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This paper analyzes the correlation and variability between surface weathering, type, color, decoration, and chemical composition of glass artifacts. Based on the interactions of these five factors, the classified glass artifacts are studied and modeled, and the unclassified glass artifacts are further investigated.

The air-sensitivity of transition metal oxide cathode materials (Na

Rechargeable aqueous Zn batteries have been widely investigated in recent years due to the merits of high safety and low cost. However inevitable dendrite growth, corrosion and hydrogen evolution of Zn anodes severely compromise the practical lifespan of rechargeable Zn batteries. Despite the encouraging improvements for Zn anodes reported in the literature, the comprehensive understanding of Zn anodes under practical conditions is still often neglected. In this article, we focus on the "less-discussed" but critically important points for rechargeable aqueous Zn batteries, including revisit of the relationship between the coulombic efficiency and lifespan of Zn anodes, the rational control of the pH environment in the vicinity of Zn anodes, the design of appropriate aqueous separators and the relevant estimation of practical energy density for aqueous Zn batteries. It concludes that energy density of 60-80 W h kg

The beneficial impact of the initial rotational |jK〉-mode selection on the vibrational-specific reactivity is discussed.

Tuning the hydrogen-bonding network and strengthening H2O–Li+–anion solvation complexes by “hydrotropic” ionic liquids provide a solution to suppress H2O activity and extend the electrochemical stability window for high-voltage aqueous batteries.

Optimal electrolyte heterogeneity decouples local and global electrolyte structures, thus enabling a locally increased Na+ concentration and global 3D rapid Na+ transport path and robust interphases in Na-ion batteries.

Fault detection for key components in the braking system of freight trains is critical for ensuring railway transportation safety. Despite the frequently employed methods based on deep learning, these fault detectors are highly reliant on hardware resources and are complex to implement. In addition, no train fault detectors consider the drop in accuracy induced by scale variation of fault parts. This paper proposes a lightweight anchor-free framework to solve the above problems. Specifically, to reduce the amount of computation and model size, we introduce a lightweight backbone and adopt an anchor-free method for localization and regression. To improve detection accuracy for multi-scale parts, we design a feature pyramid network to generate rectangular layers of different sizes to map parts with similar aspect ratios. Experiments on four fault datasets show that our framework achieves 98.44% accuracy while the model size is only 22.5 MB, outperforming state-of-the-art detectors., 9 pages, 4 figures

Uniform and compact Zn deposition-dissolution is essential to achieve high Coulombic efficiency and long lifespan for Zn anodes. More attention has been commonly focused on the suppression of macroscopic Zn dendrites in the previous reports. The rational control of the microstructure of Zn deposition to prevent the intrinsic volume expansion and pulverization of Zn metal so as to stabilize Zn anodes is less discussed. Herein, we construct a three-dimensional topological Zn deposition at the nanoscale through an in situ electrochemical process in the optimal hybrid aqueous electrolyte. The topological electrode structure can efficiently accommodate microscopic strain and volume variation and thus largely preserve the macroscopic integrity and electrical contact of Zn anodes, leading to enhanced reversibility and stability. With the unique topological structure of Zn deposition, the Coulombic efficiency of Zn anodes could reach99.9% with excellent cycling over 1182 h at 2 mA cm

The title reactions were studied at a collisional energy of 5.4 kcal mol

The title reactions were studied at a collisional energy of 10.0 kcal mol-1 in a crossed-beam, product-imaging experiment. In terms of integral cross sections, all three CH3-stretching excited CH3D(vCH3 = 1) reagents promote the reactivity in forming the predominant product pair of (vCH2D, vHCl)s = (00, 0/1)s with a prominent mode-propensity of v4 > v1-I > v1-II, where v4 denotes the degenerate mode of CH3 asymmetric stretch and v1-I and v1-II are a pair of Fermi-coupled, symmetric-stretch states. The vibrationally excited CH2D product pairs of (61, 0)s, (11, 0)s, and (31, 0)s appear to be minor channels and display a reverse propensity of v4 v1-I for (11, 0)s. Based on the observed angular distributions, we conjecture that, irrespective of the initial mode of excitation, the (00, 0)s product pair proceeds by a direct abstraction of the peripheral type, whereas the (00,1)s pair is mediated via a resonance pathway. Intriguingly, the angular distributions of the excited product pairs-(61, 0)s, (11, 0)s, and (31, 0)s-are remarkably similar and comprise the traits of both the peripheral mechanism and resonance pathway. Possible interpretation and implication are suggested. In addition, due to the spectral overlap of the REMPI bands and heavily congested image features, a robust data analysis method is developed, which enables us to extract the dynamics attributes of a weak feature buried in the proximate, more intense ones with high fidelity.

In the majority of rechargeable batteries including lithium‐ion batteries, polyvinylidene fluoride (PVdF) binders are the most commonly used binder for both anode and cathode. However, using PVdF binder requires the organic solvent of N‐methyl‐2‐pyrrolidone which is expensive, volatile, combustible, toxic, and has poor recyclability. Therefore, switching to aqueous electrode processing routes with non‐toxic binders would provide a great leap forward towards the realization of ideally fully sustainable and environmentally friendly electrochemical energy storage devices. Various water‐soluble binders (aqueous binders) were characterized and compared to the performance of conventional PVdF. Our study demonstrates that the electrochemical performance of Zn/MnO2 aqueous batteries is significantly improved by using sodium carboxymethyl cellulose (CMC) binder. In addition, CMC binders offer desirable adhesion, good wettability, homogeneous material distribution, and strong chemical stability at certain pH levels (3.5–5) without any decomposition for long‐cycle life.

Background: A metabolic “switch” from oxidative phosphorylation to glycolysis provides tumor cells with energy and biosynthetic substrates, thereby promoting tumorigenesis and malignant progression. However, the mechanisms controlling this metabolic switch in tumors is not entirely clear. Methods: Clinical specimens were used to determine the effect of SAM68 on lung adenocarcinoma (LUAD) tumorigenesis and metastasis, and mouse models and molecular biology assays were performed to elucidate the function and underlying mechanisms in vitro and in vivo. Results: SAM68 mRNA levels were higher in LUAD tissue than in normal lung tissue, indicating that SAM68 expression is upregulated in LUAD. Patients with LUAD with SAM68high (n = 257) had a higher frequency of tumor recurrence (p = 0.025) and recurrence-free survival (p = 0.013) than did those with SAM68low (n = 257). Patients with SAM68high mRNA levels (n = 257) were at a higher risk for cancer-related death (p = 0.006), and had shorter overall survival (p = 0.044) than did those with SAM68low. SAM68 promotes tumorigenesis and metastasis of LUAD cells in vitro and in vivo by regulating the cancer metabolic switch. SAM68 drives cancer metabolism by mediating alternative splicing of pyruvate kinase (PKM) pre-mRNAs, and promoting the formation of PKM2. Mechanistically, SAM68 increased the binding of the splicing repressor hnRNP A1 to exon 9 of PKM, thereby enhancing PKM2 isoform formation and PKM2-dependent aerobic glycolysis and tumorigenesis. Conclusions: SAM68 promotes LUAD cell tumorigenesis and cancer metabolic programming via binding of the 351-443 aa region of SAM68 to the RGG motif of hnRNP A1, driving hnRNP A1-dependent PKM splicing, contributing to increased oncogene PKM2 isoform formation and inhibition of PKM1 isoform formation. SAM68 is therefore a promising therapeutic target for the treatment of LUAD.

Scattering resonance is a fascinating phenomenon which manifests as a peak or a dip in an observable as a function of collisional energy (Ec). Its occurrence requires a potential well to support th...

The sodium ion battery (NIB) is a promising alternative technology for energy storage systems because of the abundance and low cost of sodium in the Earth’s crust. However, the limited cycle life a...

Stereoselectivity or stereorequirement refers to the enhancement of chemical reactivity resulting from the preferential alignment/orientation of the colliding reactants. This concept is deeply embodied in the pre-exponential A-factor of the Arrhenius rate expression or the entropy effect of thermal kinetics in physical chemistry textbooks. To understand its dynamical consequence and seek for its mechanistic origin, two different approaches of either selecting the rotational states of the reactant or aligning/orienting the reactant in the laboratory have traditionally been taken. Due to the experimental challenges, theory is far more advanced than experiment. However, even for the simple atom + diatom reaction, the physical interpretations of the calculated results can sometimes be ambiguous or controversial because of the entangled potential and kinematic factors. In this Feature Article, we try to experimentally tackle the problem for reactions with polyatomic reactants by adopting both approaches in parallel for the same reaction. By comparing the results from the two approaches as well as contrasting them with the analogous reactants-here, a symmetric-top CHD3 versus a spherical-top CH4, deeper physical insights are gained, which paves the road for future studies of complex systems and for establishing a more complete conceptual framework.

The transition state in Cl + CH4 is of Cl–H–C collinear geometry. As the reactant CH4 is vibrationally excited by a linearly polarized infrared (IR) light to the antisymmetric-stretching state of ν3 = 1, all four C–H bonds are collectively excited and any one of the H-atoms can be reactive. Yet, a strong alignment of the excited CH4(ν3 = 1), as evidenced from the striking stereo-specificity in the Cl + CH4 reaction, was clearly revealed in a previous, exploratory study. Reported here is the full account of that investigation at two collisional energies of Ec = 4.8 and 2.7 kcal mol−1, using a crossed molecular-beam, product-imaging approach. By active control of the polarization direction of an IR laser under judiciously chosen beam-geometries, a complete set of polarization-dependent differential cross sections is disentangled from the CH3(00) product images. To our surprise, the quantitative results appear nearly identical to those obtained for the isotope-substituted reaction of Cl + CHD3(ν1 = 1) → HCl(ν) + CD3(00). A detailed discussion is presented to elucidate the underlying physics for such an intriguing similarity in stereo-reactivity between a spherical-top and a symmetric-top reactant.

Real-time vision-based system of fault detection (RVBS-FD) for freight trains is an essential part of ensuring railway transportation safety. Most existing vision-based methods still have high computational costs based on convolutional neural networks. The computational cost is mainly reflected in the backbone, neck, and post-processing, i.e., non-maximum suppression (NMS). In this paper, we propose a lightweight NMS-free framework to achieve real-time detection and high accuracy simultaneously. First, we use a lightweight backbone for feature extraction and design a fault detection pyramid to process features. This fault detection pyramid includes three novel individual modules using attention mechanism, bottleneck, and dilated convolution for feature enhancement and computation reduction. Instead of using NMS, we calculate different loss functions, including classification and location costs in the detection head, to further reduce computation. Experimental results show that our framework achieves over 83 frames per second speed with a smaller model size and higher accuracy than the state-of-the-art detectors. Meanwhile, the hardware resource requirements of our method are low during the training and testing process., Comment: 11 pages, 5 figures, accepted by IEEE Transactions on Instrumentation and Measurement

Mode selectivity is a well-established concept in chemical dynamics. A polyatomic molecule possesses multiple vibrational modes and the mechanical couplings between them can result in complicated anharmonic motions that defy a simple oscillatory description. A prototypical example of this is Fermi-coupled vibration, in which an energy-split eigenstate executes coherent nuclear motion that is comprised of the constituent normal modes with distinctive phases. Will this vibrational phase affect chemical reactivity? How can this phase effect be disentangled from more classical amplitude effects? Here, to address these questions, we study the reaction of Cl with a pair of Fermi states of CH

Electrolysis in neutral pH solutions (e.g., wastewater and seawater) presents a transformative way for environmentally friendly, cost-effective hydrogen production. However, one of the biggest chal...

Molecular clustering and associated dynamic processes of lithium polysulfide species were unraveled using classical molecular dynamics and ab initio metadynamics calculations. The spectroscopic signatures of polysulfide clusters were analyzed using a multimodal analysis including experimental and computational nuclear magnetic resonance (NMR) and X-ray absorption spectroscopies. Lithium polysulfide solutes (Li2S4, Li2S6, and Li2S8) and their mixtures in a 1,3-dioxolane and 1,2-dimethoxyethane (DOL/DME) solvent undergo aggregation driven by intramolecular lithium–sulfur (Li–S) interactions, leading to distributions of cluster sizes, which could critically influence the functioning of lithium–sulfur batteries. Representative polysulfide clusters with systematic increases in molecular size were extracted from the classical molecular dynamics trajectories for subsequent structural and spectroscopic property calculations using density functional theory analysis. Structural analysis of these clusters reveals pr...

Mild aqueous Zn batteries have attracted increasing attention for energy storage due to the advantages of high safety and low cost; however, the rechargeability of Zn anodes is one major issue for practical applications. In this work, an effective approach is proposed to improve the reversibility and stability of Zn anodes using advanced acidic electrolytes. A trace amount of acetic acid (HAc) is employed as a buffering agent to provide a stable pH environment in aqueous Zn electrolytes, and thus suppress passivation from precipitation reactions on Zn electrodes. Meanwhile, tetramethylene sulfone (TMS) is introduced as the critical component to stabilize the Zn anodes in the acidic electrolyte. TMS greatly strengthens the hydrogen-bonding network with reduced H

Aqueous rechargeable batteries are desirable for energy storage because of their low cost and high safety. However, low capacity and short cyclic life are significant obstacles to their practical applications. Here, we demonstrate a highly reversible aqueous zinc–iodine battery using encapsulated iodine in microporous carbon as the cathode material by controlling solid–liquid conversion reactions. We identified the factors influencing solid–liquid conversion reactions, e.g., the pore size, surface chemistry of carbon host, and solvent effect. Rational manipulation of the competition between the adsorption in carbon and solvation in electrolytes for iodine species is responsible for the high reversibility and cyclic stability. The zinc–iodine battery delivers a high capacity of 174.4 mAh g–1 at 1C, stable cyclic life over 3000 cycles with ∼90% capacity retention, and negligible self-discharge. We believe that the principles for stabilizing the zinc–iodine system could provide new insight for other conversi...

The electrolyte is a crucial component of lithium–sulfur (Li–S) batteries, as it controls polysulfide dissolution, charge shuttling processes, and solid-electrolyte interphase (SEI) layer formation. Experimentally, the overall performance of Li–S batteries varies with choice of solvent system and Li-salt used in the electrolyte, and a lack of predictive understanding about the effects of individual electrolyte components inhibits the rational design of electrolytes for Li–S batteries. Here we analyze the role of the counteranions of common Li salts (such as TfO–, FSI–, TFSI–, and TDI–) when dissolved in DOL/DME (1:1 by vol.) for use in Li–S batteries. The evolution of ion–ion and ion–solvent interactions due to various anions was analyzed using 17O NMR and pulsed-field gradient (PFG) NMR and then correlated with electrochemical performance in Li–S cells. These data reveal that the formation of the passivation layer on the anode and the loss of active materials from the cathode (evidenced by polysulfide di...

High-surface-area, nanostructured carbon is widely used for encapsulating sulfur and improving the cyclic stability of Li–S batteries, but the high carbon content and low packing density limit the specific energy that can be achieved. Here we report an approach that does not rely on sulfur encapsulation. We used a low-surface-area, open carbon fibre architecture to control the nucleation and growth of the sulfur species by manipulating the carbon surface chemistry and the solvent properties, such as donor number and Li+ diffusivity. Our approach facilitates the formation of large open spheres and prevents the production of an undesired insulating sulfur-containing film on the carbon surface. This mechanism leads to ~100% sulfur utilization, almost no capacity fading, over 99% coulombic efficiency and high energy density (1,835 Wh kg−1 and 2,317 Wh l−1). This finding offers an alternative approach for designing high-energy and low-cost Li–S batteries through controlling sulfur reaction on low-surface-area carbon. Sulfur encapsulation with nanoporous carbon is a widely adopted approach for Li–S batteries, but this often results in low sulfur utilization and low volumetric energy density. Here the authors report a non-encapsulation approach for the growth of S-containing species with low-surface-area carbon and high energy.

The transition state, which gates and modulates reactive flux, serves as the central concept in our understanding of activated reactions. The barrier height of the transition state can be estimated from the activation energy taken from thermal kinetics data or from the energetic threshold in the measured excitation function (the dependence of reaction cross-sections on initial collision energies). However, another critical and equally important property, the angle-dependent barrier to reaction, has not yet been amenable to experimental determination until now. Here, using the benchmark reaction of Cl + CHD3(v1 = 1) as an example, we show how to map this anisotropic property of the transition state as a function of collision energy from the preferred reactant bond alignment of the backward-scattered products-the imprints of small impact-parameter collisions. The deduced bend potential at the transition state agrees with ab initio calculations. We expect that the method should be applicable to many other direct reactions with a collinear barrier.

Li–S batteries have been extensively studied using rigid carbon as the host for sulfur encapsulation, but improving the properties with a reduced electrolyte amount remains a significant challenge. This is critical for achieving high energy density. Here, we developed a soft PEO10LiTFSI polymer swellable gel as a nanoscale reservoir to trap the polysulfides under lean electrolyte conditions. The PEO10LiTFSI gel immobilizes the electrolyte and confines polysulfides within the ion conducting phase. The Li–S cell with a much lower electrolyte to sulfur ratio (E/S) of 4 gE/gS (3.3 mLE/gS) could deliver a capacity of 1200 mA h/g, 4.6 mA h/cm2, and good cycle life. The accumulation of polysulfide reduction products, such as Li2S, on the cathode, is identified as the potential mechanism for capacity fading under lean electrolyte conditions.

Recently, mild aqueous rechargeable Zn-MnO2 batteries have attracted increasing interest for energy storage due to the low cost of Zn and Mn resources, high safety, and environmental benignity. Extensive types of MnO2 have been proposed as the cathodes in the literature, but the different reported performance and lack of a thorough understanding of reactions in MnO2 cathodes greatly hinder the practical applications of mild aqueous Zn-MnO2 batteries. Here, we revealed the correlation between the reaction mechanisms and the used electrolytes for the mild aqueous zinc-electrolytic manganese dioxide (EMD) batteries. In optimal Zn(TFSI)2-based electrolyte, the EMD cathode exhibits a mixed diffusion-controlled conversion reaction between EMD and H+ and diffusion-free "pseudocapacitance"-like reactions. This mechanism enables excellent cycling stability of an EMD cathode over 5000 cycles with a capacity retention of 94.6%. This study provides a useful insight into developing reversible MnO2 cathodes through rational control of reaction mechanisms for high performance mild aqueous Zn-MnO2 batteries.

Along with the state-of-the-art lithium-ion (Li-ion) batteries approaching their limitation in specific energy density, “beyond Li-ion” battery technologies have become alternative energy storage solutions due to their higher specific energy density. Among them, rechargeable lithium metal battery (LMB) has been considered as one of the most promising battery technologies that promises a great increase in energy density. Among the known anode materials, the Li metal has some unique and attractive features, such as an ultrahigh theoretical capacity (3,860 mAh g−1), a lowest negative electrochemical potential (−3.04 vs SHE), and a low gravimetric density (0.534 g cm−1). Therefore, Li metal has rendered as a potential ultimate anode material in rechargeable batteries. Furthermore, a combination of Li metal with oxygen (O2) or sulfur (S) cathodes brings more viable options for the next-generation high-energy rechargeable batteries (3,505 Wh kg−1 for Li-O2, 2,600 Wh kg−1 for Li-S batteries) with a great reduction in battery cost due to the high abundance and broad distribution of O2 and S sources. However, the use of Li metal anode in LMBs still causes some critical issues, including the well-known Li dendritic growth, uncontrolled interfacial reactions with electrolytes, and large volumetric change during Li plating/stripping process. The “short circuit” of the battery by dendrite formation and the continuous depletion of electrolytes/active bulk lithium have been significantly challenging the practical application of rechargeable LMBs. In this chapter, we will discuss the fundamental challenges for both Li anode and cathodes and the proposed strategies for rechargeable LMBs. A perspective on the future research direction is also presented to initiate more helpful thoughts and promote to solve the critical issues in this research field.