Search

The continuous effort in making artificial neural networks more alike to human brain calls for the hardware elements to implement biological synapse-like functionalities. The recent experimental demonstration of ferroelectric-like FETs promises low-power operation as compared to the conventional ferroelectric switching devices. This work presents an in-house numerical tool, which self-consistently solves the electrostatics and time-dependent electronic and ionic transport. The tool is exploited to analyze the effect that various physical parameters such as mobility and ion concentration could have on the design of the ferroelectric-like FETs. Their suitability in emulating different functions of the biological synapses is also demonstrated. [ABSTRACT FROM AUTHOR]

When electrolyte solutions are confined in micro- and nanochannels their conductivity is significantly different from those in a bulk phase. Here we revisit the theory of this phenomenon by focusing attention on the reduction in the ion mobility with the concentration of salt and a consequent impact to the conductivity of a monovalent solution, from bulk to confined in a narrow slit. We first give a systematic treatment of electrophoresis of ions and obtain equations for their zeta potentials and mobilities. The latter are then used to obtain a simple expression for a bulk conductivity, which is valid in a concentration range up to a few molars and more accurate than prior analytic theories. By extending the formalism to the electrolyte solution in the charged channel the equations describing the conductivity in different modes are presented. They can be regarded as a generalization of prior work on the channel conductivity to a more realistic case of a nonzero reduction of the electrophoretic mobility of ions with salt concentration. Our analysis provides a framework for interpreting measurements on the conductivity of electrolyte solutions in the bulk and in narrow channels. [ABSTRACT FROM AUTHOR]

BaSnF4 is a prospective solid state electrolyte for fluoride ion batteries. However, the diffusion mechanism of the fluoride ions remains difficult to study, both in experiments and in simulations. In principle, ab initio molecular dynamics could allow to fill this gap, but this method remains very costly from the computational point of view. Using machine learning potentials is a promising method that can potentially address the accuracy issues of classical empirical potentials while maintaining high efficiency. In this work, we fitted a dipole polarizable ion model and trained machine learning potential for BaSnF4 and made comprehensive comparisons on the ease of training, accuracy and efficiency. We also compared the results with the case of a simpler ionic system (NaF). We show that contrarily to the latter, for BaSnF4 the machine learning potential offers much higher versatility. The current work lays foundations for the investigation of fluoride ion mobility in BaSnF4 and provides insight on the choice of methods for atomistic simulations. [ABSTRACT FROM AUTHOR]

High-resolution ion mobility (resolving power > 200) coupled with mass spectrometry (MS) is a powerful analytical tool for resolving isobars and isomers in complex samples. High-resolution ion mobility is capable of discerning additional structurally distinct features, which are not observed with conventional resolving power ion mobility (IM, resolving power ~ 50) techniques such as traveling wave IM and drift tube ion mobility (DTIM). DTIM in particular is considered to be the "gold standard" IM technique since collision cross section (CCS) values are directly obtained through a first-principles relationship, whereas traveling wave IM techniques require an additional calibration strategy to determine accurate CCS values. In this study, we aim to evaluate the separation capabilities of a traveling wave ion mobility structures for lossless ion manipulation platform integrated with mass spectrometry analysis (SLIM IM-MS) for both lipid isomer standards and complex lipid samples. A cross-platform investigation of seven subclass-specific lipid extracts examined by both DTIM-MS and SLIM IM-MS showed additional features were observed for all lipid extracts when examined under high resolving power IM conditions, with the number of CCS-aligned features that resolve into additional peaks from DTIM-MS to SLIM IM-MS analysis varying between 5 and 50%, depending on the specific lipid sub-class investigated. Lipid CCS values are obtained from SLIM IM (TW(SLIM)CCS) through a two-step calibration procedure to align these measurements to within 2% average bias to reference values obtained via DTIM (DTCCS). A total of 225 lipid features from seven lipid extracts are subsequently identified in the high resolving power IM analysis by a combination of accurate mass-to-charge, CCS, retention time, and linear mobility-mass correlations to curate a high-resolution IM lipid structural atlas. These results emphasize the high isomeric complexity present in lipidomic samples and underscore the need for multiple analytical stages of separation operated at high resolution. [ABSTRACT FROM AUTHOR]

Complex coacervates play essential roles in various biological processes and applications. Although substantial progress has been made in understanding the molecular interactions driving complex coacervation, the mechanisms stabilizing coacervates against coalescence remain experimentally challenging and not fully elucidated. We recently showed that polydiallyldimethylammonium chloride (PDDA) and adenosine triphosphate (ATP) coacervates stabilize upon their transfer to deionized (DI) water. Here, we perform molecular dynamics simulations of PDDA-ATP coacervates in supernatant and DI water, to understand the ion dynamics and structure within stable coacervates. We found that transferring the coacervates to DI water results in an immediate ejection of a significant fraction of small ions (Na+ and Cl−) from the surface of the coacervates to DI water. We also observed a notable reduction in the mobility of these counterions in coacervates when in DI water, both in the cluster-forming and slab simulations, together with a lowered displacement of PDDA and ATP. These results suggest that the initial ejection of the ions from the coacervates in DI water may induce an interfacial skin layer formation, inhibiting further mobility of ions in the skin layer. Transferring coacervates based on polydiallyldimethylammonium chloride and adenosine triphosphate into deionized water has been experimentally demonstrated to stabilize them against coalescence. Here, molecular modeling and simulations are used to study the coacervation and stabilization of the relevant polyelectrolyte mixture, systematically investigating the structural and dynamic properties that lead to stability. [ABSTRACT FROM AUTHOR]

To enhance the performance and widespread use of solid oxide fuel cells (SOFCs), addressing the low-temperature (< 650 °C) electrochemical performance and operational stability issues of cathode materials is crucial. Here, we propose an innovative approach to enhance oxygen ion mobility and electrochemical performance of perovskite oxide by substituting some oxygen sites with chlorine anions. The designed SrTa0.1Fe0.9O3-δ-xClx (x = 0.05 and 0.10) exhibits improved performance compared to SrTa0.1Fe0.9O3-δ (STF). SrTa0.1Fe0.9O2.95-δCl0.05 (STFCl0.05) shows the lowest area-specific resistance (ASR) value on Sm0.2Ce0.8O1.9 (SDC) electrolyte. At 600 °C, STFCl0.05 achieves an ASR value of 0.084 Ω·cm2, and a single cell with STFCl0.05 reaches a higher peak power density (PPD) value (1143 mW·cm-2) than that with STF (672 mW·cm-2). Additionally, besides exhibiting excellent oxygen reduction reaction (ORR) activity at lower temperatures, the STFCl0.05 cathode demonstrates good CO2 tolerance and operational stability. Symmetrical cell operation lasts for 150 h, and single cell operation endures for 720 h without significant performance decline. The chlorine doping approach effectively enhances ORR activity and stability, making STFCl0.05 a promising cathode material for low-temperature SOFCs. [ABSTRACT FROM AUTHOR]

Developing new enantioselective reactions is an important part of chemical discovery but requires time and resources to test large arrays of potential reaction conditions. New techniques are required to analyse many different reactions quickly and efficiently. Mass spectrometry is a high‐throughput method; when combined with ion‐mobility spectrometry, this technique can monitor diastereomeric reaction intermediates and thus be a handle to study enantioselective reactions. Through this technique and others, it was noted before that in the organocatalytic 1,4‐addition to α,β‐unsaturated aldehydes, the abundance of initial diastereomeric intermediates correlates strongly to that of the final enantiomeric products. This work determines isomeric abundance for various catalysts and aldehydes and uses it to predict the enantiomeric excess of two control reactions. The prediction matches well for one reaction but does not predict the obtained results for the second. This finding confirms that the E/Z ratio of the iminium intermediates can be used as a predictor for some reactions, but the kinetics of the following steps can dramatically change the true enantioselectivity. [ABSTRACT FROM AUTHOR]

Chiral analysis is of high interest in many fields such as chemistry, pharmaceuticals and metabolomics. Mass spectrometry and ion mobility spectrometry are useful analytical tools, although they cannot be used as stand-alone methods. Here, we propose an efficient strategy for the enantiomer characterization of amino acids (AAs) using non-covalent copper complexes. A single ion mobility monitoring (SIM2) method was applied on a TIMS-ToF mass spectrometer to maximize the detection and mobility separation of isomers. Almost all of the 19 pairs of proteinogenic AA enantiomers could be separated with at least one combination with the chiral references L-Phe and L-Pro. Furthermore, we extended the targeted SIM2 method by stitching several mobility ranges, in order to be able to analyze complex mixtures in a single acquisition while maintaining high mobility resolution. Most of the enantiomeric pairs of AAs separated with the SIM2 method were also detected with this approach. The SIM2 stitching method thus opens the way to a more comprehensive chiral analysis with TIMS-ToF instruments. [ABSTRACT FROM AUTHOR]

nH-Perfluoroalkyl carboxylic acids (nH-PFCAs) are emerging pollutants. Their identification by ion mobility is frustrated by the nH-PFCAs having unexpectedly small collision cross sections (CCS). Theory and experiment agree that this is because nH-PFCA ions undergo internal hydrogen bridging, and this insight will help guide the creation of more accurate methods for pollutant identification. [ABSTRACT FROM AUTHOR]

Materials with high ion mobility are widely used in many fields of modern science and technology. Over the last 40 years, they have thoroughly changed our world. The paper characterizes the structural features of minerals and their synthetic analogs possessing this property. Special attention is paid to the ionic conductors with tetrahedral (zincite- and wurtzite-like), octahedral (ilmenite-like), and mixed (NASICON-like) frameworks. It is emphasized that the main conditions for fast ionic transport are related to the size and positions occupied by a mobile ion, their activation energy, the presence and diameter of conduction channels running inside the structure, isomorphic impurities, and other structural peculiarities. The results of the studies of solid electrolytes are dispersed in different editions, and the overview of new ideas related to their crystal structures was the focus of this paper. [ABSTRACT FROM AUTHOR]

Recently, ion mobility spectrometry‐mass spectrometry (IMS‐MS) has become more readily incorporated into various omics‐based workflows. These growing applications are due to developments in instrumentation within the last decade that have enabled higher‐resolution ion mobility separations. Two such platforms are the cyclic (cIMS) and structures for lossless ion manipulations (SLIM), both of which use traveling wave ion mobility spectrometry (TWIMS). High‐resolution separations achieved with these techniques stem from the drastically increased pathlengths, on the order of 10 s of meters to >1 km, in both cIMS‐MS and SLIM IMS‐MS, respectively. Herein, we highlight recent developments and advances, for the period 2019–2023, in high‐resolution traveling wave‐based IMS‐MS through instrumentation, calibration strategies, hyphenated techniques, and applications. Specifically, we will discuss applications including CCS calculations in multipass IMS‐MS separations, coupling of IMS‐MS with chromatography, imaging, and cryogenic infrared spectroscopy, and isomeric separations of glycans, lipids, and other small metabolites. [ABSTRACT FROM AUTHOR]

Human milk oligosaccharides (HMOs) are an important class of biomolecules responsible for the healthy development of the brain‐gut axis of infants. Unfortunately, their accurate characterization is largely precluded due to a variety of reasons – there are over 200 possible HMO structures whereas only 10s of these are available as authentic analytical standards. Furthermore, their isomeric heterogeneity stemming from their many possible glycosidic linkage positions and corresponding α/β anomericities further complicates their analyses. While liquid chromatography coupled to tandem mass spectrometry remains the gold standard for HMO analyses, it often times cannot resolve all possible isomeric species and thus warrants the development of other orthogonal approaches. High‐resolution ion mobility spectrometry coupled to mass spectrometry has emerged as a rapid alternative to condensed‐phase separations but largely has remained limited to qualitative information related to the resolution of isomers. In this work, we have assessed the use of permethylation to improve both the resolution and sensitivity of HMO analyses with cyclic ion mobility separations coupled with mass spectrometry. In addition to this, we have developed the first‐ever high‐resolution collision cross‐section database for permethylated HMOs using our previously established calibration protocol. We envision that this internal reference database generated from high‐resolution cyclic ion mobility spectrometry‐mass spectrometry will greatly aid in the accurate characterization of HMOs and provide a valuable, orthogonal, approach to existing liquid chromatography–tandem mass spectrometry‐based methods. [ABSTRACT FROM AUTHOR]

[Display omitted] • Sodium ions inside biomolecular condensates experience heterogeneous dynamics. • An integrative 23Na NMR relaxation-based approach is developed. • This approach allows separating contribution of various sodium ion populations. • Three populations of sodium ions with distinct dynamics detected in agarose gels. Metal ions, including biologically prevalent sodium ions, can modulate electrostatic interactions frequently involved in the stability of condensed compartments in cells. Quantitative characterization of heterogeneous ion dynamics inside biomolecular condensates demands new experimental approaches. Here we develop a 23Na NMR relaxation-based integrative approach to probe dynamics of sodium ions inside agarose gels as a model system. We exploit the electric quadrupole moment of spin-3/2 23Na nuclei and, through combination of single-quantum and triple-quantum-filtered 23Na NMR relaxation methods, disentangle the relaxation contribution of different populations of sodium ions inside gels. Three populations of sodium ions are identified: a population with bi-exponential relaxation representing ions within the slow motion regime and two populations with mono-exponential relaxation but at different rates. Our study demonstrates the dynamical heterogeneity of sodium ions inside agarose gels and presents a new experimental approach for monitoring dynamics of sodium and other spin-3/2 ions (e.g. chloride) in condensed environments. [ABSTRACT FROM AUTHOR]

The chemical looping oxidative dehydrogenation (CL‐ODH) of ethane represents a highly effective approach for converting ethane into the value‐added product ethylene. This investigation focused on the synthesis of SrMnO3 and its halide ions doped derivatives (SrMnO3Cl and SrMnO3Br) through the sol‐gel method. The performance of these perovskites, employed as oxygen carriers in CL‐ODH of ethane, was explored. The results unveiled several advantageous outcomes arising from the incorporation of halide ions (Cl− and Br−) with larger radius into the oxygen sites of the SrMnO3 perovskite. Halide ions doping notably induced cell volume expansion and enhanced lattice fringe spacing. Furthermore, it contributed to elevated oxygen vacancy concentration, increased Mn4+/Mn3+ molar ratio, and improved oxygen ions mobility within the bulk lattice. Fixed‐bed experiments demonstrated that these redox catalysts, doped with halide ions, exhibited outstanding activity and stability during cycling tests, exhibiting enhanced both ethylene selectivity and yield in CL‐ODH of ethane. In summary, the introduction of halide ions into SrMnO3 emerges as a promising strategy for enhancing the performance of CL‐ODH in ethane conversion for SrMnO3 based oxygen carriers. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

Polymer cation exchange membranes (CEMs) are widely used in water treatment processes. The fundamental factors that control the separation and selectivity of cations with different valences in CEMs are not fully understood. In this study, we use atomistic molecular dynamics simulations to investigate the underlying molecular mechanisms that control the mobility of cations with different valences in Nafion membranes. Our results indicate structural differences in binding of monovalent and divalent cations, which gives rise to differences in ion diffusion in Nafion. Monovalent cations are shown to be "territorially" bound, i.e., bound while partially hydrated, to the fixed charge groups whereas divalent cations are shown to be "site" bound, i.e., bound while fully dehydrated, to the charge groups on the polymer. This difference in binding structure gives rise to differences in transport characteristics of cations in Nafion. [ABSTRACT FROM AUTHOR]

Rationale: In soft chemical ionization mass spectrometry, analyte ions are produced via ion–molecule reactions in the reactor. When an electric field E is imposed, the ion drift velocity vd determines the reaction time and the effective ion temperature. Agreement between experimental ion mobilities and theoretical predictions confirms the accuracy of the ion residence time measurement procedure. Methods: A selected ion flow‐drift tube (SIFDT), an instrument with a chemical ionization source, was used to produce protonated aldehydes and selectively inject them into the resistive glass drift tube filled with He. Arrival‐time distributions of ions were obtained using the Hadamard modulation. Reduced ion mobilities were then obtained at a pressure of 2 hPa in the E/N range of 5–15 Td. Theoretical ion mobility values were calculated using two methods: hard‐sphere approximation and trajectory modelling. Results: The measured mobilities of three saturated and three unsaturated protonated aldehydes do not show substantial variation across the studied E/N range. Effective temperatures calculated using the Wannier formula from measured gas temperatures ranged from 300 to 315 K. Experimentally obtained values of the near‐zero‐ E/N‐reduced ion mobilities agree with both methods of calculations typically within ±3% standard deviation (maximum ±5%). Conclusions: The experimental SIFDT values of reduced mobilities in He of protonated aldehyde molecules generated from a chemical ionization source are in close agreement with two different theoretical methods based on the density functional theory calculations of ion geometries and partial atomic charges. Besides its fundamental importance, the ion mobility results validate the correct operation of the drift tube reactor and the ion residence time measurement procedure. Diffusion losses can also be determined from these results. [ABSTRACT FROM AUTHOR]

The development of improved solid electrolytes (SEs) plays a crucial role in the advancement of bulk‐type solid‐state battery (SSB) technologies. In recent years, multicomponent or high‐entropy SEs are gaining increased attention for their advantageous charge‐transport and (electro)chemical properties. However, a comprehensive understanding of how configurational entropy affects ionic conductivity is largely lacking. Herein we investigate a series of multication‐substituted lithium argyrodites with the general formula Li6+x[M1aM2bM3cM4d]S5I, with M being P, Si, Ge, and Sb. Structure‐property relationships related to ion mobility are probed using a combination of diffraction techniques, solid‐state nuclear magnetic resonance spectroscopy, and charge‐transport measurements. We present, to the best of our knowledge, the first experimental evidence of a direct correlation between occupational disorder in the cationic host lattice and lithium transport. By controlling the configurational entropy through compositional design, high bulk ionic conductivities up to 18 mS cm−1 at room temperature are achieved for optimized lithium argyrodites. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors via entropy engineering, overcoming compositional limitations for the design of advanced electrolytes and opening up new avenues in the field. [ABSTRACT FROM AUTHOR]

Black soldier fly (BSF) melanin is a new supply of the brown-black pigment eumelanin. Given that eumelanin is a model bioelectronic material for applications such as medical devices and sensors, understanding BSF melanin's electrical properties is important to confirm its viability as an advanced material. Presented here is a systematic, hydration dependent alternating current study of BSF melanin utilising both H2O and D2O vapours. There is a clear difference between the vapours, enabling a thorough analysis including Nyquist plots with model circuit analysis, broad band dielectric spectroscopic modelling as well as applying the Trukhan model to understand free ion concentration and mobility changes as a function of hydration. We find that BSF melanin behaves similarly to previous reports on synthetic systems, and the analysis here sheds additional light on potential charge transport changes. Significantly, a key finding is that there are two different mobility mechanisms for ion transport depending on hydration. [ABSTRACT FROM AUTHOR]

In the realm of quantitative proteomics, data-independent acquisition (DIA) has emerged as a promising approach, offering enhanced reproducibility and quantitative accuracy compared to traditional data-dependent acquisition (DDA) methods. However, the analysis of DIA data is currently hindered by its reliance on project-specific spectral libraries derived from DDA analyses, which not only limits proteome coverage but also proves to be a time-intensive process. To overcome these challenges, we propose ProPept-MT, a novel deep learning-based multi-task prediction model designed to accurately forecast key features such as retention time (RT), ion intensity, and ion mobility (IM). Leveraging advanced techniques such as multi-head attention and BiLSTM for feature extraction, coupled with Nash-MTL for gradient coordination, ProPept-MT demonstrates superior prediction performance. Integrating ion mobility alongside RT, mass-to-charge ratio (m/z), and ion intensity forms 4D proteomics. Then, we outline a comprehensive workflow tailored for 4D DIA proteomics research, integrating the use of 4D in silico libraries predicted by ProPept-MT. Evaluation on a benchmark dataset showcases ProPept-MT's exceptional predictive capabilities, with impressive results including a 99.9% Pearson correlation coefficient (PCC) for RT prediction, a median dot product (DP) of 96.0% for fragment ion intensity prediction, and a 99.3% PCC for IM prediction on the test set. Notably, ProPept-MT manifests efficacy in predicting both unmodified and phosphorylated peptides, underscoring its potential as a valuable tool for constructing high-quality 4D DIA in silico libraries. [ABSTRACT FROM AUTHOR]

Regulation of the surface film characteristics of Li‐metal is a pivotal strategy for augmenting the electrochemical performance of Li‐metal batteries. This investigation elucidates a straightforward approach to surface film modification, namely, pre‐treatment via a CO2 gas reaction, and its subsequent impact on the electrochemical attributes of Li‐metal electrodes. Analysis of the topography and composition of the Li metal surfaces revealed the transformation of the surface film into a more uniform layer enriched with inorganic compounds, including Li2CO3 and Li2O, by pre‐treatment. This pre‐treatment process significantly enhances the electrochemical properties, such as cyclability and overpotential, in Li/Li symmetric cells, primarily because of the formation of an improved solid‐electrolyte interphase (SEI) derived from the altered surface film on Li metal electrodes. The reformed SEI significantly increases the mobility of Li ions through the interphase, thereby attenuating the impedance associated with Li‐ion migration within the SEI. This resistance attenuation is instrumental in alleviating the overpotentials, thereby significantly refining the electrochemical plating and stripping dynamics of Li metal electrodes. [ABSTRACT FROM AUTHOR]

Copyright of Inorganic Chemicals Industry is the property of Editorial Office of Inorganic Chemicals Industry and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

Modulation efficiency and mechanisms of repetitively pulsed streamer discharge in humid air are ambiguous with dramatic variations in free electron availability, residual ion mobility, enhanced heat release, etc, caused by water molecules intentionally supplemented or existing in the surrounding environment. The inception and propagation patterns of repetitively pulsed streamer discharge modulated by superimposed DC bias are experimentally investigated in the needle-plane electrode configuration. The inception voltage decreases due to negative ion drift under positive DC bias. The secondary streamer with a bright glowing cloud prolongs towards the plane electrode and the diameter decreases under positive DC bias. The primary streamer tends to propagate along the off-axis direction under negative DC bias. The number of applied pulses before breakdown decreases with the increase in positive DC bias and illustrates an insignificant dependence on the negative DC bias. The effect of air humidity is more pronounced than the DC bias. The streamer inception, propagation, and morphological transition are explained by residual space charge distributions and drift velocity. [ABSTRACT FROM AUTHOR]

Glycosaminoglycans (GAGs) are linear and acidic polysaccharides. They are ubiquitous molecules, which are involved in a wide range of biological processes. Despite being structurally simple at first glance, with a repeating backbone of alternating hexuronic acid and hexosamine dimers, GAGs display a highly complex structure, which predominantly results from their heterogeneous sulfation patterns. The commonly applied method for compositional analysis of all GAGs is "disaccharide analysis." In this process, GAGs are enzymatically depolymerized into disaccharides, derivatized with a fluorescent label, and then analysed through liquid chromatography. The limiting factor in the high throughput analysis of GAG disaccharides is the time‐consuming liquid chromatography. To address this limitation, we here utilized trapped ion mobility‐mass spectrometry (TIM‐MS) for the separation of isomeric GAG disaccharides, which reduces the measurement time from hours to a few minutes. A full set of disaccharides comprises twelve structures, with eight possessing isomers. Most disaccharides cannot be differentiated by TIM‐MS in underivatized form. Therefore, we developed chemical modifications to reduce sample complexity and enhance differentiability. Quantification is performed using stable isotope labelled standards, which are easily available due to the nature of the performed modifications. [ABSTRACT FROM AUTHOR]

Na1.36(Si0.86Ga0.14)2As2.98 and Li1.5Ga0.9Si3.1As4 were synthesized by heating mixtures of the elements at 950 °C. The crystal structures were determined by single crystal X-ray diffraction (Na1.36(Si0.86Ga0.14)2As2.98: I41/a, Z = 100, a = 19.8772(4) Å, c = 37.652(1) Å; Li1.5Ga0.9Si3.1As4: C2/c, Z = 8, a = 10.8838(6) Å, b = 10.8821(6) Å, c = 13.1591(7) Å). Na1.36(Si0.86Ga0.14)2As2.98 crystallizes similar to NaSi2P3 with interpenetrating networks of vertex-sharing T4 and T5 supertetrahedra. Gallium substitution at the silicon sites increases the charge of the cluster network, which is compensated for by a 36% higher sodium content. Since in contrast to NaSi2P3, all sodium sites are now fully occupied, there is no significant ion mobility, as indicated by 23Na-NMR. Consequently, the total sodium-ion conductivity of Na1.36(Si0.86Ga0.14)2As2.98 amounts to only 1.6(1) × 10−7 S cm−1 and is therefore three orders of magnitude lower than in NaSi2P3. Li1.5Ga0.9Si3.1As4 crystallizes in a new structure type with layers of edge-sharing (Si1−xGax)As4 tetrahedra alternating with layers that contain infinite Sin zigzag chains. Lithium ions reside in channels between the chains, and thus, the structure does not provide three dimensional pathways for ion conduction and the measured total Li-ion conductivity amounts to only 1.3(1) × 10−7 S cm−1. [ABSTRACT FROM AUTHOR]

In addition to providing critical knowledge of the accurate mass of ions, ion mobility‐mass spectrometry (IM‐MS) delivers complementary data relating to the conformation and size of ions in the form of an ion mobility spectrum and derived parameters, namely, the ion's mobility (K) and the IM‐derived collision cross section (CCS). However, the maximum amount of information obtained in IM‐MS measurements is not currently transferred into analytical databases including the full mobility spectra (CCS distributions) as well as capturing of additional ion species (e.g., adducts) into the same compound entry. We introduce CCSfind, a new tool for building comprehensive databases from experimental IM‐MS measurements of small molecules. CCSfind allows predicted ion species to be chosen for input chemical formulae, which are then targeted by CCSfind after parsing open source mzML input files to provide a unified set of results within a single data processing step. CCSfind can handle both chromatographically separated isomers and IM separation of isomeric ions (e.g., "protomers" or conformers of the same ion species) with simple user control over the output for new database entries in SQL format. Files of up to 1 GB can be processed in less than 2 min on a desktop computer with 32 GB RAM with computational time scaling linearly with the size of the input mzML file or the number of input molecular formulae. Results are manually reviewed, annotated with experimental settings, before committing the database where the full dataset can be retrieved. [ABSTRACT FROM AUTHOR]

Large perpendicular magnetic anisotropy (PMA) and spin-orbit torques are two essential requirements for high-density and energy-efficient spintronic devices. Recent advances in magneto-electric and magneto-ionic control of PMA and spin-orbit torques have opened a pathway to explore different oxide materials with large dielectric constant and high ion mobility. Motivated by interesting memristive properties of HfOx, here, using broadband ferromagnetic resonance measurements, we study the spin pumping in-plane to perpendicularly magnetized W(5 nm)/CoFeB(tCFB) system capped with 4 nm HfOx thin films. We find a large spin pumping and significant PMA strength for HfOx-based thin films. Using ferromagnetic thickness dependence, we also calculate the spin mixing conductance in the trilayer system which is found to be similar to MgO-based thin film stacks. These results will be highly useful for various spintronic applications with electro-static, ionic and memristive gating. [ABSTRACT FROM AUTHOR]

Tea leaves are rich in diverse bioactive compounds. The tea accession TRI 2043 is unique due to its pigmented leaves caused by anthocyanins, clonal origin, resistance to blister blight disease, and high pubescence density. Because of its peculiarity, TRI 2043 is used to produce high-quality silver tip tea, a premium type of tea that commands high prices. This study was carried out to clarify and elucidate the types of anthocyanins in this particular accession. Four different anthocyanin species were identified and quantitated as cyanidin-3-O-β-d-galactoside and delphinidin-3-O-β-d-galactoside equivalents for leaf blades and stems of the cultivar TRI 2043. The characterization was performed by comparison with commercially available reference substances and further confirmed using ion mobility high-resolution time-of-flight-mass spectrometry (IMS-HRTOF-MS). Quantitation was carried out using ultra-high-performance liquid chromatography ultraviolet–visible detection (UHPLC-UV-vis) with cyanidin-3-O-β-d-glucoside as an internal standard. E- and Z-geometric isomers of 6-p-coumaroyl derivates of delphinidin and cyanidin-3-O-β-d-galactopyranosides were observed, and collision cross section (CCS) values were determined for all four different anthocyanidin species. The content of anthocyanins in leaf blades of cultivar TRI 2043 was 856.32 ± 41.56 µg/g dry weight, with cyanidin being the more abundant anthocyanin (69.8%). Conversely, the stem material contained an anthocyanin amount of 459.5 ± 44.7 µg/g dry weight, with a higher content of delphinidin (69.6%). In summary, an enrichment strategy using analytical membrane chromatography was established to fully elucidate and quantify the anthocyanin profile of plant samples such as the special tea variety TRI 2043. [ABSTRACT FROM AUTHOR]

Meibomian Glands (MG) are sebaceous glands responsible for the production of meibum, the main component of the Tear Film Lipid Layer (TFLL). The TFLL facilitates the spread of the tear film over the ocular surface, provides stability and reduces tear evaporation. Alterations in meibum composition lead to different ocular alterations like Meibomian Gland Dysfunction (MGD) and subsequent Evaporative Dry Eye (EDE). The aim of the present study was to investigate the composition and abundance of meibum lipids and their relationship with eyelid margin abnormalities, lipid layer patterns and MG status. The study utilizes a lipidomic approach to identify and quantify lipids in meibum samples using an Elute UHPLC system. This system considered all four dimensions (mass/charge, retention time, ion mobility and intensity) to provide the accurate identification of lipid species. Samples were categorized as healthy or low/no signs of alteration (group 1) or severe signs of alteration or EDE/MGD (group 2). The current investigation found differences in Variable Importance in Projection lipid abundance between both groups for the MGD signs studied. Changes in meibum composition occur and are related to higher scores in eyelid margin hyperaemia, eyelid margin irregularity, MG orifice plugging, MG loss and lipid layer pattern. [ABSTRACT FROM AUTHOR]

Collision cross‐section values, which can be determined using ion mobility experiments, are sensitive to the structures of protein ions and useful for applications to structural biology and biophysics. Protein ions with different charge states can exhibit very different collision cross‐section values, but a comprehensive understanding of this relationship remains elusive. Here, we review cation‐to‐anion, proton‐transfer reactions (CAPTR), a method for generating a series of charge‐reduced protein cations by reacting quadrupole‐selected cations with even‐electron monoanions. The resulting CAPTR products are analyzed using a combination of ion mobility, mass spectrometry, and collisional activation. We compare CAPTR to other charge‐manipulation strategies and review the results of various CAPTR‐based experiments, exploring their contribution to a deeper understanding of the relationship between protein ion structure and charge state. [ABSTRACT FROM AUTHOR]

Identification and specific quantification of isomers in a complex biological matrix by mass spectrometry alone is not an easy task due to their identical chemical formula and therefore their same mass‐to‐charge ratio (m/z). Here, the potential of direct introduction combined with ion mobility–mass spectrometry (DI‐IM‐MS) for rapid quantification of isomers as human milk oligosaccharides (HMOs) was investigated. Differences in HMO profiles between various analyzed breast milk samples were highlighted using the single ion mobility monitoring (SIM2) acquisition for high ion mobility resolution detection. Furthermore, the Se+ (secretor) or Se− (non‐secretor) phenotype could be assigned to breast milk samples studied based on their HMO contents, especially on the response of 2′‐fucosyllactose (2'‐FL) and lacto‐N‐fucopentaose I (LNFP I). The possibility of quantifying a specific isomer in breast milk by DI‐IM‐MS was also investigated. The standard addition method allowed the determination of the 2'‐FL despite the presence of other oligosaccharides, including 3‐fucosyllactose (3‐FL) isomer in breast milk. This proof‐of‐concept study demonstrated the high potential of such an approach for the rapid and convenient quantification of isomers in complex mixtures. [ABSTRACT FROM AUTHOR]

Herein, I provide a personal perspective on high‐resolution multipass ion mobility spectrometry‐mass spectrometry (IMS‐MS), with a specific emphasis on cyclic (cIMS) and structures for lossless ion manipulations (SLIM IMS)‐based separations. My overarching goal for this perspective was to detail what I believe will be the key important areas in which IMS‐MS will help shape the bioanalytical community and especially omics‐based research. [ABSTRACT FROM AUTHOR]

Ion transport in organic mixed ionic-electronic conductors (OMIECs) is crucial due to its direct impact on device response time and operating mechanisms but is often assessed indirectly or necessitates extra assumptions. Operando x-ray fluorescence (XRF) is a powerful, direct probe for elemental characterization of bulk OMIECs and was used to directly quantify ion composition and mobility in a model OMIEC, poly(3,4-ethylenedioxythiophene)- poly(styrene sulfonate) (PEDOT:PSS), during device operation. The first cycle revealed slow electrowetting and cation-proton exchange. Subsequent cycles showed rapid response with minor cation fluctuation (~5%). Comparison with optical-tracked electrochromic fronts revealed mesoscale structure-dependent proton transport. The calculated effective ion mobility demonstrated thickness-dependent behavior, emphasizing an interfacial ion transport pathway with a higher mobile ion density. The decoupling of interfacial effects on bulk ion mobility and the decoupling of cation and proton migration elucidate ion transport in conventional and emerging OMIEC-based devices and has broader implications for other ionic conductors writ large. [ABSTRACT FROM AUTHOR]

2D lead halide perovskites with tunable optoelectronic properties through modulating inorganic components and organic spacer ligands represent a promising candidate in perovskite optoelectronics. However, an intrinsic soft lattice of perovskites gives rise to a vacancy‐mediated halide ion migration, which further affects the long‐term stability of materials as well as devices. Here, halide ion mobility is evaluated using two different 2D perovskites yielded with butylammonium (BA) for the Ruddlesden–Popper (RP) phase and butane‐1,4‐diamine (BDA) for the Dion–Jacobson (DJ) phase, respectively. By probing the halide ion migration kinetics in the physically paired 2D bromide and iodide perovskite films, the softer lattice (RP) shows a lower activation energy of 50.9 kJ mol−1 as compared to that of more rigid lattice (DJ) of 60.8 kJ mol−1. Given similar halide diffusion pathlength and halide mixing chemical potential, the binding mode (RP and DJ) can indeed dictate the overall halide ion stability. Understanding such halide ion mobility is important in designing perovskites with increased stability and performances at material and device levels. [ABSTRACT FROM AUTHOR]

The utilization of pristine graphene as an anode material in sodium-ion batteries (SIBs) is limited by its inherent chemical inertness toward Na-ions. To address this issue, we propose a two-dimensional carbon allotrope (named as TD-graphene) by assembling tricyclo[4.4.1.11,6]dodecane (C12H20) skeleton. The topological non-hexagonal feature of C12H20 increases the degree of local carbon-ring disorder and introduces additional electron-deficient regions on the surface, thus enhancing the adsorption capability of Na. TD-graphene demonstrates exceptional stability across the energetic, thermodynamic, dynamic, and mechanical aspects. As a promising anode for SIBs, it exhibits an intrinsic metallicity, an ultra-high storage capacity (1487.58 mA h g−1), a low diffusion barrier (0.20 eV), a low average open-circuit voltage (0.33 V), and a small lattice expansion (0.6%). The presence of solvents with high dielectric constants improves the adsorption and migration capability of Na. Furthermore, taking into account the limitation of single-layer materials in practical applications, we employ h-BN as a promising substrate for TD-graphene, which can boost the Na adsorption and diffusion performance. These results render TD-graphene as a promising high-performance anode material for SIBs. [ABSTRACT FROM AUTHOR]

The drift of multiply protonated poly(ethylene oxide) chains in helium in electrostatic fields of various strengths is simulated using the molecular dynamics method. The simulation results are compared with the predictions of the kinetic theory of ion mobility, which relates the effect of increasing field strength to increasing ion temperature. As would be expected, the internal temperature of the ion Tion increases with increasing random kinetic energy received by the ion from the field. However, it grows more slowly than expected in the two-temperature theory. Ion mobility is calculated as a function of the field strength E at constant gas temperature T (300 K) and as a function of T at low E. The results of these two series of calculations are compared at the same internal ion temperatures. The results coincide at Tion close to T. At high ion temperatures, they diverge somewhat (by about 8% at Tion = 600 K), which does not agree with the theory. Conformations and sizes of drifting ions, as well as their collision cross sections, calculated from the mobility, indicate that an increase in the number of attached protons leads to unfolding of the polymer chain. This effect is in satisfactory agreement with the Rayleigh criterion for the stability of a charged drop. An increase in field strength affects the collision cross section for several reasons. They include an increase in ion temperature leading to larger ion sizes, a decrease in the influence of long-range attractive interactions, and dipole alignment that is more pronounced with fewer protons attached. [ABSTRACT FROM AUTHOR]

The kinetics of O2− ions were numerically studied in He and Ar with a small admixture of O2 in a strong electric field through a Monte Carlo simulation. Cross sections for elastic scattering between O2− ions and He and Ar atoms were determined by adjusting cross section values to obtain good agreement between calculated and measured ion mobilities in pure helium and argon. Ion transport coefficients, mean energy, and detachment rate were calculated for various mole fractions of O2 and values of the reduced electric field. It was shown that the O2− ion mobility, mean energy, and detachment rate in He:O2 mixtures are much higher than those in Ar:O2 mixtures and air. A great difference between the properties of O2− ions in He–O2 and Ar–O2 mixtures was explained on the basis of the difference in the polarizability and mass for He and Ar atoms. Calculated detachment rates can be used for simulating guided ionization waves in He and Ar flows ejected into ambient air. [ABSTRACT FROM AUTHOR]

Charge accumulation usually happens on the surface of spacers under DC operation, which is susceptible to inducing surface flashover. In order to explore the surface charge accumulation mechanisms and the influences of dielectric conductivity, gas ion mobility, and temperature field on the surface charges, a time-varying charge density model at the gas–solid interface of spacers was established. The results of the simulation show that the discontinuity of the current density between the spacer bulk side and the gas ion flow is the fundamental reason for the charge accumulation on the spacer surface. Additionally, the value of current density fluxes at the interface continues to decrease with the change of the electric field, and the progress of charge transfer gradually stabilizes. Moreover, the dielectric conductivity directly affects the charge accumulation process, and there is a critical conductivity in which the effect of charge conduction in dielectrics counteracts that of gas-phase charge deposition, theoretically. When the conductivity is higher than the critical conductivity, the solid-side charge conduction is the main source of the surface charge accumulation, while the gas-phase charge deposition on the gas side plays a dominant role when the conductivity is lower than the critical conductivity. The charge accumulation is not significantly affected by gas ion mobility when the temperature is evenly distributed. However, under the temperature field with gradient distribution, the current density fluxes at the interface change, causing the polarity reverse of the accumulated charge. In the high-temperature region, the volume current density surges simultaneously with the conductivity, leading to a higher density of surface charge accumulation. Lastly, the design of spacers needs to keep the current densities on both sides of the interface as similar as possible in order to avoid excessive charge gathering in localized areas. [ABSTRACT FROM AUTHOR]

Characterization at the subunit level enables detailed mass spectrometric characterization of posttranslational modifications (PTMs) of monoclonal antibodies (mAbs). The implemented reduction often leaves the intramolecular disulfide bridges intact. Here, we present a capillary electrophoretic (CE) method based on a neutral-coated capillary for the separation of immunoglobulin G-degrading enzyme of Streptococcus pyogenes (IdeS) digested and reduced mAb subunits followed by mass spectrometry (MS), MS/MS identification, and trapped ion mobility mass spectrometry (timsTOF). Our CE approach enables the separation of (i) different subunit moieties, (ii) various reduction states, and (iii) positional isomers of these partly reduced subunit moieties. The location of the remaining disulfide bridges can be determined by middle-down electron transfer higher energy collisional dissociation (EThcD) experiments. All these CE-separated variants show differences in ion mobility in the timsTOF measurements. Applying the presented CE-MS/MS method, reduction parameters such as the use of chaotropic salts were studied. For the investigated antibodies, urea improved the subunit reduction significantly, whereas guanidine hydrochloride (GuHCl) leads to multiple signals of the same subunit in the CE separation. The presented CE-MS method is a powerful tool for the disulfide-variant characterization of mAbs on the subunit level. It enables understanding disulfide bridge reduction processes in antibodies and potentially other proteins. [ABSTRACT FROM AUTHOR]

Plasma proteomics holds immense potential for clinical research and biomarker discovery, serving as a non-invasive "liquid biopsy" for tissue sampling. Mass spectrometry (MS)-based proteomics, thanks to improvement in speed and robustness, emerges as an ideal technology for exploring the plasma proteome for its unbiased and highly specific protein identification and quantification. Despite its potential, plasma proteomics is still a challenge due to the vast dynamic range of protein abundance, hindering the detection of less abundant proteins. Different approaches can help overcome this challenge. Conventional depletion methods face limitations in cost, throughput, accuracy, and off-target depletion. Nanoparticle-based enrichment shows promise in compressing dynamic range, but cost remains a constraint. Enrichment strategies for extracellular vesicles (EVs) can enhance plasma proteome coverage dramatically, but current methods are still too laborious for large series. Neat plasma remains popular for its cost-effectiveness, time efficiency, and low volume requirement. We used a test set of 33 plasma samples for all evaluations. Samples were digested using S-Trap and analyzed on Evosep One and nanoElute coupled to a timsTOF Pro using different elution gradients and ion mobility ranges. Data were mainly analyzed using library-free searches using DIA-NN. This study explores ways to improve proteome coverage in neat plasma both in MS data acquisition and MS data analysis. We demonstrate the value of sampling smaller hydrophilic peptides, increasing chromatographic separation, and using library-free searches. Additionally, we introduce the EV boost approach, that leverages on the extracellular vesicle fraction to enhance protein identification in neat plasma samples. Globally, our optimized analysis workflow allows the quantification of over 1000 proteins in neat plasma with a 24SPD throughput. We believe that these considerations can be of help independently of the LC–MS platform used. [ABSTRACT FROM AUTHOR]

The single‐layer organic light‐emitting devices provide a promising way for low‐cost, large‐area displays. Iridium (III) complex may play an important role to achieve this target due to its unique ionic characteristics. To achieve high‐performance single‐layer devices, blending the salt additives into the active layer is an effective strategy. However, the effects of different cation and anion additives on the device's performance are still unclear. Herein, the single‐layer light‐emitting devices are fabricated by using solution‐processed iridium (III) complex mixed with various molecular salts. It is implied in the results that the improvement of the device luminescence and recombination efficiency is owing to the enhanced carrier injection and improved carrier balance in the emitting layer by the ion‐additive‐induced electrical double layer at the interface. The smaller cation can improve the carrier injection of the device more efficiently due to the stronger ion mobility and the anion with the smaller association coefficient shows a better device performance since the stronger dissociation ability of the ions can lead to a better ion migration ability. In addition, the introduction of poly (methyl methacrylate) into the active film can improve the single‐layer device performances by reducing leak current in bulk. [ABSTRACT FROM AUTHOR]

The results of previously published studies of the ion mobility, phase transitions, and electrophysical properties of tetrafluoroantimonates(iii) with heteroatomic cation sublattices composed of alkali metal and ammonium cations are analyzed, corrected, supplemented, and summarized. The influence of outer-sphere monovalent cations of different nature on the character of ion mobility, phase transitions, and conductivity in crystalline tetrafluoroantimonates(iii) is considered. It was found that phase transitions of most compounds in question are followed by the formation of superionic β-phases with a high conductivity of the order of 10−4–10−2 S cm−1 in the temperature range of 400–500 K. [ABSTRACT FROM AUTHOR]

An experimental investigation on synthesis of nanocrystalline nickels by pulsed current electrodeposition has been carried out in an additive-free Watts bath employing nickel-sulphate solution with similar nickel ion concentrations. Aluminum was used as a substrate. It demonstrated the advantage of easier removal process of electrodeposited nanocrystalline nickel from its substrate. Whereas the use of high-purity nickel anode was intended to replace nickel ions, which decreased during electrodeposition. Different peak current densities of 450, 750 and 1000 mA/cm² were applied. A pulsed current was set at a similar pulse pattern of on-time and off-time of 1 ms and 9 ms respectively. The shorter on-time demonstrated the ability to limit ion deposition, which was related to the formation of finer grains. The off-time arrangement was targeted to ensure that the ion mobility had completely stopped. Higher current density demonstrated a dominant impact on deposits, generating a higher nucleation rate that is related to depositing nanocrystalline nickel. A peak current density of 1000 mA/cm² produced grain sizes in the nanoscale regime. Without any additional additive, nanocrystalline nickel was successfully yielded. Investigation of grain size obtained from the 1000 mA/cm² has been conducted by extracting full width at half maximum peak intensity (FWHM) revealed from X-ray diffraction (XRD) and Transmission Electron Microscopy (TEM) exhibited consistent results of 22 nm and 25.4±3.4 nm, respectively. It is also evidence of the significant role of pulsed current density. In inclusion, nanocrystalline nickel can be synthesized in an electrodeposition bath without any addition of additives. [ABSTRACT FROM AUTHOR]

Natural environment hosts a considerable amount of accessible energy, comprising mechanical, thermal, and chemical potentials. Environment-induced nanogenerators are nanomaterial-based electronic chips that capture environmental energy and convert it into electricity in an environmentally friendly way. Polymers, characterized by their superior flexibility, lightweight, and ease of processing, are considered viable materials. In this paper, a thorough review and comparison of various polymer-based nanogenerators were provided, focusing on their power generation principles, key materials, power density and stability, and performance modulation methods. The latest developed nanogenerators mainly include triboelectric nanogenerators (TriboENG), piezoelectric nanogenerators (PENG), thermoelectric nanogenerators (ThermoENG), osmotic power nanogenerator (OPNG), and moist-electric generators (MENG). Potential practical applications of polymer-based nanogenerator were also summarized. The review found that polymer nanogenerators can harness a variety of energy sources, with the basic power generation mechanism centered on displacement/conduction currents induced by dipole/ion polarization, due to the non-uniform distribution of physical fields within the polymers. The performance enhancement should mainly start from strengthening the ion mobility and positive/negative ion separation in polymer materials. The development of ionic hydrogel and hydrogel matrix composites is promising for future nanogenerators and can also enable multi-energy collaborative power generation. In addition, enhancing the uneven distribution of temperature, concentration, and pressure induced by surrounding environment within polymer materials can also effectively improve output performance. Finally, the challenges faced by polymer-based nanogenerators and directions for future development were prospected. [ABSTRACT FROM AUTHOR]

The present study is aimed to formulate a numerical model to simulate hydrogeochemical reactions controlling pyrite oxidation in unsaturated aquifers under non-uniform flow conditions. A coupled flow and multi-component transport model is solved using a finite difference scheme to simulate the concentration distribution of oxygen (O2), ferrous (Fe2+), ferric (Fe3+), sulphate (SO42−) and hydrogen (H+) ions. An attempt is made to quantify the transport characteristics of pyrite oxidation ions by analysing the spatial moments of concentration profiles. The simulation results suggest that the variable flow rate in the vertical direction significantly enhances the pyrite oxidation near the ground surface. Peak concentration of Fe2+, Fe3+, and SO42− near the ground surface is found to be approximately 2–3 times higher in the case of variable flow. The pH level near the ground surface drops considerably when variable flow conditions exist in the unsaturated zone. The variation in flow parameters such as porosity, and water saturation and reaction parameters such as oxygen diffusion rate and the oxygen consumption rate are found to affect the mass and mobility of Fe2+, Fe3+, and SO42− considerably. Although there has been substantial research on hydrogeochemical events associated with pyrite oxidation in the past, there has been very less focus on the transport qualities of the ions produced in groundwater. The mobility assessment of pyrite oxidation ions in aquifer presented in the study is beneficial to understand the groundwater quality risk associated with mining and to plan and implement effective remediation strategies for the restoration of affected aquifers. [ABSTRACT FROM AUTHOR]

Gold nanoparticles (AuNPs) synthesized in the 1–3 nm range have a specific number of gold core atoms and outer protecting ligands. They have become one of the "hot topics" in recent decades because of their interesting physical and chemical properties. The characterization of their structures is usually achieved by crystal X‐ray diffraction although the structures of some AuNPs remain unknown because they have not been successfully crystallized. An alternative method for studying the structure of AuNPs is electrospray ionization–ion mobility–tandem mass spectrometry (ESI‐IM‐MSMS). This research evaluated how effectively ESI‐IM‐MSMS using the commercially available Waters Synapt XS instrument yielded useful structural information from two AuNPs; Au23(S‐tBu)16 and Au30(S‐tBu)18. The study used the maximum range of available collision energies along with ion mobility separation to measure the energy‐dependence of the product ions and their drift times which is a measure of their spatial size. For Au23(S‐tBu)16, the dissociation gave the masses of the outer protecting monomeric [RS–Au–SR] and trimeric [SR–Au–SR–Au–SR–Au–SR] staples where R = tBu, and complete dissociation of the outer layer Au and tBu groups to reveal the Au15S8 core. For Au30(S‐tBu)18, the dissociation products was primarily through the loss of the partial ligands S‐tBu and tBu from the outer protecting layer and the loss of single Au4(S‐tBu)4 unit. These results showed the that ESI‐IM‐MSMS analysis of the smaller Au23(S‐tBu)16 gave information on all it major structural components whereas for Au30(S‐tBu)18, the overall structural information was limited to the ligands of the outer layer. [ABSTRACT FROM AUTHOR]

The performance of all‐solid‐state batteries (ASSBs) relies on the Li+ transport and stability characteristics of solid electrolytes (SEs). Li3PS4 is notable for its stability against lithium metal, yet its ionic conductivity remains a limiting factor. This study leverages local structural disorder via O substitution to achieve an ionic conductivity of 1.38 mS cm−1 with an activation energy of 0.34 eV for Li3PS4−xOx (x = 0.31). Optimal O substitution transforms Li+ transport from 2D to 3D pathways with increased ion mobility. Li3PS3.69O0.31 exhibits improvements in the critical current density and stability against Li metal and retains its electrochemical stability window compared with Li3PS4. The practical implementation of Li3PS3.69O0.31 in ASSBs half‐cells, particularly when coupled with TiS2 as the cathode active material, demonstrates substantially enhanced capacity and rate performance. This work elucidates the utility of introducing local structural disorder to ameliorate SE properties and highlights the benefits of strategically combining the inherent strengths of sulfides and oxides via creating oxysulfide SEs. [ABSTRACT FROM AUTHOR]

Ion mobility in electrolytes and electrodes is an important performance parameter in electrochemical devices, particularly in batteries. In this review, the authors concentrate on the charge carrier mobility in crystalline battery materials where the diffusion basically corresponds to hopping processes between lattice sites. However, in spite of the seeming simplicity of the migration process in crystalline materials, the factors governing mobility in these materials are still debated. There are well‐accepted factors contributing to the ion mobility such as the size and the charge of the ions, but they are not sufficient to yield a complete picture of ion mobility. In this review, possible factors influencing ion mobility in crystalline battery materials are critically discussed. To gain insights into these factors, chemical trends in batteries, both as far as the charge carriers as well as the host materials are concerned, are discussed. Furthermore, fundamental questions, for example, about the nature of the migrating charge carriers, are also addressed. [ABSTRACT FROM AUTHOR]

The performance of all‐solid‐state batteries (ASSBs) relies on the Li+ transport and stability characteristics of solid electrolytes (SEs). Li3PS4 is notable for its stability against lithium metal, yet its ionic conductivity remains a limiting factor. This study leverages local structural disorder via O substitution to achieve an ionic conductivity of 1.38 mS cm−1 with an activation energy of 0.34 eV for Li3PS4−xOx (x = 0.31). Optimal O substitution transforms Li+ transport from 2D to 3D pathways with increased ion mobility. Li3PS3.69O0.31 exhibits improvements in the critical current density and stability against Li metal and retains its electrochemical stability window compared with Li3PS4. The practical implementation of Li3PS3.69O0.31 in ASSBs half‐cells, particularly when coupled with TiS2 as the cathode active material, demonstrates substantially enhanced capacity and rate performance. This work elucidates the utility of introducing local structural disorder to ameliorate SE properties and highlights the benefits of strategically combining the inherent strengths of sulfides and oxides via creating oxysulfide SEs. [ABSTRACT FROM AUTHOR]

Gangliosides are highly abundant in the human brain where they are involved in major biological events. In brain cancers, alterations of ganglioside pattern occur, some of which being correlated with neoplastic transformation, while others with tumor proliferation. Of all techniques, mass spectrometry (MS) has proven to be one of the most effective in gangliosidomics, due to its ability to characterize heterogeneous mixtures and discover species with biomarker value. This review highlights the most significant achievements of MS in the analysis of gangliosides in human brain cancers. The first part presents the latest state of MS development in the discovery of ganglioside markers in primary brain tumors, with a particular emphasis on the ion mobility separation (IMS) MS and its contribution to the elucidation of the gangliosidome associated with aggressive tumors. The second part is focused on MS of gangliosides in brain metastases, highlighting the ability of matrix-assisted laser desorption/ionization (MALDI)-MS, microfluidics-MS and tandem MS to decipher and structurally characterize species involved in the metastatic process. In the end, several conclusions and perspectives are presented, among which the need for development of reliable software and a user-friendly structural database as a search platform in brain tumor diagnostics. [ABSTRACT FROM AUTHOR]