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Abstract The degradation of lithium-ion batteries has become a concerning issue. One problem is metal ion dissolution from the cathode material, such as Mn2+ dissolution from spinel-type LiMn2O4 (LMO). However, direct observation of the dissolution process has yet to be reported. Here, we establish in-situ 1H nuclear magnetic resonance imaging (MRI) measurement as an efficient technique to observe Mn2+ dissolution from a model lithium battery with LMO as the cathode. We observe an increase in the MRI signal intensity near the cathode, confirming the dissolution of Mn2+ from the cathode to the electrolyte. Moreover, we show that Mn2+ dissolution from LMO can be suppressed using an appropriate choice of electrolytes. We believe the method developed here can answer the long-time unanswered question of when, where, and how the metal ion dissolution occurs in the lithium-ion battery electrode and can be extended to other electrochemical systems.

Abstract Lithium metal as a negative electrode material offers ten times the specific capacity of graphitic electrodes, but its rechargeable operation poses challenges like excessive and continuous interphase formation, high surface area lithium deposits and safety issues. Improving the lithium | electrolyte interface and interphase requires powerful surface analysis techniques, such as ToF-SIMS sputter depth profiling.This study investigates lithium metal sections with an SEI layer by ToF-SIMS using different sputter ions. An optimal sputter ion is chosen based on the measured ToF-SIMS sputter depth profiles and SEM analysis of the surface damage. Further, this method is adapted to lithium metal foil with an intermetallic coating. ToF-SIMS sputter depth profiles in both polarities provide comprehensive insights into the coating structure. Both investigations highlight the value of ToF-SIMS sputter depth profiling in lithium metal battery research and offer guidance for future studies.

Efficient recycling processes of lithium ion batteries are critical for advancing the sustainability of this technology. Yet, the quantitative analysis of potential electrolyte residues in wastewaters generated in the recycling process can be challenging. This study introduces a robust method that combines solid‐phase extraction with gas chromatography‐flame ionization detection for quantifying organic carbonate electrolyte solvents and their degradation products in aqueous samples. A quantitative extraction of all target analytes is achieved using the polystyrene‐divinylbenzene‐based stationary phase LiChrolut EN. Method optimization and limitations are evaluated by varying mass loading, load and elution volume, enabling preconcentration factors >250 for linear and oligomeric carbonates. More hydrophilic cyclic carbonates exhibit lower preconcentration potential due to reduced retention on the cartridge. However, limits of quantification in the water sample in a range of a few hundred ppb are achieved for cyclic carbonates (186 ppb for ethylene carbonate, 119 ppb for vinylene carbonate) and down to the single‐digit ppb range for linear and oligomeric carbonates. Additionally, effective matrix elimination is demonstrated through the removal of ionic compounds, such as conductive salts, while the extraction efficiency is independent of the matrix. In conclusion, a robust quantification method is developed, suitable for monitoring wastewater treatment processes and environmental samples.

Although lithium-ion batteries are successfully used in electronic devices and electric vehicles, the steadily increasing price of their raw materials and increasing anxiety about Li resources and reserves raise concerns about exploring cheaper and sustainable alternatives. Sodium-ion batteries are one of the most promising energy storage systems but still cannot replace the status of lithium-ion batteries. One challenge of commercialization of sodium-ion batteries is their cathode material. Inspired by layered LiTMO2 (TM = transition metal) as cathode materials for lithium-ion batteries, layered NaxTMO2 materials are investigated as cathode materials for sodium-ion batteries. Although layered NaxTMO2 materials show high theoretical capacities and operating voltage windows, their cycling stability and rate capability still need to be improved. The electrochemical behavior of layered NaxTMO2 materials is correlated to the extraction and insertion of Na atoms during charge and discharge accompanied by structural changes, respectively. Understanding these structural changes during cycling of layered NaxTMO2 materials may initiate strategies to improve their electrochemical performance. Thus, the correlation between composition, structure and synthesis of layered NaxTMO2 materials is discussed in the present paper. Besides, the structural changes during cycling of layered NaxTMO2 materials are summarized according to their crystal structure accompanied by varied stacking of TMO2 and NaO2 layers. Based on this structure information, strategies are introduced to optimize the electrochemical performance of layered NaxTMO2 using design of their bulk crystal structures, local configurations around TM atoms and surface structures.

State‐of‐the‐art ternary layered oxide cathode active materials in Li‐ion batteries (LIBs) consist of polycrystalline (PC), i.e., micron‐sized secondary particles, which in turn consist of numerous nanosized primary particles. Recent approaches to develop single crystals (SCs), i.e., single and separated micron‐sized primary particles, appear promising in terms of cycle life given their mechanical stability. However, a direct and systematic (“fair”) comparison of SC with PC in LIB cell application remains a challenge due to both differences on material level and state‐of‐charge (SoC), as SCs typically have slightly lower delithiation capacities/Li+ extraction ratios. In this work, PC and SC Li[Ni0.8Mn0.1Co0.1]O2 (NMC811) are synthesized with comparable bulk and surface characteristics from identical self‐synthesized precursors. Indeed, the cycle life of SCs is not only superior, when conventionally charged to equal upper cutoff voltage (UCV), as shown in NMC||Li and NMC||graphite cells, but also after adjusting UCVs to similar SoCs, where bigger SCs counterintuitively have even a better rate performance and cycle life.

Minor amounts of tungsten (W) are well known to improve Ni‐rich layered oxide‐based cathode active materials (CAMs) for Li ion batteries. Herein, W impacts are validated and compared for varied concentrations and incorporation routes in aqueous media for LiNi0.90Co0.06Mn0.04O2 (NCM90‐6‐4), either via modification of a precursor NixCoyMnz(OH)2 (pCAM) within a sol–gel reaction or directly during synthesis, i.e., either via an W‐based educt or during co‐precipitation in a continuously operated Couette–Taylor reactor. In particular, the sol–gel modification is shown to be beneficial and reveals >500 cycles for ≈80% state‐of‐health NCM90‐6‐4||graphite cells. It can be related to homogeneously W‐modified surface as well as smaller and elongated primary particles, whereas the latter are suggested to better compensate anisotropic lattice stress and decrease amount of microcracks, consequently minimizing further rise in surface area and the accompanied failure cascades (e.g., phase changes, metal dissolution, and crosstalk). Moreover, the different incorporation routes are shown to reveal different outcomes and demonstrate the complexity and sensitivity of W incorporation.

Abstract Despite a substantial impact on various economic and cell technology factors, the influence of electrolyte quantities is rarely addressed in research. This study examines the impact of varying electrolyte quantities on cell performance and aging processes using three different electrolytes: LP57 (1 M LiPF6 in ethylene carbonate:ethyl methyl carbonate (EC:EMC 3:7 w/w), LP572 (LP57+2 wt.% vinylene carbonate (VC)) and LP57 + absVC (18.351 mg VC). Comprehensive analytical post mortem investigations revealed that continuous excessive electrolyte decomposition determines the performance of cells using LP57, leading to enhanced irreversible lithium‐ion loss and interphase thickening with increasing electrolyte volume. Impedance rise due to the growth of the interphase was also identified as the cause of degrading cell performance with rising amounts of LP572, attributed to an increasingly pronounced consumption of VC rather than electrolyte aging effects. By varying the electrolyte quantity while maintaining a constant amount VC within the cell system, the differences in cell performance were minimized, and observed deteriorating effects were suppressed. This study demonstrates the sensitive interdependence of electrolyte volume and additive concentration, practically affecting aging behavior. Comprehensively understanding the characteristics of each individual electrolyte component and tailoring the electrolytes to cell‐specific cell properties proves to be crucial to optimize cell performance.

Aqueous processing of lithium (ion) battery cathodes based on Ni‐rich layered oxides like LiNi0.83Co0.12Mn0.05O2 (NCM) can reduce costs, increase sustainability, and pave the way for F‐free, e.g., biopolymeric binders, however, the degradation of water‐sensitive Ni‐rich NCM remains a challenge. Besides strategies like NCM coatings and processing additives, customized binders can be performance‐decisive via impacting both, electrode processing aspects (paste viscosity, particle dispersibility, etc.) and chemical interactions with NCM surface, though, a distinction between these two impacting factors is difficult given their mutual influences. For this reason, a bifunctional binder system is chosen in this work, i.e., highly viscous xanthan and low viscous pullulan, both polysaccharides known from the food industry, which realize constant viscosity and processing, finally enabling systematic investigation of binder modifications (here pullulan) with various side groups. In fact, while the rate performance remains constant, suggesting a similar composite network with comparable electronic and ionic conductivities, the modified binders affect the NCM||graphite cycle life, where a higher substitution degree of carboxymethylated pullulan can even compete with N‐methyl‐2‐pyrrolidone/polyvinylidene difluoride state‐of‐the‐art system at conventional upper charge voltage (4.2 V); while at 4.5 V water‐reasoned NCM damages get obvious, as seen by enhanced electrode cross‐talk via transition metal deposition on anode.

LiNixMnyCozO2 cathode materials combined with Si‐based anode materials are current state‐of‐the‐art high energy density chemistries for lithium ion batteries. Increasing the upper cut‐off voltage is an intriguing approach to achieve even higher energy density in lithium ion batteries. However, poor oxidation stability of the state‐of‐the‐art electrolytes leads to transition metal dissolution (TMD), migration, and deposition (TMDMD) on the negative electrode, followed by sudden and rapid capacity fade. Furthermore, the chemical instability of the lithium hexafluorophosphate causes hydro‐fluoric acid to develop, which targets the native SiOx layers on silicon anodes and breaks the chemical bond to the carboxymethylcellulose sodium salt binder. Herein, a fluorine‐rich electrolyte formulation consisting of lithium‐bis(fluorsulfonyl)imide with fluoroethylene carbonate (FEC): bis(2,2,2,) trifluoroethyl carbonate (BFEC) was applied in NMC811||10%SiOx‐90%graphite cells to achieve high oxidation stability and prevent TMD and deposition. Up‐to‐date, this is the premier electrochemical performance reported in literature with a capacity retention of 94.5% and 92.2% with 0.5 °C and 4.5 V upper cut‐off voltage cycling at 20 and 40 °C after 100 cycles, respectively. The post mortem analysis showed that stabilization is achieved by forming inorganic‐ and salt‐rich interphases that protect the electrolyte versus decomposition at the electrode.

Li/Mn‐rich layered oxide (LMR) cathode active materials promise exceptionally high practical specific discharge capacity (>250 mAh g−1) as a result of both conventional cationic and anionic oxygen redox. The latter requires electrochemical activation at high cathode potential (>4.5 V vs Li|Li+), though it is accompanied by capacity and voltage fade in the course of continuous release of lattice oxygen, layered‐to‐spinel phase transformation, redox couple shift, as well as transition metal dissolution, whereas the latter is particularly detrimental for graphite‐based anodes due to electrode crosstalk. Herein, the degradation is investigated in LMR || graphite full cells by systematically varying the voltage windows, analyzing electrochemical data and changes at the anode surface. Based on this, the optimal operational voltage window, i.e., upper and lower cutoff voltage (UCV and LCV), is elaborated to finally solve the dilemma of decent cycle life (at high UCVs) and insufficient LMR activation/capacity (at low UCV) and is shown to be superior via distinguishing between formation and postformation cycles of 4.5 and 4.3 V, respectively.

Abstract Multi‐walled carbon Nanotubes (MWCNTs) are hailed as beneficial conductive agents in Silicon (Si)‐based negative electrodes due to their unique features enlisting high electronic conductivity and the ability to offer additional space for accommodating the massive volume expansion of Si during (de‐)lithiation. However, both MWCNTs and Siirreversibly consume an enormous amount of Li inventory to principally form a Solid Electrolyte Interphase (SEI) and due to other parasitic reactions, which results in lowering the Coulombic Efficiency (CE), rapid decrease in reversible capacity, and shorter battery life.To tackle these hurdles, electrochemical prelithiation is adopted as a taming strategy to mitigate the large capacity loss (nearly reducing the first irreversible capacity by ≈60%) of MWCNT‐Si/Graphite (Gr) negative electrode‐based full‐cells. In contrast, a yardstick negative electrode utilizing commercially used Super P (Super P‐Si/Gr) showed a reduction of ≈47% after in vitro pre‐doping with lithium, which is considerably smaller compared to that of MWCNTs‐based electrode design. Furthermore, the Initial CE, life cycle, and rate capability are enhanced by prelithiation. Interestingly, prelithiation brings more impact on MWCNTs ‐Si/Gr than with Super P‐Si/Gr design. An in‐depth analysis using X‐ray photoelectron spectroscopy (XPS), RAMAN Spectroscopy, Attenuated Total Reflection Fourier Transform Infrared Spectroscopy (ATR FTIR), laser microscopy, and Scanning Electron Microscopy (SEM) reveal deeper insights into the differences in SEI layer between prelithiated MWCNTs and their Super P‐based electrode counterparts.

Abstract Lithium metal batteries are promising next‐generation rechargeable batteries with high energy density. However, the high reactivity of lithium metal leads to an undesirable growth of high surface area lithium during electrodeposition and ‐dissolution and remains a key challenge that must be addressed to enable commercialization. Modification of the Li metal surface to obtain protective coatings is a common method to overcome these challenges. In this study, the influence of the thickness of an intermetallic coating on Li metal is investigated after application by means of thermal evaporation. In addition, the relevance of pre‐treatments in reducing the native layer thickness and surface roughness by roll‐pressing Li metal prior to coating is demonstrated. Morphological analyses are performed on cross‐sections prepared under cryogenic conditions to investigate the origin of high surface area lithium growth and coating cracks after electrodeposition and ‐dissolution processes. The results obtained support the conclusion that the exclusive combination of roll‐pressed Li metal foil followed by coating reduces overvoltage and improves cycle life at elevated current densities.

The high energy density, nickel‐rich layered cathode material LiNi0.8Mn0.1Co0.1O2 (NMC811) is recognized as a promising candidate for next‐generation battery chemistries. However, due to their structural and interfacial instability, nickel‐rich NMC cathodes still face a number of challenges in practical application. For this reason, the design and development of novel electrolyte formulations, able to stabilize the nickel‐rich cathode|electrolyte interface, are highly demanded. In this work, a novel electrolyte is developed using lithium (difluoromethanesulfonyl) (trifluoromethanesulfonyl)imide (LiDFTFSI) and lithium hexafluorophosphate (LiPF6) as salt blend in an organic carbonate‐solvent based solvent mixture. The presence of LiDFTFSI notably enhances the electrochemical performance of the resulting NMC811||graphite cells. Further advancement of the considered cell chemistry is achieved by introducing the well‐known functional electrolyte additive vinylene carbonate (VC), which was found to feature a synergistic effect with LiDFTFSI. The formation of a homogenous, effective, and robust solid electrolyte interphase (SEI) as well as cathode electrolyte interphase (CEI) on the corresponding electrodes resulted in superior electrochemical performance.

Abstract Silicon has attracted considerable attention for use as high-capacity anodes of lithium-ion microbatteries. However, its extreme volume change upon (de-)lithiation still poses a challenge for adoption as it leads to severe active lithium loss that shortens the cycle life. Here, we fabricate three-dimensional monocrystalline vertical silicon nanowires on a silicon wafer using low-cost metal-assisted chemical etching, then cover them with lithium using thermal evaporation prior to the battery operation as the pre-lithiation step, to investigate its impact on electrochemical performance. To reveal the underlying physical and electrochemical mechanisms, we also process a comparative planar monocrystalline silicon. We find that pre-lithiation results in improved (de-)lithiation behavior, especially in planar silicon-based cells, while silicon nanowire-based cells exhibit low capacity in early cycles. This study sheds light on the surface design and structural modification of monocrystalline silicon nanowires with respect to pre-lithiation by lithium thermal evaporation.

Abstract Organic radical batteries (ORBs) represent a viable pathway to a more sustainable energy storage technology compared to conventional Li-ion batteries. For further materials and cell development towards competitive energy and power densities, a deeper understanding of electron transport and conductivity in organic radical polymer cathodes is required. Such electron transport is characterised by electron hopping processes, which depend on the presence of closely spaced hopping sites. Using a combination of electrochemical, electron paramagnetic resonance (EPR) spectroscopic, and theoretical molecular dynamics as well as density functional theory modelling techniques, we explored how compositional characteristics of cross-linked poly(2,2,6,6-tetramethyl-1-piperidinyloxy-4-yl methacrylate) (PTMA) polymers govern electron hopping and rationalise their impact on ORB performance. Electrochemistry and EPR spectroscopy not only show a correlation between capacity and the total number of radicals in an ORB using a PTMA cathode, but also indicates that the state-of-health degrades about twice as fast if the amount of radical is reduced by 15%. The presence of up to 3% free monomer radicals did not improve fast charging capabilities. Pulsed EPR indicated that these radicals readily dissolve into the electrolyte but a direct effect on battery degradation could not be shown. However, a qualitative impact cannot be excluded either. The work further illustrates that nitroxide units have a high affinity to the carbon black conductive additive, indicating the possibility of its participation in electron hopping. At the same time, the polymers attempt to adopt a compact conformation to increase radical–radical contact. Hence, a kinetic competition exists, which might gradually be altered towards a thermodynamically more stable configuration by repeated cycling, yet further investigations are required for its characterisation.

The purpose of this study was to investigate the calendar aging of lithium-ion batteries by using both open circuit and floating current measurements. Existing degradation studies usually focus on commercial cells. The initial electrolyte composition and formation protocol for these cells is often unknown. This study investigates the role of electrolyte additives, specifically, vinylene carbonate (VC) and fluoroethylene carbonate (FEC), in the aging process of lithium-ion batteries. The results showed that self-discharge plays a significant role in determining the severity of aging for cells without additives. Interestingly, the aging was less severe for the cells without additives as they deviated more from their original storage state of charge. It was also observed that the addition of VC and FEC had an effect on the formation and stability of the solid electrolyte interphase (SEI) layer on the surface of the carbonaceous anode. By gaining a better understanding of the aging processes and the effects of different electrolyte additives, we can improve the safety and durability of lithium-ion batteries, which is critical for their widespread adoption in various applications.

Surgery of the aortic arch remains a complex procedure, with neurological events such as stroke remaining its most dreaded complications. Changes in surgical technique and the continuous innovation in neuroprotective strategies have led to a significant decrease in cerebral and spinal events. Different modes of cerebral perfusion, varying grades of hypothermia, and a number of pharmacological strategies all aim to reduce hypoxic and ischemic cerebral injury, yet there is no evidence indicating the clear superiority of one method over another. While surgical results continue to improve, novel hybrid and interventional techniques are just entering the stage and the question of optimal neuroprotection remains up to date. Within this perspective statement, we want to shed light on the current evidence and controversies of cerebral protection in aortic arch surgery, as well as what is on the horizon in this fast-evolving field. We further present our institutional approach as a large tertiary aortic reference center.

Losses of Li inventory in lithium‐ion batteries lead to losses in capacity and can be compensated by electrode prelithiation before cell assembly or before cell formation. The approach of chemical prelithiation, for example, via Li arene complex (LAC)‐based solutions is technically an apparently simple and promising approach. Nevertheless, as shown herein on the example of Si‐based anodes and LAC solutions based on 4,4′‐dimethylbiphenyl (4,4′‐DMBP), several practical challenges need to be considered. Given their reactivity, the LAC solution can not only decompose itself within a range of a few hours, as seen by discoloration and confirmed via mass spectrometry, but can also decompose its solvent and binder of added composite electrodes. Effective prelithiation requires an excess in capacity of the LAC solution (relative to anode capacity) and optimized system characteristic conditions (time, temperature, etc.) as exemplarily shown by comparing Si‐based nanoparticles with nanowires. It is worth noting that the prelithiation degree alone does not determine the boost in cycle life, but relevantly depends on previously applied prelithiation conditions (e.g., temperature), as well.

Abstract Full exhaustion in specific energy/energy density of state‐of‐the‐art LiNixCoyMnzO2 (NCM)‐based Li‐ion batteries (LIB) is currently limited for reasons of NCM stability by upper cut‐off voltages (UCV) below 4.3 V. At higher UCV, structural decomposition triggers electrode crosstalk in the course of enhanced transition metal dissolution and leads to severe specific capacity/energy fade; in the worst case to a sudden death phenomenon (roll‐over failure). The additive lithium difluorophosphate (LiDFP) is known to suppress this by scavenging dissolved metals, but at the cost of enhanced toxicity due to the formation of organofluorophosphates (OFPs). Addition of film‐forming electrolyte additives like vinylene carbonate (VC) can intrinsically decrease OFP formation in thermally aged LiDFP‐containing electrolytes, though the benefit of this dual‐additive approach can be questioned at higher UCVs. In this work, VC is shown to decrease the formation of potentially toxic OFPs within the electrolyte during cycling at conventional UCVs but triggers OFP formation at higher UCVs. The electrolyte contains soluble VC‐polymerization products. These products are formed at the cathode during VC oxidation (and are found within the cathode electrolyte interphase (CEI), suggesting an OFP electrode crosstalk of VC decomposition species, as the OFP‐precursor molecules are shown to be formed at the anode.

Abstract LiNi1/3Mn1/3Co1/3O2 (NMC‐111) is one of the most popular cathode materials in Li‐ion batteries. However, chemical and structural instabilities of the cathode/electrolyte interface at high charge cut‐off voltages cause capacity fading. Surface modifications using metal oxides are promising candidates to suppress capacity fading. Here a systematic study on the degradation mechanism of an uncoated NMC‐111 powder electrode is presented. Moreover, the effect of an Al‐doped ZnO (Al:ZnO) coating layer on the structural and chemical stabilities of NMC‐111 electrode cycled at high charge cut‐off voltages is analyzed using X‐ray photoelectron spectroscopy, scanning electron microscopy and analytical transmission electron microscopy as well as electrochemical testing. The coating is applied to commercial NMC‐111 powder using a microwave‐assisted sol‐gel synthesis method. In the case of uncoated NMC‐111 electrodes, pitting corrosion due to hydrofluoric acid attacking the electrode surface, cation mixing, and an irreversible phase transformation from a trigonal layered to a rock‐salt phase occurs, causing capacity fading. While, in the case of Al:ZnO – coated NMC‐111 electrodes, pitting corrosion, cation mixing, and the irreversible phase transformation are mitigated. Therefore, the capacity retention and rate capability are improved as the coating layer protects the electrode surface from the direct electrolyte exposure.

Abstract Electrolytes are considered crucial for the performance of batteries, and therefore indispensable for future energy storage research. This paper presents data that describes the effect of the electrolyte composition on the ionic conductivity. In particular, the data focuses on electrolytes composed of ethylene carbonate (EC), propylene carbonate (PC), ethyl methyl carbonate (EMC), and lithium hexafluorophosphate (LiPF6). The mass ratio of EC to PC was varied, while keeping the mass ratio of (EC + PC) and EMC at fixed values of 3:7 and 1:1. The conducting salt concentration was also varied during the study. Conductivity data was obtained from electrochemical impedance spectroscopy (EIS) measurements at various temperatures. Based on the thus obtained temperature series, the activation energy for ionic conduction was determined during the analysis. The data is presented here in a machine-readable format and includes a Python package for analyzing temperature series of electrolyte conductivity according to the Arrhenius equation and EIS data. The data may be useful e.g. for the training of machine learning models or for reference prior to experiments.

All-solid-state lithium batteries performance is affected by the solid electrolyte interphase (SEI) and electrically disconnected (“dead”) Li metal. Here, via operando NMR measurements, the authors quantify the Li metal in the SEI and “dead” regions using various inorganic solid-state electrolytes.

A multilayered ternary solid polymer electrolyte (TSPE) is presented. First, the influence of polyethylene oxide degradation on cell failure, development of subsequent volatile degradation products, and cell impedance is analyzed. The low electrochemical stability window/oxidative stability (≥3.8 V) results in side‐chain oxidation and loss of active material. Subsequently, electrolyte stability is improved and a thin‐film (≤50 μm) TSPE with three functional layers is developed to match the wide‐ranging electrolyte requirements toward Li metal anodes and different cathode materials like LiNi0.6Mn0.2Co0.2O2 and LiFePO4 (NCM622, LFP). The high‐voltage stability of ≥4.75 V makes the TSPE a promising candidate in high‐voltage applications. Because of high Coulombic efficiencies in NMC622‖Li metal (99.7%) and LFP‖Li metal (99.9%) cells, the presented electrolyte enables stable long‐term cycling with great capacity retention of 86% and 94%, respectively. The temperature stability of >300 °C and the capability to prevent high surface area Li and dendrite formation (even at an areal capacity utilization of >40 mAh cm−2) contribute to high safety under a wide range of conditions.

Dieser Beitrag untersucht den Zusammenhang von Fleischalternativen und Männlichkeitskonstruktionen. Der Untersuchung wird eine theoretische Perspektive auf Geschlecht und Lebensmittel zugrunde gelegt, die es erlaubt, die Ko-Materialisierung von Fleischalternativen, Körpern und Männlichkeiten zu analysieren. Empirisch baut der Beitrag auf einem breit angelegten qualitativen Forschungsdesign auf. Im Zentrum stehen Ethnografien bei Ernährungsmessen und Expert*inneninterviews. Die Analyse zeigt, dass Fleischalternativen vom Lebensstil und der Ideologie des Veganismus getrennt positioniert und mit der Kategorie der „Flexitarier*innen“ verbunden werden. Dabei steht ‚nutritionales‘ Wissen im Vordergrund, wodurch Fleisch und Fleischalternativen als Proteinquellen inszeniert werden. Protein wiederum wird unmittelbar männlich vergeschlechtlicht, da es für den muskulösen Körper notwendig ist. Die analysierten diskursiven Praxen nehmen veganen Lebensmitteln eine unmännliche Symbolik und reproduzieren ein Männlichkeitsideal, das sich durch seine körperliche Kraft auszeichnet und sich so von Weiblichkeit abhebt.

Summary: Laser desorption/ionization-mass spectrometry (LDI-MS) is introduced as a complementary technique for the analysis of interphases formed at electrode|electrolyte interfaces in lithium ion batteries (LIBs). An understanding of these interphases is crucial for designing interphase-forming electrolyte formulations and increasing battery lifetime. Especially organic species are analyzed more effectively using LDI-MS than with established methodologies. The combination with trapped ion mobility spectrometry and tandem mass spectrometry yields additional structural information of interphase components. Furthermore, LDI-MS imaging reveals the lateral distribution of compounds on the electrode surface. Using the introduced methods, a deeper understanding of the mechanism of action of the established solid electrolyte interphase-forming electrolyte additive 3,4-dimethyloxazolidine-2,5-dione (Ala-N-CA) for silicon/graphite anodes is obtained, and active electrochemical transformation products are unambiguously identified. In the future, LDI-MS will help to provide a deeper understanding of interfacial processes in LIBs by using it in a multimodal approach with other surface analysis methods to obtain complementary information.

A major challenge of Li metal electrodes is the growth of high surface area lithium during Li deposition with a variety of possible shapes and growing mechanisms. They are reactive and lead to active lithium losses, electrolyte depletion and safety concerns due to a potential risk of short-circuits and thermal runaway. This work focuses on the mechanism of tip-growing Li dendrite as a particular high surface area lithium morphology. Its formation mechanism is well-known and is triggered during concentration polarization, i.e. during mass (Li+) transport limitations, which has been thoroughly investigated in literature with liquid electrolytes. This work aims to give a stimulating perspective on this formation mechanism by considering solid polymer electrolytes. The in-here shown absence of the characteristic “voltage noise” immediately after complete concentration polarization, being an indicator for tip-growing dendritic growth, rules out the occurrence of the particular tip-growing morphology for solid polymer electrolytes under the specific electrochemical conditions. The generally poorer kinetics of solid polymer electrolytes compared to liquid electrolytes imply lower limiting currents, i.e. lower currents to realize complete concen­tration polarization. Hence, this longer-lasting Li-deposition times in solid polymer electro­lytes are assumed to prevent tip-growing mechanism via timely enabling solid electrolyte interphase formation on fresh Li deposits, while, as stated in previous literature, in liquid electrolytes, Li dendrite tip-growth process is faster than solid electrolyte interphase forma­tion kinetics. It can be reasonably concluded that tip-growing Li dendrites are in general practically unlikely for both, (i) the lower conducting electrolytes like solid polymer electro­lytes due to enabling solid electrolyte interphase formation and (ii) good-conducting electro­lytes like liquids due to an impractically high current required for concentration polarization.

Recent advances in label-free high-throughput screening via matrix-assisted laser desorption/ionization time-of-flight (MALDI-TOF) mass spectrometry (MS) offer unprecedented opportunities for the identification of novel chemical starting points in target-based drug discovery. A clear advantage of the technology is the possibility for label-free, direct quantification of analytes with high precision and robustness. Here we have expanded the range of analytes and biology that can be addressed via MALDI-TOF HTS, by developing a method based on post-reaction pyrylium-based derivatization to detect 3-methoxytyramine, the physiological enzyme product of the catechol-O-methyltransferase (COMT) enzyme. The introduction of pyrylium-type reagents as universal derivatization strategy under aqueous conditions for molecules containing primary amines represents a valuable addition to the toolbox of MALDI-TOF assay development. Characterization of COMT's enzymatic activity and inhibition by reference inhibitors, and comparison of the results obtained in our assay with data from previous mechanistic studies validated the performance of this new method. To address the problem of isobaric interference, a source of false results in MALDI-TOF assays measuring low molecular weight analytes, we devised a differential derivatization workflow which can potentially replace other counter- or orthogonal assays in future screening campaigns. Finally, we report on the first label-free HTS campaign for the identification of COMT inhibitors performed in miniaturized 1536-well microtiter plate format via MALDI-TOF MS analysis.

The drying of electrodes for lithium-ion batteries is one of the most energy- and cost-intensive process steps in battery production. Laser-based drying processes have emerged as promising candidates for electrode manufacturing due to their direct energy input, spatial homogeneity within the laser spot, and rapid controllability. However, it is unclear to what extent electrode and cell quality are affected by higher heating and drying rates. Hybrid systems as a combination of laser- and convection-based drying were investigated in an experimental study with water-processed LFP cathodes. The manufactured electrodes were compared with purely laser-dried and purely convection-dried samples in terms of drying times and quality characteristics. The electrodes were characterized with regard to physical properties like adhesion and electronic conductivity, as well as electrochemical performance using the rate capability. Regarding adhesion and electronic conductivity, the LFP-based cathodes dried in the hybrid-drying process by laser and convection showed similar quality characteristics compared to conventionally dried cathodes, while, at the same time, significantly reducing the overall drying time. In terms of electrochemical performance, measured by the rate capability, no significant differences were found between the drying technologies used. These findings demonstrate the great potential of laser- and convection-based hybrid drying of LFP cathodes to enhance the electrode-drying process in terms of energy efficiency and operational costs.

Abstract Silicon (Si)‐based negative electrodes have attracted much attention to increase the energy density of lithium ion batteries (LIBs) but suffer from severe volume changes, leading to continuous re‐formation of the solid electrolyte interphase and consumption of active lithium. The pre‐lithiation approach with the help of positive electrode additives has emerged as a highly appealing strategy to decrease the loss of active lithium in Si‐based LIB full‐cells and enable their practical implementation. Here, the use of lithium squarate (Li2C4O4) as low‐cost and air‐stable pre‐lithiation additive for a LiNi0.6Mn0.2Co0.2O2 (NMC622)‐based positive electrode is investigated. The effect of additive oxidation on the electrode morphology and cell electrochemical properties is systematically evaluated. An increase in cycle life of NMC622||Si/graphite full‐cells is reported, which grows linearly with the initial amount of Li2C4O4, due to the extra Li+ ions provided by the additive in the first charge. Post mortem investigations of the cathode electrolyte interphase also reveal significant compositional changes and an increased occurrence of carbonates and oxidized carbon species. This study not only demonstrates the advantages of this pre‐lithiation approach but also features potential limitations for its practical application arising from the emerging porosity and gas development during decomposition of the pre‐lithiation additive.

Abstract Dual‐graphite batteries (DGBs), being an all‐graphite‐electrode variation of dual‐ion batteries (DIBs), have attracted great attention in recent years as a possible low‐cost technology for stationary energy storage due to the utilization of inexpensive graphite as a positive electrode (cathode) material. However, DGBs suffer from a low specific energy limited by the capacity of both electrode materials. In this work, a composite of black phosphorus with carbon (BP‐C) is introduced as negative electrode (anode) material for DIB full‐cells for the first time. The electrochemical behavior of the graphite || BP‐C DIB cells is then discussed in the context of DGBs and DIBs using alloying anodes. Mechanistic studies confirm the staging behavior for anion storage in the graphite positive electrode and the formation of lithiated phosphorus alloys in the negative electrode. BP‐C containing full‐cells demonstrate promising electrochemical performance with specific energies of up to 319 Wh kg–1 (related to masses of both electrode active materials) or 155 Wh kg–1 (related to masses of electrode active materials and active salt), and high Coulombic efficiency. This work provides highly relevant insights for the development of advanced high‐energy and safe DIBs incorporating BP‐C and other high‐capacity alloying materials in their anodes.

Magnesium-sulfur batteries offer several advantages compared to lithium-sulfur batteries, including a more stable anode and lower material costs. Here, the challenges and prospects for both classes of batteries are discussed, including their outlook for practical energy and cost levels.

In sub-surface drilling rigs, one key critical crisis is unwanted influx into the borehole as a result of increasing the influx rate while drilling deeper into a high-pressure gas formation. Although established risk assessments in drilling rigs provide a high degree of protection, uncertainty arises due to the behavior of the formation being drilled into, which may cause crucial situations at the rig. To overcome such uncertainties, real-time sensor measurements are used to predict, and thus prevent, such crises. In addition, new understandings of the effective events were derived from raw data. In order to avoid the computational overhead of input feature analysis that hinders time-critical prediction, EventTracker sensitivity analysis, an incremental method that can support dimensionality reduction, was applied to real-world data from 1600 features per each of the 4 wells as input and 6 time series per each of the 4 wells as output. The resulting significant input series were then introduced to two classification methods: Random Forest Classifier and Neural Networks. Performance of the EventTracker method was understood correlated with a conventional manual method that incorporated expert knowledge. More importantly, the outcome of a Neural Network Classifier was improved by reducing the number of inputs according to the results of the EventTracker feature selection. Most important of all, the generation of results of the EventTracker method took fractions of milliseconds that left plenty of time before the next bunch of data samples.

To achieve a broader public acceptance for electric vehicles based on lithium-ion battery (LIB) technology, long driving ranges, low cost, and high safety are needed. A promising pathway to address these key parameters lies in the further improvement of Ni-rich cathode materials for LIB cells. Despite the higher achieved capacities and thus energy densities, there are major drawbacks in terms of capacity retention and thermal stability (of the charged cathode) which are crucial for customer acceptance and can be mitigated by protecting cathode particles. We studied the impact of surface modifications on cycle life and thermal stability of LiNi0.90Co0.05Mn0.05O2 layered oxide cathodes with WO3 by a simple sol–gel coating process. Several advanced analytical techniques such as low-energy ion scattering, differential scanning calorimetry, and high-temperature synchrotron X-ray powder diffraction of delithiated cathode materials, as well as charge/discharge cycling give significant insights into the impact of surface coverage of the coatings on mitigating degradation mechanisms. The results show that successful surface modifications of WO3 with a surface coverage of only 20% can prolong the cycle life of an LIB cell and play a crucial role in improving the thermal stability and, hence, the safety of LIBs.

Government investment constitutes a large portion of overall investment in research and development of lithium-ion batteries (LIBs) and other future battery technologies with the goal of electrifying the transportation sector and so removing a major source of global greenhouse gas emissions. Poor investments, however, can result in taxpayer funding losses and political backlash, making clear communication and informed decision-making critical. This manuscript presents the Battery Component Readiness Level scale, an overhauled version of the Technology Readiness Level (TRL) scale currently utilized by the EU for innovation programs that has been customized for use in battery technology development. It retains the structure of the EU TRL scale while adding in-depth description of technology-specific development as well as discussion of aspects such as manufacturability and cost that are necessary to understand technological promise and risk. Its use by the EU and other parties involved in battery development can thus improve communication between all involved sectors, from government to academia to industry, and can aid in better-informed decision-making regarding investments. This can ultimately contribute to a more efficient electrification of the transportation sector and any other sectors where batteries display transformative potential.

We present a genome assembly from an individual female Ischnura elegans (the blue-tailed damselfly; Arthropoda; Insecta; Odonata; Coenagrionidae). The genome sequence is 1,723 megabases in span. The majority of the assembly (99.55%) is scaffolded into 14 chromosomal pseudomolecules, with the X sex chromosome assembled.

The implementation of orbitrap mass spectrometry for target analysis of volatile species in aged lithium-ion batteries was performed in a case study on butyl carbonates. In comparison to previously applied single quadrupole-based methods, major improvements were obtained. • Sensitivity was improved by effectively background free extracted ion chromatograms of identified marker fragment ions. • Typical isobaric interferences of typical carbonate fragment ions e.g. caused by column bleeding were identified and false positive identification avoided. • Analysis of isotope labeled electrolytes was optimized regarding mass spectrometric data reliability with mass accuracies 100,000.

Dual-graphite batteries (DGBs), which are based on anion intercalation into graphite positive electrodes, exhibit great potential for stationary energy storage due to use of more sustainable and low-cost electrode materials and processing routes. Binary-mixed highly concentrated electrolytes (HCEs) appeal highly suitable for the high operating voltages of DGBs, although the lack of sufficient insights into the formation of graphite intercalation compounds (GICs) limits the cell performance in terms of specific capacity and lifetime so far. Herein, anion intercalation from single-salt HCEs (LiPF6 and LiBF4) and an equimolar binary mixture of LiPF6/LiBF4 are studied in graphite || Li metal cells, revealing an improved performance in terms of specific capacity and Coulombic efficiency in the order LiPF6 > LiPF6/LiBF4 > LiBF4. LiBF4-based cells exhibit an increased onset potential for anion intercalation and higher area specific impedance, suggesting an ineffective interphase formation at graphite. X-ray diffraction reveals GIC formation, while a lower stage number is achieved for the LiBF4-based HCE. 19F MAS NMR spectroscopy analysis at various states-of-charge confirms no significant charge transfer between the intercalated anions and the graphite host and suggest preferred intercalation of PF6- compared to BF4- as well as a high translational and/or rotational mobility of the intercalated anions.

Aqueous processing of positive electrode active materials (AMs) could enable a more economical and environmentally friendly production of lithium‐ion batteries. Intrinsically, aqueous processing of positive AMs is hampered by lithium‐proton exchange in the AM surface, leading to a poor electrochemical performance and a resulting strong increase in the pH value in the electrode paste, thereby corroding the aluminum current collector. Herein, the influence of different lithium salts as processing additive to tailor the pH value of the electrode paste, the manganese dissolution during processing, and the electrochemical performance is described for aqueous processing of LiNi0.5Mn1.5O4‐based positive electrodes. Positive electrodes, based on an aqueous LiNi0.5Mn1.5O4‐based electrode paste which is mixed with LiN(SO2CF3)2 (LiTFSI), achieve a comparable electrochemical performance to state‐of‐the‐art nonaqueous‐processed electrodes. Manganese dissolution into the electrode paste is examined by inductively coupled plasma‐mass spectrometry (ICP‐MS), showing that the addition of lithium salts to the electrode paste substantially decreases manganese leaching during processing. Furthermore, postmortem analysis shows that the addition of LiTFSI to the electrode paste has a positive effect not only during processing but also on charge/discharge cycling performance.

Renewable energy sources have been a topic of ever-increasing interest, not least due to escalating environmental changes. The significant rise of research into energy harvesting and storage over the years has yielded a plethora of approaches and methodologies, and associated reviews of individual aspects thereof. Here, we aim at highlighting a rather new avenue within the field of batteries, the (noaqueous) all-organic redox-flow battery, albeit seeking to provide a comprehensive and wide-ranging overview of the subject matter that covers all associated aspects. This way, subject matter on a historical perspective, general types of redox-flow cells, electrolyte design and function, flow kinetics, and cell design are housed within one work, providing perspective on the all-organic redox-flow battery in a broader sense.

Summary: Further increase in the specific energy/energy density of lithium ion batteries can be achieved via further increase of charge cell voltage. However, an enhanced electrode cross-talk, i.e., transition metal (TM) dissolution from cathode and deposition on the anode, drastically limits the cycle life, even leading to rollover failure. In this work, the commonly used film-forming electrolyte additives vinylene carbonate (VC), fluoroethylene carbonate (FEC), and lithium difluorophosphate (LiDFP) are thoroughly evaluated regarding their ability to suppress the issues originating from electrode cross-talk. Neither the VC- nor the FEC-containing electrolytes can suppress it, as evidenced by the presence of Ni, Co, and Mn on the graphite anode; although different for the FEC, the deposited TMs and intertwined Li deposits are homogeneously distributed in the presence of VC. Despite suppression of rollover failure in this manner, VC still cannot compete with LiDFP because LiDFP is able to complex TMs and provide TM-scavenging agents, i.e., PO3F− and PO42−, thus, effectively suppressing electrode cross-talk in the first place and effectively preventing the concomitant failure cascade.

In the face of emerging technological achievements, cyber security remains a significant issue. Despite the new possibilities that arise with such development, these do not come without a drawback. Attackers make use of the new possibilities to take advantage of possible security defects in new systems. Advanced-persistent-threat (APT) attacks represent sophisticated attacks that are executed in multiple steps. In particular, network systems represent a common target for APT attacks where known or yet undiscovered vulnerabilities are exploited. For this reason, intrusion detection systems (IDS) are applied to identify malicious behavioural patterns in existing network datasets. In recent times, machine-learning (ML) algorithms are used to distinguish between benign and anomalous activity in such datasets. The application of such methods, especially autoencoders, has received attention for achieving good detection results for APT attacks. This paper builds on this fact and applies several autoencoder-based methods for the detection of such attack patterns in two datasets created by combining two publicly available benchmark datasets. In addition to that, statistical analysis is used to determine features to supplement the anomaly detection process. An anomaly detector is implemented and evaluated on a combination of both datasets, including two experiment instances–APT-attack detection in an independent test dataset and in a zero-day-attack test dataset. The conducted experiments provide promising results on the plausibility of features and the performance of applied algorithms. Finally, a discussion is provided with suggestions of improvements in the anomaly detector.

The here shown data support the article “The Sand Equation and its Enormous Practical Relevance for Solid-State Lithium Metal Batteries”. [1] In this data set, all cells include the poly (ethylene oxide)-based solid polymer electrolyte (PEO-based SPE). The behaviour in symmetric Li||Li cells are provided in a three-electrode cell setup, thus with the use of a reference electrode. Moreover, the Sand behaviour is reported for varied negative electrodes with the focus on polarization onset, defined as transition time. The data of the electrochemical response after the variation of additional parameter, i.e. SPE thicknesses, are shown, as well. The theoretical Sand equation is linked with practically obtained values also for varied Li salt concentration. Finally, the discharge behaviour is provided including further charge/discharge cycles with the use of LiNi0.6Mn0.2Co0.2O2 (NMC622) as active material for positive electrodes.

Summary: Single-ion conducting polymer electrolytes exhibit great potential for next-generation high-energy-density Li metal batteries, although the lack of sufficient molecular-scale insights into lithium transport mechanisms and reliable understanding of key correlations often limit the scope of modification and design of new materials. Moreover, the sensitivity to small variations of polymer chemical structures (e.g., selection of specific linkages or chemical groups) is often overlooked as potential design parameter. In this study, combined molecular dynamics simulations and experimental investigations reveal molecular-scale correlations among variations in polymer structures and Li+ transport capabilities. Based on polyamide-based single-ion conducting quasi-solid polymer electrolytes, it is demonstrated that small modifications of the polymer backbone significantly enhance the Li+ transport while governing the resulting membrane morphology. Based on the obtained insights, tailored materials with significantly improved ionic conductivity and excellent electrochemical performance are achieved and their applicability in LFP||Li and NMC||Li cells is successfully demonstrated.

Summary: Inhomogeneous lithium deposition or dendrite formation and occurrence of “dead lithium” fractions are challenging issues, hampering the commercial application of lithium metal batteries. Conditions and strategies for minimizing potential failure of lithium metal anodes are currently not fully understood, despite recent progress. We report a protocol utilizing in situ and ex situ 7Li solid-state NMR spectroscopy to quantify irreversible lithium losses in batteries, clearly distinguishing losses due to SEI formation and fractions of “dead lithium,” revealing a distribution of different lithium metal microstructures on both working and counter electrodes upon plating and stripping. Estimates of dead lithium fractions of 3.3% ± 0.6% (with 5% FEC) and 9.4% ± 0.6% (without 5% FEC) are determined. The proposed protocol affords benchmarking of commercial cells, including future design of suitable strategies for effective development and tailoring of electrolyte formulations, fostering further advancement of high-performance energy storage applications.

Summary: Frequently, poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) reveal a failure with high-voltage electrodes, e.g. LiNi0.6Mn0.2Co0.2O2 in lithium metal batteries, which can be monitored as an arbitrary appearance of a “voltage noise” during charge and can be attributed to Li dendrite-induced cell micro short circuits. This failure behavior disappears when incorporating linear PEO-based SPE in a semi-interpenetrating network (s-IPN) and even enables an adequate charge/discharge cycling performance at 40°C. An impact of any electrolyte oxidation reactions on the performance difference can be excluded, as both SPEs reveal similar (high) bulk oxidation onset potentials of ≈4.6 V versus Li|Li+. Instead, improved mechanical properties of the SPE, as revealed by compression tests, are assumed to be determining, as they mechanically better withstand Li dendrite penetration and better maintain the distance of the two electrodes, both rendering cell shorts less likely.

This work investigates the comprehensive recycling of graphite and cathode active materials (LiNi0.6Mn0.2Co0.2O2, abbreviated as NMC) from spent lithium-ion batteries via pretreatment and flotation. Specific analytical methods (SPME-GC-MS and Py-GC-MS) were utilized to identify and trace the relevant influencing factors. Two different pretreatment methods, which are Fenton oxidation and roasting, were investigated with respect to their influence on the flotation effectiveness. As a result, for NMC cathode active materials, a recovery of 90% and a maximum grade of 83% were obtained by the optimized roasting and flotation. Meanwhile, a graphite grade of 77% in the froth product was achieved, with a graphite recovery of 75%. By using SPME-GC-MS and Py-GC-MS analyses, it could be shown that, in an optimized process, an effective destruction/removal of the electrolyte and binder residues can be reached. The applied analytical tools could be integrated into the workflow, which enabled process control in terms of the pretreatment sufficiency and achievable separation in the subsequent flotation.

The flammability and toxicity of the currently used electrolytes are the concerns that must be addressed. Here the authors show a non-fluorinated and non-toxic ionomeric aqueous gel electrolyte called water-in-ionomer that allows an enlargement of electrochemical stability window and design of environmentally friendly battery cell chemistries.

The article is based on a series of surveys started in early December 2012 and ended in May 2018. The main goal of the study was a survey of the local resident breeding population of Yellow-Billed Kite (Milvus aegyptius). In total, 74 active nests and 2 inactive nests of Yellow-Billed Kite were found in surroundings of Cairo, Luxor, Lake Nasser and Abu Simbel.

In this work, silicon/carbon composites are synthesized by forming an amorphous carbon matrix around silicon nanoparticles (Si-NPs) in a hydrothermal process. The intention of this material design is to combine the beneficial properties of carbon and Si, i.e., an improved specific/volumetric capacity and capacity retention compared to the single materials when applied as a negative electrode in lithium-ion batteries (LIBs). This work focuses on the influence of the Si content (up to 20 wt %) on the electrochemical performance, on the morphology and structure of the composite materials, as well as the resilience of the hydrothermal carbon against the volumetric changes of Si, in order to examine the opportunities and limitations of the applied matrix approach. Compared to a physical mixture of Si-NPs and the pure carbon matrix, the synthesized composites show a strong improvement in long-term cycling performance (capacity retention after 103 cycles: ≈55% (20 wt % Si composite) and ≈75% (10 wt % Si composite)), indicating that a homogeneous embedding of Si into the amorphous carbon matrix has a highly beneficial effect. The most promising Si/C composite is also studied in a LIB full cell vs a NMC-111 cathode; such a configuration is very seldom reported in the literature. More specifically, the influence of electrochemical prelithiation on the cycling performance in this full cell set-up is studied and compared to non-prelithiated full cells. While prelithiation is able to remarkably enhance the initial capacity of the full cell by ≈18 mAh g−1, this effect diminishes with continued cycling and only a slightly enhanced capacity of ≈5 mAh g−1 is maintained after 150 cycles.