ASAP-QTOF. This approach was successfully transferred to the Radian ASAP MS, which is more deployable in the field. Overall, this study demonstrated the potential of ASAP-MS as a rapid fingerprinting tool for differentiating spring and autumn Tieguanyin.
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Espectrometria de Massas em Tandem , Estações do Ano , Análise Discriminante , Análise por ConglomeradosRESUMO
The influence mechanism of different geological parameters on the activation of small faults under mining in the deep coal face was investigated by numerical simulation. The study shows that (1) the degree of influence of six parameters including the fault lateral pressure coefficient λ, elastic modulus E, Poisson's ratio µ, cohesion c, internal friction angle φ, and fault inclination angle θ on the activation of small faults was ranked in order as θ > λ > φ > µ > E > c. (2) The lateral pressure coefficient λ of the fault zone rock mass, the internal friction angle φ, and the fault inclination angle θ had a great influence on the fault activation. The larger the λ of the fault zone rock mass was, the smaller the φ was, the larger the subsidence amount drop of the rock layers on both sides of the fault was, and the greater the severity of the fault activation was. The fault activation degree decreased first, then increased, and then decreased with the increase of θ. When θ was 15 and 60°, there was relatively severe fault activation. When θ was 75°, the fault was not easy to activate. (3) Poisson's ratio µ, elastic-modulus E, and cohesion c of the fault zone rock mass had little effect on the fault activation. The larger the E of the fault zone rock mass was, the larger the µ was, the smaller the c was, and the possibility of fault activation increased slightly. The research results can provide important theoretical support for the theoretical research on fault activation, on-site roof management, and mining schedule arrangement in the mining process of deep coal face.
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Acidizing technology is an important means to increase production in oil-gas reservoirs. In recent years, acidizing technology has been widely used to increase the permeability of coal seams to enhance gas extraction, where acidizing fluid is the key factor to determine the permeability improvement effect by acidizing technology. In order to clarify the influence of mixed acid fluid on the pore structure of high rank coal and seek the optimal mixed acid fluid suitable for acidizing and permeability improvement of high rank coal in the Jiaozuo coal mine area. Taking the Jiulishan Mine in the Jiaozuo mining area as an example, low field nuclear magnetic resonance (LFNMR) test and static dissolution test were conducted to obtain the T 2 spectrum, porosity, movable fluid saturation, pore throat distribution, nuclear magnetic permeability, and dissolution rate of coal samples before and after treatment with distilled water and three mixed acid fluids. On this basis, the influence of mixed acid fluid on the pore structure of high rank coal was analyzed and the optimal mixed acid fluid suitable for high rank coal was selected. The results showed that the pore size, number, and volume of all kinds of pore sizes of coal samples treated with distilled water all decreased, which was manifested by the decrease of effective porosity and nuclear magnetic permeability. After acidification, the proportion of micropore volume in coal decreased significantly, the number and proportion of pore volume of mesopores and macropore-microfractures increased significantly, and the connectivity between mesopores and macropore-microfractures was enhanced, which was characterized by the increase in effective porosity and nuclear magnetic permeability of coal samples. After acidification, the pore-throat ratio of adsorption pores of all coal samples decreased, while the pore-throat ratio of seepage pores increased. By comparatively analyzing the change law of pore structure of coal samples before and after acidizing with three kinds of mixed acid fluids, the optimal mixed acid fluid suitable for acidizing and permeability improvement of high rank coal in the Jiaozuo coal mine area was selected, which was 12%HCL +3%HF.
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Gas explosion is one of the main causes of casualties in coal mines. Studying the propagation law of shock wave of mine gas explosion can reduce the economic loss and personnel injury caused by mine gas explosion. To solve the difficulty in the research of shock wave propagation of gas explosion in the mine scale, the segmented relay simulation method of shock wave propagation of gas explosion in a coal mine was put forward, the related key problems were studied, and the results were successfully applied in Yangchangwan No. 2 Mine. The results show the following: (1) When the length of the forked roadway exceeds 50 m, the length of the forked roadway has little effect on the shock wave overpressure in the main roadway. When the length of the forked roadway is short, the closure of the forked roadway has a great influence on the change curve of the shock wave overpressure in the main roadway. Therefore, the length of the bifurcation roadway should not be less than 50 m in numerical simulation. (2) The angle of the bifurcated roadway has a great influence on the shock wave propagation of explosion in the main roadway. With the increase in the angle of the bifurcated roadway, the overpressure in the main roadway tends to increase at first and then decrease, and the peak overpressure is the highest when the angle of the bifurcated roadway is 90°. (3) The influence range of the roadway pressure-outlet boundary is about 5 m, and the dynamic parameter monitoring point should be set at about 10 m away from the pressure outlet; dynamic boundary monitoring parameters should include static pressure, dynamic pressure, and temperature. (4) When the gas explosion occurs in the heading face, the shock wave will cause great damage to the adjacent heading face. When the shock wave reaches the head-on and upper corner of the heading face, it will be reflected violently, which will cause the local overpressure to rise obviously. The peak overpressure and gas accumulation length conform to the logarithmic function.
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Single molecule localization microscopy based on photoactivation is a powerful tool for investigating the ultrastructure of cells. We developed a general strategy for photoactivatable fluorophores, using 2,3-dihydro-1,4-oxathiine group (SO) as a tag to attach to various skeletal structures, including coumarin, BODIPY, rhodamine, and cyanine. The conjugation of SO resulted in a significant loss of fluorescence due to photoinduced electron transfer (PeT). Under the irradiation of excitation light, singlet oxygen generated by the fluorophores converted the SO moiety into its ester derivative, terminated the PeT process, and restored the fluorescence. Single molecule localization imaging was achieved using a dual functional illuminating beam in the visible, acting as both the activating and the exciting source. We successfully applied these photoactivatable probes for time-lapse super-resolution tracking in living cells and super-resolution imaging of microtubule structures in neurons.
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Corantes Fluorescentes , Imagem Individual de Molécula , Microscopia de Fluorescência/métodos , Imagem Individual de Molécula/métodos , Corantes Fluorescentes/química , Rodaminas/química , IonóforosRESUMO
Tieguanyin oolong tea (TOT), a semi-oxidized tea originating from Anxi county in China, is categorized into jade TOT, medium-baked TOT, and deep-baked TOT, based on different baking processes. To study the effects of baking, chemical analysis, sensory evaluation, and bioactivity assessments of the three TOTs were conducted. The results indicated that the baking process promoted the formation of colored macromolecules (e.g., theabrownins), which affected the color of tea infusion. Free amino acids underwent the Maillard reaction and generated specific Maillard reaction products, such as 5-hydroxymethylfurfural and furfural, which modified the taste and aroma. Floral and fresh volatiles were remarkably reduced, while multiple new volatiles were produced, forming a typically baked aroma. The antioxidant activity and antibacterial activity were reduced after baking, which might be associated with the decrease of monomeric catechins. These results provide a scientific basis for understanding the changes caused by the baking process.
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A new boric agent with bridged structure, boric acid D, was first synthesized and used as an excellent chiral derivative agent for highly efficient enantiodiscrimination of various diols. The derivatization reaction is fast and complete, easy to operate and has high accuracy in measurement of ee values. The characteristic split NMR signals are well-distinguishable with a large chemical shift nonequivalence (up to 0.39 ppm).
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Tieguanyin is one of the most consumed oolong teas because of its distinctive flavor. The brewing process is crucial for the flavor performance of traditional teas, thus the effects of brewing conditions, including water/tea ratio (R), brewing temperature (T), and time (S) on the sensory traits, chemical composition, and antioxidant activity of Tieguanyin tea infusion were investigated using quadratic orthogonal regression design. Results showed that R affected all the quality variables most, its reduction could lead to the promotion of tea infusion concentration, antioxidant activity, and taste intensity, which was favored by the tea consumers drinking tea almost daily (DTD) but unacceptable for those drinking tea hardly (DTH). Based on the optimization of brewing conditions in response surface methodology (RSM), we recommended several brewing schemes for diverse consume goals: R = 34 mL/g, T = 80 °C, S = 80 s for DTH; R = 39 mL/g, T = 100 °C, S = 127 s for DTO (the consumers drinking tea occasionally); R = 20 mL/g, T = 100 °C, S = 100 s for DTD; R = 26 mL/g, T = 100 °C and S = 127 s for the common consumers seeking for flavor and health benefits. These results would be helpful for tea consumers with multiple demands.
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A simple chiral binuclear titanium complex ((S)-Ti2L3Na4) was first prepared and served as an excellent chiral sensor for discriminating a variety of chiral ammoniums by 1H NMR. In the presence of trifluoroacetic acid, the in-situ-generated ammoniums of varied amines can be effectively resolved by (S)-Ti2L3Na4. The different binding forces between (S)-Ti2L3Na4 and two enantiomers of analytes generate different shielding effects on two enantiomers, resulting in a split in the distinguishable chemical shift.
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BACKGROUND: Despite potential for improving patient outcomes, studies using three-dimensional measurements to quantify proximal tibial sclerotic bone and its effects on prosthesis stability after total knee arthroplasty (TKA) are lacking. Therefore, this study aimed to determine: (1) the distribution range of tibial sclerotic bone in patients with severe genu varum using three-dimensional measurements, (2) the effect of the proximal tibial sclerotic bone thickness on prosthesis stability according to finite-element modelling of TKA with kinematic alignment (KA), mechanical alignment (MA), and 3° valgus alignment, and (3) the effect of short extension stem augment utilization on prosthesis stability. METHODS: The sclerotic bone in the medial tibial plateau of 116 patients with severe genu varum was measured and classified according to its position and thickness. Based on these cases, finite-element models were established to simulate 3 different tibial cut alignments with 4 different thicknesses of the sclerotic bone to measure the stress distribution of the tibia and tibial prosthesis, the relative micromotion beneath the stem, and the influence of the short extension stem on stability. RESULTS: The distribution range of proximal tibial sclerotic bone was at the anteromedial tibial plateau. The models were divided into four types according to the thickness of the sclerotic bone: 15 mm, 10 mm, 5 mm, and 0 mm. The relative micromotion under maximum stress was smallest after MA with no sclerotic bone (3241 µm) and largest after KA with 15 mm sclerotic bone (4467 µm). Relative micromotion was largest with KA and smallest with MA in sclerotic models with the same thickness. Relative micromotion increased as thickness of the sclerotic bone increased with KA and MA (R = 0.937, P = 0.03 and R = 0.756, P = 0.07, respectively). Relative micromotion decreased with short extension stem augment in the KA model when there was proximal tibial sclerotic bone. CONCLUSIONS: The influence of proximal tibial sclerotic bone on prosthesis's stability is significant, especially with KA tibial cut. Tibial component's short extension stem augment can improve stability.
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Genu Varum/cirurgia , Prótese do Joelho , Osteoartrite do Joelho/cirurgia , Osteosclerose/diagnóstico por imagem , Tíbia/diagnóstico por imagem , Idoso , Artroplastia do Joelho , Feminino , Análise de Elementos Finitos , Genu Varum/complicações , Humanos , Imageamento Tridimensional , Masculino , Pessoa de Meia-Idade , Osteoartrite do Joelho/complicações , Osteosclerose/etiologia , Falha de Prótese , Tíbia/cirurgiaRESUMO
In this paper, we introduce a novel sub-bottom profiler, making good use of the Mills cross configuration of multibeam sonar and synthetic aperture techniques of the synthetic aperture sonar system. The receiver array is mounted along the ship keel, while the transmitter array is mounted perpendicular to the receiver array. With the synthetic aperture technique, the along-track resolution can be greatly improved. The system often suffers from motion error, which severely degrades the imaging performance. To solve this problem, the imaging algorithm with motion compensation (MC) is proposed. With the presented method, the motion error is first estimated based on overlapped elements between successive pulses. Then, the echo data is processed by using the range migration algorithm based on the phase center approximation (PCA) method, which simultaneously performs the MC with the estimated motion error. In order to validate the proposed sub-bottom profiler and data processing method, some simulations and lake trial results are discussed. The processing results of the real data further indicate that the presented configuration has great potential to find buried objects in seabed sediments.
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An axially chiral binuclear µ-hydroxo Pd complex (BPHP) first served as an excellent chiral sensor for discriminating a variety of analytes including amino alcohol, amino amide, amino acid, mandelic acid, diol, diamine, and monoamine by 31P{1H} NMR. A detailed recognition mechanism was proposed based on the single crystal and mass spectrum of Pd-complexes. In general, BPHP sensor, through extracting the acidic hydrogen of an analyte by its Pd-OH group, forms stable diastereomeric complexes with two enantiomers of the analyte giving well distinguishable split 31P{1H} NMR signals for chiral discrimination.