Enhanced Electrocatalytic Water Oxidation by Interfacial Phase Transition and Photothermal Effect in Multiply Heterostructured Co9S8/Co3S4/Cu2S Nanohybrids

The rational design of advanced nanohybrids (NHs) with optimized interface electronic environment and rapid reaction kinetics is pivotal to electrocatalytic schedule. Herein, we developed a multiple heterogeneous Co₉S₈/Co₃S₄/Cu₂S nanoparticle in which Co₃S₄ germinates between Co₉S₈ and Cu₂S. Using high-angle annular-dark-field imaging and theoretical calculation, it was found that the integration of Co₉S₈ and Cu₂S tends to trigger the interface phase transition of Co₉S₈, leading to Co₃S₄ interlayer due to the low formation energy of Co₃S₄/Cu₂S (−7.61 eV) than Co₉S₈/Cu₂S (−5.86 eV). Such phase transition not only lowers the energy barrier of oxygen evolution reaction (OER, from 0.335 eV to 0.297 eV), but also increases charge carrier density (from 7.76×10¹⁴ to 2.09×10¹⁵ cm⁻³), and creates more active sites. Compared to Co₉S₈ and Cu₂S, the Co₉S₈/Co₃S₄/Cu₂S NHs also demonstrate notable photothermal effect that can heat the catalyst locally, offset the endothermic enthalpy change of OER, and promote carrier migrate, reaction intermediates adsorption/deprotonation to improve reaction kinetics. Profiting from these favorable factors, the Co₉S₈/Co₃S₄/Cu₂S catalyst only requires an OER overpotential of 181 mV and overall water splitting cell voltage of 1.43 V to driven 10 mA cm⁻² under the irradiation of near-infrared light, outperforming those without light irradiation and many reported Co-based catalysts.     

Improving Low-temperature Performance and Stability of Na2Ti6O13 Anodes by the Ti−O Spring Effect through Nb-doping

Na₂Ti₆O₁₃ (NTO) with high safety has been regarded as a promising anode candidate for sodium-ion batteries. In the present study, integrated modification of migration channels broadening, charge density re-distribution, and oxygen vacancies regulation are realized in case of Nb-doping and have obtained significantly enhanced cycling performance with 92 % reversible capacity retained after 3000 cycles at 3000 mA g⁻¹. Moreover, unexpected low-temperature performance with a high discharge capacity of 143 mAh g⁻¹ at 100 mA g⁻¹ under −15 °C is also achieved in the full cell. Theoretical investigation suggests that Nb preferentially replaces Ti3 sites, which effectively improves structural stability and lowers the diffusion energy barrier. What's more important, both the in situ X-ray diffraction (XRD) and in situ Raman furtherly confirm the robust spring effect of the Ti−O bond, making special charge compensation mechanism and respective regulation strategy to conquer the sluggish transport kinetics and low conductivity, which plays a key role in promoting electrochemical performance.     

A Subtle Change in the Flexible Achiral Spacer Does Matter in Supramolecular Chirality: Two-Fold Odd-Even Effect in Polymer Assemblies

Precise control over the chirality and morphologies of polymer assemblies, a remaining challenge for both chemists and materials scientists, is receiving ever-increasing attention in the recent years. Herein, we report the subtle manipulation of the achiral spacers from the chiral stereocenter to the azobenzene (Azo) unit, of which the chiroptical consistency or chiroptical inversion of self-assemblies could be successfully controlled and present “two-fold” odd-even effect. Furthermore, morphological transitions from 0D spherical micelles, 1D worms, and nanowires to 3D vesicles, spindle- and dumbbell-shaped vesicles were also unexpectedly found to exhibit odd-even correlations. These observations were collectively elucidated by mesomorphic properties, stacking modes, chiroptical dynamics, and stimuli-responsive behaviors. Negligible modifications to the spacer structures can enable remarkable modulation of supramolecular chirality and anisotropic topologies in polymer assemblies, which is of great significance for the design of complex chiral functional polymers.     

On the role of a torsion‐like field in a scenario for the Spin Hall Effect

Starting from a field theory action that describes a Dirac fermion, we propose and analyze a model based on a low‐relativistic Pauli equation coupled to a torsion‐like term to study Spin Hall Effect (SHE). We point out a very particular connection between the modified Pauli equation and the (SHE), where what we refer to torsion as field playing an important role in the spin‐orbit (SO) coupling process. In this scenario, we present a proposal of a spin‐type current, considering the tiny contributions of torsion in connection with intrinsic anisotropy of the crystal electric field.     

Statistically and Computationally Efficient Estimating Equations for Large Spatial Datasets

For Gaussian process models, likelihood-based methods are often difficult to use with large irregularly spaced spatial datasets, because exact calculations of the likelihood for n observations require O(n³) operations and O(n²) memory. Various approximation methods have been developed to address the computational difficulties. In this article, we propose new, unbiased estimating equations (EE) based on score equation approximations that are both computationally and statistically efficient. We replace the inverse covariance matrix that appears in the score equations by a sparse matrix to approximate the quadratic forms, then set the resulting quadratic forms equal to their expected values to obtain unbiased EE. The sparse matrix is constructed by a sparse inverse Cholesky approach to approximate the inverse covariance matrix. The statistical efficiency of the resulting unbiased EE is evaluated both in theory and by numerical studies. Our methods are applied to nearly 90,000 satellite-based measurements of water vapor levels over a region in the Southeast Pacific Ocean.     

结合NSDTCT和稀疏表示的遥感图像融合

为了提高全色图像与多光谱图像的融合质量,提出一种基于非下采样双树复轮廓波变换和稀疏表示的图像融合算法.对多光谱图像进行亮度-色度-饱和度变换,再对亮度分量和全色图像进行直方图匹配及亮度平滑滤波处理.利用非下采样双树复轮廓波变换处理亮度分量和全色图像,得到对应的高低频系数.对于低频系数,利用稀疏表示进行融合,采用空间频率和l1范数双指标取大的融合规则得到稀疏表示系数;对于高频系数,将改进的拉普拉斯能量和作为脉冲耦合神经网络的外部输入项,提出了改进的脉冲耦合神经网络的融合策略.最后进行非下采样双树复轮廓波逆变换和亮度-色度-饱和度逆变换得到融合结果.实验结果表明,该算法最大限度地保留光谱信息的同时可以提高空间分辨率,视觉效果及客观指标均优于经典的融合算法.     

基于半监督稀疏多流形嵌入的高光谱影像分类

提出了一种半监督稀疏多流形嵌入方法,并应用于高光谱影像分类.该方法充分利用少量标记和大量无标记样本,采用稀疏表示方法得到样本的稀疏系数,并选取来自同一流形的点作为近邻点,然后构建相似图来表征多流形结构,得到样本在每个流形上低维鉴别特征,增加来自同一流形的数据点聚集性,进而提升分类性能.本文方法在PaviaU和Salinas两个高光谱数据集上的总体分类准确度分别达到84.91%和89.74%,相较于其他方法明显提高了地物分类性能.     

Calibration of Stress-triaxiality Dependent Crack Formation Criteria: A New Hybrid Experimental–Numerical Method

A new experimental technique has been developed to investigate the onset of fracture in metals at low and intermediate stress triaxialities. The gage section of a flat specimen has been designed such that cracks are most likely to initiate within the specimen center, remote from the specimen boundaries. Along with the specimen, a biaxial testing device has been built to apply a well-defined displacement field to the specimen shoulders. The stress state within the specimen is adjusted by changing the biaxial loading angle. Using this new experimental technique, the crack initiation in metals can be studied experimentally for stress triaxialities ranging from 0.0 to 0.6. The stress and strain fields within the specimen gage section are determined from finite element analysis. The reliability of the computational model of the test set-up has been verified by comparing the simulation results with laser speckle-interferometric displacement measurements during testing. Sample experiments have been performed on the Al-7Si-Mg gravity die casting alloy. A three-step hybrid experimental–numerical calibration procedure has been proposed and applied to determine a phenomenological crack formation criterion for the Al-7Si-Mg alloy.