Swapping catalytic active sites from cationic Ni to anionic F in Fe–F–Ni3S2 enables more efficient alkaline oxygen evolution reaction and urea oxidation reaction

Electrolysis of water for producing hydrogen instead of traditional fossil fuels is one of the most promising methods to alleviate environmental pollution and energy crisis. In this work, Fe and F ion co-doped Ni₃S₂ nanoarrays grown on Ni foam substrate were prepared by typical hydrothermal and sulfuration processes for the first time. Density functional theory (DFT) calculation demonstrate that the adsorption energy of the material to water is greatly enhanced due to the doping of F and Fe, which is conducive to the formation of intermediate species and the improvement of electrochemical performance of the electrode. The adsorption energy of anions (F and S) and cations (Fe and Ni) to water in each material was also calculated, and the results showed that F ion showed the most optimal adsorption energy of water, which proved that the doping of F and Fe was beneficial to improve the electrochemical performance of the electrode. It is worth noting that the surface of Fe–F–Ni₃S₂ material will undergo reconstruction during the process of water oxidation reaction and urea oxidation reaction, and amorphous oxides or hydroxides in situ would be formed on the surface of electrode, which are the real active species.     

Facile preparation of SnS2 nanoflowers and nanoplates for the application of high-performance hybrid supercapacitors

In this work, the SnS₂ nanoflowers (SnS₂ NFs) were solvothermally prepared in the solvent of ethanol, while SnS₂ nanoplates (SnS₂ NPs) were obtained through the identical conditions except for the solvent of water. The flowers were assembled with numerous nanosheets with very thin thickness, and the NPs exhibited hexagonal shape. When used as the battery-type electrode material for supercapacitors, the SnS₂ NFs delivered a specific capacity of as high as 264.4 C g^?1 at 1 A g^?1, which was higher than the 201.6 C g^?1 of SnS₂ NPs. Furthermore, a hybrid supercapacitor (HSC) was assembled with the SnS₂ as positive electrode and activated carbon (AC) as negative electrode, respectively. The SnS₂ NFs//AC HSC exhibited a high energy density of 28.1 Wh kg^?1 at 904.3 W kg^?1, which was higher than the 24.2 Wh kg^?1 at 844.3 W kg^?1 of SnS₂ NPs//AC HSC. Especially, when the power density was enhanced to the highest value of 8666.8 W kg^?1, the NFs-based device could still hold 20.4 Wh kg^?1. In addition, both HSC devices showed an excellent cycling stability after 5000 cycles at 5 A g^?1. The present method is simple and can be extended to the preparation of other transition metal sulfides (TMSs)-based electrode materials with brilliant electrochemical performance for supercapacitors.     

Heterofullerene C48B12-impregnated MOF-5 and IRMOF-10 for hydrogen storage: A combined DFT and GCMC simulations study

The H₂ storage properties of isoreticular metal-organic framework materials (IRMOFs), MOF-5 and IRMOF-10, impregnated with different numbers and types of heterogeneous C₄₈B₁₂ molecules were investigated using density functional theory and grand canonical Monte Carlo (GCMC) calculations. The excess hydrogen adsorption isotherms of IRMOFs at 77 K within 20 bar indicate that suitable number and type of C₄₈B₁₂ molecules play a crucial role in improving the H₂ storage properties of IRMOFs. Among the studied pure and nC₄₈B₁₂ (n = 1, 2, 4, 8) in Ci symmetry impregnating into MOF-5, at 77 K under 6 bar, MOF-5-4C₄₈B₁₂ with a 3.5 wt% and 29.9 g/L hydrogen storage density, and at 77 K under 12 bar, the pure MOF-5 with a 4.9 wt% and 31.0 g/L hydrogen storage density has the best hydrogen storage properties. Whereas, among the studied pure and nC₄₈B₁₂ (n = 1, 2, 4, 8) in S6 symmetry impregnating into IRMOF-10, IRMOF-10-8C₄₈B₁₂ always shows the best hydrogen storage properties among the pure and C₄₈B₁₂-impregnated IRMOF-10 at 77 K within 20 bar. IRMOF-10-8C₄₈B₁₂ has a 6.0 wt% and 34.6 g/L hydrogen storage density at 77 K under 6 bar, and has a 7.1 wt% and 41.4 g/L hydrogen storage density at 77 K under 12 bar. The confinement effect of IRMOFs on C₄₈B₁₂ molecules, and steric hindrance effect of C₄₈B₁₂ molecules on IRMOFs mainly affects the H₂ uptake capacity by comparing the absolute H₂ molecules in individual IRMOFs units, C₄₈B₁₂ molecules, and IRMOFs-nC₄₈B₁₂ compounds. The absolute hydrogen adsorption profiles show that eight C₄₈B₁₂ molecules impregnating into MOF-5 can exert obvious steric effects for H₂ adsorption. The saturated gravimetric and volumetric H₂ densities of IRMOF-10-8C₄₈B₁₂ higher than those of MOF-5-8C₄₈B₁₂ due to with larger free volume.     

High-entropy titanate pyrochlore as newly low-thermal conductivity ceramics

Low-thermal conductivity ceramics play an indispensable role in maximizing the efficiency and durability of hot end components. Pyrochlore, particularly zirconate pyrochlore, is currently a highly promising and widely studied candidate for its extremely low thermal conductivity. However, there are still few pyrochlores that offer both stiffness, insulation, and good thermal expansion properties. In this work, the solidification method was innovatively introduced into the preparation of titanate pyrochlore, and combined it with the compositional design of high-entropy. Through careful composition design and solidification control, the high-density and uniform elements distributed high-entropy titanate pyrochlore ceramics were successfully prepared. These samples possess high hardness (15.88 GPa) and Young’s modulus (295.5 GPa), low thermal conductivity (0.947 W·m^?1·K^?1), excellent thermal expansion coefficient (11.6 ×10^?6/K) and an exquisite balance between stiffness and insulation (E/κ, 312.1 GPa·W^?1·m·K), in which the E/κ exhibits the highest value among the current reported works.     

基于人工神经网络的智能化架空线路应变快速解调方法北大核心

为了提高智能化光纤复合架空线路态势感知的实时性,将人工神经网络方法应用于光纤沿线应变解调,确定了神经网络的结构。编程实现了基于洛伦兹模型的最小二乘谱拟合方法和神经网络方法,采用不同信噪比和布里渊频移的布里渊谱训练神经网络,将它们应用于某光纤复合架空线路沿线光纤应变的测量,从不同角度比较了两种方法的计算结果。计算结果表明,神经网络方法能有效获得光纤沿线的布里渊频移进而获得应变,具有与谱拟合方法相似的准确性,但应变解调时间仅约为谱拟合方法的1/20000。研究结果为提高智能光纤复合架空线路态势感知的实时性提供了参考。     

Nonlinearity in regulating the metal to insulator transition of ReNiO3 towards low temperature range

Among the existing material family of the correlated oxides, the rare earth nickelates (ReNiO₃) exhibit broadly adjustable metal to insulator transition (MIT) properties that enables correlated electronic applications, such as thermistors, thermochromics, and logical devices. Nevertheless, how to accurately control the critical temperature (T_MIT) of ReNiO₃ via the co-occupation of the rare-earth elements is yet worthy to be further explored. Herein, we demonstrate the non-linearity in adjusting the T_MIT of ReNiO₃ towards lower temperatures via introducing Pr co-occupation within ReNiO₃ (e.g., Pr_xNd_1-xNiO₃ and Pr_xSm_1-xNiO₃) as synthesized by KCl molten-salt assisted high oxygen pressure reaction approach. Although the T_MIT is effectively reduced via Pr substitution, it does not strictly follow a linear relationship, in particular, when there is large difference in the ionic radius of the co-occupation rare-earth elements. Furthermore, the most significant deviation in T_MIT from the expected linear relationship appears at an equal co-occupation ratio of the two different rare-earth elements, while the abruption in the variation of resistivity across T_MIT is also reduced. The present work highlights the importance to use adjacent rare-earth elements with co-occupation ratio away from 1:1 for achieving more linear adjustment in designing the metal to insulator transition properties for ReNiO₃.     

分布式多元随机动态场景生成及快速精准场景降维算法

高比例新能源及多源耦合是电力系统发展的重要特征,这也为系统稳定经济运行提出了新挑战。该文以园区型多能系统为对象,研究了分布式多元随机动态场景分析,从多时空角度有效量化不确定因素给系统造成的影响,可为系统灵活重构、多维度协同运行与决策提供有力模型与场景支撑。首先由预测误差驱动拟合多元功率预测误差概率分布,全面反映随机功率出力信息,提高模型泛化性;以时序相关范围参数为数据驱动关联变量,高效动态控制波动强度;最终场景生成利用逆变换映射思想保证置信度。然后针对典型场景提取,提出一种综合递归聚类思想的多段嵌套削减算法,结合改进Wasserstein距离指标,兼具准确、时效、稳定方面的优势。最后由对比实验论证该方法的前沿有效性。     

不同进水流速对泵站进水池漩涡的影响

为探究泵站进水流速大小与泵站进水池水流流态、漩涡的产生与发展变化规律,结合泵站实际运行情况,建立引渠、前池、进水池和进水管的泵站物理模型和湍流数学模型,采用VOF模型和非定常的SST k-ω湍流模型对9种不同流速的泵站进水水流特性进行数值模拟,分析不同进水流速的泵站进水池水流流场分布、漩涡涡量的变化及分布规律。研究结果表明:当进水流速为0.322 2～0.564 2 m/s时,泵站表面漩涡的强度随进水流速的增大而增强:当进水流速为0.322 2～0.401 6 m/s时,进水池出现Ⅲ、Ⅳ型漩涡;当进水流速为0.483 5 m/s时,进水池出现Ⅴ型漩涡;当进水流速为0.520 8～0.564 2 m/s时,进水池出现Ⅵ型漩涡。将数值计算结果与模型试验结果进行对比,两者基本吻合。研究结果可为泵站工程设计提供参考。     

Coupling effects of water content,temperature, oxygen density,and polytetrafluoroethylene loading on oxygen transport through ionomer thin film on platinum surface in catalyst layer of proton exchange membrane fuel cell

In this work, coupling effects of water content, temperature, oxygen density, and polytetrafluoroethylene (PTFE) loading on oxygen transport through an ionomer thin film on a platinum surface in a catalyst layer of a proton exchange membrane (PEM) fuel cell are investigated using molecular dynamics approach. Taguchi orthogonal algorithm is employed to comprehensively analyze the coupling effects in a limited number of cases. It is found that the effect of operation temperature is the weakest among the four factors, which has the smallest effect index 14.4. Coupling effects including the PTFE loadings on the oxygen transfer through the ionomer thin film is uncovered. Less PTFE loadings should be beneficial for the oxygen transfer. The chemical potential gradient is considered as the major driven force for the oxygen transport through the ionomer thin film, and oxygen density is the dominating factor, significantly affecting the chemical potential in the thin film.     

Additional deepwater sampling of prey fish in Lake Michigan annual bottom trawl survey reveals new insights for depth distribution dynamics

Beginning in 2013, sites at the 128-m bottom depth contour were added to the sampling design of the annual Lake Michigan bottom trawl survey for prey fish, which has been conducted by the U.S. Geological Survey Great Lakes Science Center (GLSC) each fall since 1973, to better assess fish depth distributions in a changing ecosystem. The standard sampling design included bottom depths from 9 to 110 m, although the GLSC also sporadically conducted bottom trawl tows at the 128-m bottom depth contour during 1973–1988. Enactment of this new sampling design in 2013 revealed that mean biomass density of deepwater sculpins (Myoxocephalus thompsonii) at the 128-m depth exceeded the sum of mean biomass densities at shallower depths, indicating that the bulk of the deepwater sculpin population is residing in waters deeper than 110 m. Thus, our findings supported the hypothesis that the depth distribution of the deepwater sculpin population had shifted to deeper waters beginning in 2007, thereby explaining, at least in part, the marked decline in deepwater sculpin abundance since 2006 based on the standard sampling design. In contrast, our results did not support the hypothesis that the slimy sculpin (Cottus cognatus) population had shifted to deeper waters sometime after 2000. A portion of the burbot (Lota lota) population may have also shifted in depth distribution to waters deeper than 110 m after 2007, based on our results. Our findings have served as an impetus to further expand the range of depths sampled in our bottom trawl survey.