Power spectral density analysis for nonlinear systems based on Volterra series

Applied Mathematics and Mechanics - A consequence of nonlinearities is a multi-harmonic response via a mono-harmonic excitation. A similar phenomenon also exists in random vibration. The power...     

石墨烯负载的氧配位钴单原子稳定金属锂负极

Lithium (Li)-based batteries are the dominant energy source for consumer electronics, grid storage, and electrified transportation. However, the development of batteries based on graphite anodes is hindered by their limited energy density. With its ultrahigh theoretical capacity (3860 mAh∙g⁻¹), low redox potential (−3.04 V), and satisfactorily low density (0.54 g∙cm⁻³), Li metal is the most promising anode for next-generation high-energy-density batteries. Unfortunately, the limited cycling life and safety issues raised by dendrite growth, unstable solid electrolyte interphase, and "dead Li" have inhibited their practical use. An effective strategy is to develop a suitable lithiophilic matrix for regulating initial Li nucleation behavior and controlling subsequent Li growth. Herein, single-atom cobalt coordinated to oxygen sites on graphene (Co-O-G SA) is demonstrated as a Li plating substrate to efficiently regulate Li metal nucleation and growth. Owing to its dense and more uniform lithiophilic sites than single-atom cobalt coordinated to nitrogen sites on graphene (Co-N-G SA), high electronic conductivity, and high specific surface area (519 m²∙g⁻¹), Co-O-G SA could significantly reduce the local current density and promote the reversibility of Li plating and stripping. As a result, the Co-O-G SA based Li anodes exhibited a high Coulombic efficiency of 99.9% at a current density of 1 mA∙cm⁻² with a capacity of 1 mAh∙cm⁻², and excellent rate capability (high current density of 8 mA∙cm⁻²). Even at a high plating capacity of 6 mAh∙cm⁻², the Co-O-G SA electrode could stably cycle for an ultralong lifespan of 1300 h. In the symmetric battery, the Co-O-G SA based Li anode (Co-O-G SA/Li) possessed a stable voltage profile of 18 mV for 780 h at 1 mA∙cm⁻², and even at a high current density of 3 mA∙cm⁻², its overpotential maintained a small hysteresis of approximately 24 mV for > 550 h. Density functional theory calculations showed that the surface of Co-O-G SA had a stronger interaction with Li atoms with a larger binding energy, −3.1 eV, than that of Co-N-G SA (−2.5 eV), leading to a uniform distribution of metallic Li on the Co-O-G SA surface. More importantly, when matched with a sulfur cathode, the resulting Co-O-G SA/lithium sulfur full batteries exhibited a high capacity of 1002 mAh∙g⁻¹, improved kinetics with a small polarization of 191 mV, and an ultralow capacity decay rate of 0.036% per cycle for 1000 cycles at 0.5C (1C = 1675 mA∙g⁻¹) with a steady Coulombic efficiency of nearly 100%. Therefore, this work provides novel insights into the coordination environment of single atoms for the chemistry of Li metal anodes for high-energy-density batteries.     

An ab initio-based global potential energy surface for the SH3 system and full-dimensional state-to-state quantum dynamics study for the H2 + HS → H2S + H reaction

An accurate potential energy surface for the ground electronic state of SH₃ system has been constructed with 41,882 high level ab initio energy points and the neural network fitting method. The time-dependent wave packet method has been used to calculate the first state-to-state differential cross sections for the title reaction up to 1.2 eV in full dimensions, based on the reactant–product decoupling scheme. It is found that the majority of H₂S are produced in the ground vibrational state, with a large fraction of available energy for the reaction ending up as product translational motion. The differential cross sections at the threshold energy are dominated by a very narrow peak in the backward direction. With the increase of collision energy, the width of the angular distribution increases considerably, which is a typical feature of a direct reaction via abstract mechanism, similar to the H₂ + OH → H₂O + H reaction. © 2018 Wiley Periodicals, Inc.     

Research progress of Pt and Pt-based cathode electrocatalysts for proton-exchange membrane fuel cells

Proton-exchange membrane fuel cells (PEMFCs) have been widely used commercially to solve the energy crisis and environmental pollution. The oxygen reduction reaction (ORR) at the cathode is the rate-determining step in PEMFCs. Platinum (Pt) catalysts are used to accelerate the ORR kinetics. Pt's scarcity, high cost, and instability in an acidic environment at high potentials seriously hinder the commercialization of PEMFCs. Therefore, studies should explore electrocatalysts with high catalytic activity, enhanced stability, and low-Pt loading. This review briefly introduces the research progress on Pt and Pt-based ORR electrocatalysts for PEMFCs, including anticorrosion catalyst supports, Pt, and Pt-based alloy electrocatalysts. Advanced preparation technology and material characterization of Pt-based ORR electrocatalysts are necessary to improve the performance and corresponding reaction mechanisms.     

Comprehensive Profiling by Non-targeted Stable Isotope Tracing Capillary Electrophoresis-Mass Spectrometry: A New Tool Complementing Metabolomic Analyses of Polar Metabolites

Mass spectrometry (MS) driven metabolomics is a frequently used tool in various areas of life sciences; however, the analysis of polar metabolites is less commonly included. In general, metabolomic analyses lead to the detection of the total amount of all covered metabolites. This is currently a major limitation with respect to metabolites showing high turnover rates, but no changes in their concentration. Such metabolites and pathways could be crucial metabolic nodes (e.g., potential drug targets in cancer metabolism). A stable-isotope tracing capillary electrophoresis–mass spectrometry (CE-MS) metabolomic approach was developed to cover both polar metabolites and isotopologues in a non-targeted way. An in-house developed software enables high throughput processing of complex multidimensional data. The practicability is demonstrated analyzing [U-¹³C]-glucose exposed prostate cancer and non-cancer cells. This CE-MS-driven analytical strategy complements polar metabolite profiles through isotopologue labeling patterns, thereby improving not only the metabolomic coverage, but also the understanding of metabolism.     

基于扩展多面体的离散单元法及其作用于圆桩的冰载荷计算

对于具有复杂几何形态的多面体单元,线性接触模型不能准确地计算不同接触模式下的作用力,且接触变形和作用力方向也不易判断.基于闵可夫斯基和(Minkowski sum)方法的扩展多面体单元能够准确描述非规则颗粒单元的几何形态,并可精确计算单元间的接触碰撞作用.该方法具有接触判断简单、计算效率高的特点.它将基本多面体和扩展球体相叠加以形成具有光滑棱边和角点的扩展多面体单元.考虑扩展多面体单元相互作用过程中角点、棱边和平面之间的不同接触模式,发展了相应的非线性黏弹性接触模型. 该接触模型将不同接触模型下的法向刚度统一表述为单元接触中接触点处等效曲率半径的函数;黏滞力和切向弹性力接触模型则借鉴球体单元非线性接触模型的处理方法. 为检验扩展多面体的可靠性,对碎冰区冰块对圆桩结构的冰载荷进行了离散元分析. 采用沃洛诺伊(Voronoi)切割算法获得了碎冰的初始随机分布状态,并考虑了海冰在运动过程中的海水浮力和拖曳力.计算表明该扩展多面体单元可描述海冰在海流拖曳下的运动过程以及圆桩结构的动冰力特性.在此基础上进一步分析了冰速和冰块尺寸对圆桩冰力的影响,并确定了冰力在圆桩上的分布规律. 最后,讨论了目前扩展多面体单元在计算冰载荷方面的局限性和改进方法.     

Estimation of particle dynamics in 2-D fluidized beds using particle tracking velocimetry

The experimental characterization of particle dynamics in fluidized beds is of great importance in fostering an understanding of solid phase motion and its effect on particle properties in granulation processes. Commonly used techniques such as particle image velocimetry rely on the cross-correlation of illumination intensity and averaging procedures. It is not possible to obtain single particle velocities with such techniques. Moreover, the estimated velocities may not accurately represent the local particle velocities in regions with high velocity gradients. Consequently, there is a need for devices and methods that are capable of acquiring individual particle velocities. This paper describes how particle tracking velocimetry can be adapted to dense particulate flows. The approach presented in this paper couples high-speed imaging with an innovative segmentation algorithm for particle detection, and employs the Voronoi method to solve the assignment problem usually encountered in densely seeded flows. Lagrangian particle tracks are obtained as primary information, and these serve as the basis for calculating sophisticated quantities such as the solid-phase flow field, granular temperature, and solid volume fraction. We show that the consistency of individual trajectories is sufficient to recognize collision events.