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Abstract Promoting safer and more cost‐effective lithium‐ion battery manufacturing practices, while also advancing recycling initiatives, is intrinsically tied to reducing reliance on fluorinated polymers like polyvinylidene difluoride (PVDF) as binders and minimizing the use of hazardous and expensive solvents such as N‐methyl pyrrolidone (NMP). In pursuit of this objective, olefin‐ and rubber‐based polymers have been investigated as promising alternatives for binder materials in high‐energy Ni‐rich LiNixCoyMnzO2 (NCM, x≥0.8) cathodes for lithium‐ion batteries (LIBs). Alternative binders such as polyisobutylene (PIB), poly(styrene‐butadiene‐styrene) (SBS), nitrile butadiene rubber (NBR), and its hydrogenated version (HNBR) offer versatile solutions. These polymers can be dissolved in industrial solvents, such as toluene, and have been further processed into homogeneous cathode slurries, thus facilitating the manufacturing of high‐energy Ni‐rich NCM cathodes for lithium‐ion batteries. The evaluation of NCM811 cathodes obtained from PIB, SBS, NBR, and HNBR has involved a thorough assessment of their physical and chemical properties, electrochemical performance, and production expenses, compared with NCM811 cathodes based on PVDF. Notably, cathodes employing PIB and HNBR have exhibited outstanding qualities, showcasing high specific capacity and remarkable electrochemical stability akin to PVDF‐based counterparts. Furthermore, the alternative binders′ superior adhesion, elasticity, and thermal stability have facilitated obtaining uniform and mechanically stable cathode films. Furthermore, using toluene, with its low vapor pressure, has significantly reduced energy costs associated with drying processes, thereby enhancing the overall cost‐effectiveness of the NCM811 cathodes.

The aqueous processing of cathode materials for lithium-ion batteries (LIBs) has both environmental and cost benefits. However, high-loading, water-based electrodes from the layered oxides (e.g., NMC) typically exhibit worse electrochemical performance than NMP-based electrodes. In this work, primary, binary, and ternary binder mixtures of aqueous binders such as CMC, PAA, PEO, SBR, and Na alginate, in combination with bare and C-coated Al current collectors, were explored, aiming to improve the rate capability performance of NMC811 electrodes with high areal capacity (≥4 mAh cm−2) and low binder content (3 wt.%). Electrodes with a ternary binder composition (CMC:PAA:SBR) have the best performance with bare Al current collectors, attaining a specific capacity of 150 mAh g−1 at 1C. Using carbon-coated Al current collectors results in improved performance for both water- and NMP-based electrodes. This is further accentuated for Na-Alg and CMC:PAA binder compositions. These electrodes show specific capacities of 170 and 80 mAh g−1 at 1C and 2C, respectively. Although the specific capacities at 1C are comparable to those for NMP-PVDF electrodes, they are approximately 50% higher at the 2C rate. This study aims to contribute to the development of sustainably processed NMC electrodes for high energy density LIBs using water as solvent.

Magnesium-ion batteries represent promising environmentally sustainable energy-storage systems with higher energy densities than their lithium counterparts. In this work, the charge storage mechanisms of the olivine-related compound (Mg0.5Ni0.5)3(PO4)2 using Mg2+ and Li+ ions were investigated and compared for the first time when copper was chosen as the current collector. A comprehensive physicochemical and electrochemical characterization was performed on the pristine powder and electrodes at different states of charge. Although (Mg0.5Ni0.5)3(PO4)2 is electrochemically active, it undergoes irreversible conversion reactions in both Mg and Li chemistries. The conversion reactions proceed with an ionic exchange between structural Ni2+ and Mg2+ or Li+ cations, which results in the formation of sarcopside-Mg3(PO4)2, a Cu–Ni alloy and poorly crystalline Li3PO4, respectively. A capacity of 600 mA h g−1 was achieved with a Li metal counter electrode in the Li cell since the conversion reaction could go to completion. A capacity of 92 mA h g−1 was delivered in the Mg cell using an activated carbon counter electrode. These findings shed light on the fundamental mechanism of activity in olivine-related compounds, underlining the importance of performing systematic studies to unveil the complex interactions between both single-valent and multivalent ions with novel structures.

Multi-layer coating of electrodes with different material compositions helps unlock the full potential of high-loaded electrodes. Within this work, LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes with an areal capacity of >8.5 mA h cm−2 and tuned binder concentrations were fabricated by using an industrially relevant roll-to-roll process. Rate capability tests revealed an increase in practical specific discharge capacity independent from the C-rate for cathodes with reduced binder concentration in the top layer. At high current densities (C-rate of 1C) an improved performance of up to 27% was achieved. Additionally, at lower C-rates, binder gradients perpendicular to the current collector have beneficial effects on thick electrodes. However, surface analysis and electrochemical impedance spectroscopy revealed that without an adequate connection between the active material particles through a carbon-binder domain, charge transfer resistance limits cycling performance at high current densities.

Developing high specific energy Lithium-ion (Li-ion) batteries is of vital importance to boost the production of efficient electric vehicles able to meet the customers’ expectation related to the electric range of the vehicle. One possible pathway to high specific energy is to increase the operating voltage of the Li-ion cell. Cathode materials enabling operation above 4.2 V are available. The stability of the positive electrode-electrolyte interface is still the main bottleneck to develop high voltage cells.Moreover, important research efforts are devoted to the substitution of graphite anodes with Li metal: this would improve the energy density of the cell dramatically. The use of metallic lithium is prevented by the dendrite growth during charge, with consequent safety problems. To suppress the formation of dendrites solid-state electrolytes are considered the most promising approach.For these reasons the present review summarizes the most recent research efforts in the field of high voltage solid-state electrolytes for high energy density Li-ion cells.

The chemical diffusion coefficient in LiNi1/3Mn1/3Co1/3O2 was determined via the galvanostatic intermittent titration technique in the voltage range 3 to 4.2 V. Calculated diffusion coefficients in these layered oxide cathodes during charging and discharging reach a minimum at the open-circuit voltage of 3.8 V and 3.7 V vs. Li/Li+, respectively. The observed minima of the chemical diffusion coefficients indicate a phase transition in this voltage range. The unit cell parameters of LiNi1/3Mn1/3Co1/3O2 cathodes were determined at different lithiation states using ex situ crystallographic analysis. It was shown that the unit cell parameter variation correlates well with the observed values for chemical diffusion in NMC cathodes; with a notable change in absolute values in the same voltage range. We relate the observed variation in unit cell parameters to the nickel conversion into the trivalent state, which is Jahn-Teller active, and to the re-arrangement of lithium ions and vacancies.

Manufacturing thick electrodes for Li-ion batteries is a challenging task to fulfill, but leads to higher energy densities inside the cell. Water-based processing even adds an extra level of complexity to the procedure. The focus of this work is to implement a multi-layered coating in an industrially relevant process, to overcome issues in electrode integrity and to enable high electrochemical performance. LiNi0.8Mn0.1Co0.1O2 (NMC811) was used as the active material to fabricate single- and multi-layered cathodes with areal capacities of 8.6 mA h cm−2. A detailed description of the manufacturing process is given to establish thick defect-free aqueous electrodes. Good inter-layer cohesion and adhesion to the current collector foil are achieved by multi-layering, as confirmed by optical analysis and peel testing. Furthermore, full cells were assembled and rate capability tests were performed. These tests show that by multi-layering, an increase in specific discharge capacity (e.g., 20.7% increase for C/10) can be established for all tested C-rates.

Coating conducting polymers onto active cathode materials has been proven to mitigate issues at high current densities stemming from the limited conducting abilities of the metal-oxides. In the present study, a carbon coating was applied onto nickel-rich NMC622 via polymerisation of furfuryl alcohol, followed by calcination, for the first time. The formation of a uniform amorphous carbon layer was observed with scanning- and transmission-electron microscopy (SEM and TEM) and X-ray photoelectron spectroscopy (XPS). The stability of the coated active material was confirmed and the electrochemical behaviour as well as the cycling stability was evaluated. The impact of the heat treatment on the electrochemical performance was studied systematically and was shown to improve cycling and high current performance alike. In-depth investigations of polymer coated samples show that the improved performance can be correlated with the calcination temperatures. In particular, a heat treatment at 400 °C leads to enhanced reversibility and capacity retention even after 400 cycles. At 10C, the discharge capacity for carbon coated NMC increases by nearly 50% compared to uncoated samples. This study clearly shows for the first time the synergetic effects of a furfuryl polymer coating and subsequent calcination leading to improved electrochemical performance of nickel-rich NMC622.

The end-of-life event of the battery system of an electric vehicle is defined by a fixed end-of-life threshold value. However, this kind of end-of-life threshold does not capture the application and battery characteristics and, consequently, it has a low accuracy in describing the real end-of-life event. This paper proposes a systematic methodology to determine the end-of-life threshold that describes accurately the end-of-life event. The proposed methodology can be divided into three phases. In the first phase, the health indicators that represent the aging behavior of the battery are defined. In the second phase, the application specifications and battery characteristics are evaluated to generate the end-of-life criteria. Finally, in the third phase, the simulation environment used to calculate the end-of-life threshold is designed. In this third phase, the electric-thermal behavior of the battery at different aging conditions is simulated using an electro-thermal equivalent circuit model. The proposed methodology is applied to a high-energy electric vehicle application and to a high-power electric vehicle application. The stated hypotheses and the calculated end-of-life threshold of the high-energy application are empirically validated. The study shows that commonly assumed 80 or 70% EOL thresholds could lead to mayor under or over lifespan estimations.

Surface degradation of Ni-enriched layered cathode material Li[Ni0.6Mn0.2Co0.2]O2 (NMC622) is the main reason that leads to large capacity decay during long-term cycling. In the frame of this research, an amorphous SiO2 coating was applied onto the surface of the commercially available NMC622 powder by a wet coating process, through the condensation reaction of tetraethyl orthosilicate. The chemical composition of the coating layer was analyzed by inductively-coupled plasma. The morphology was studied by scanning electron microscopy and transmission electron microscopy. Electrochemical properties, including cyclic voltammetry, galvanostatic cycling, and rate capability measurements in a half-cell configuration, were tested to compare the electrochemical behavior of the non-coated and coated NMC622 materials. It is shown that the rate performance of the NMC622 materials is not affected by the coating layer. After 700 cycles in the range of 3.0−4.3 V at 2 C discharge, the cells with SiO2-coated NMC622 materials retained 80% of their initial capacity, which is higher than the uncoated ones (74%). Physicochemical characterizations, e.g., XRD and SEM, were performed post-mortem to reveal the stabilizing mechanism of the SiO2-coated NMC622 electrodes after long-term cycling. Based on these results, this is due to the shielding effect of the coating between the NMC622 particle surface and the liquid electrolyte, along with its scavenging effect on HF. SiO2 coating is therefore a facile surface modification method that results in potentially significant enhancement of the cyclic stability of Ni-rich NMC materials.

Aberrant liquid-to-solid phase transitions of biomolecular condensates have been linked to various neurodegenerative diseases. However, the underlying molecular interactions that drive aging remain enigmatic. Here, we develop quantitative time-resolved crosslinking mass spectrometry to monitor protein interactions and dynamics inside condensates formed by the protein fused in sarcoma (FUS). We identify misfolding of the RNA recognition motif of FUS as a key driver of condensate aging. We demonstrate that the small heat shock protein HspB8 partitions into FUS condensates via its intrinsically disordered domain and prevents condensate hardening via condensate-specific interactions that are mediated by its α-crystallin domain (αCD). These αCD-mediated interactions are altered in a disease-associated mutant of HspB8, which abrogates the ability of HspB8 to prevent condensate hardening. We propose that stabilizing aggregation-prone folded RNA-binding domains inside condensates by molecular chaperones may be a general mechanism to prevent aberrant phase transitions.

This paper presents a set of norm-creative innovation tactics developed in collaborative design research projects with the objective of creating more inclusive solutions. Unawareness of social norms are exemplified through some of the flaws design has contributed to. The norm-creative approach explored in this paper involves a first step of being norm-critical, i.e. challenging social norms that contributes to inequalities and social exclusion, and a second step of being norm-creative, i.e. developing design solutions that counteract such norms through design thinking of what might be. The tactics were developed by extracting and articulating knowledge and experiences from various strands of design methodologies, successively tweaked with norm-creative perspectives and then probed in a series of collaborative design projects. The resulting tactics serve three key roles: Firstly, they contribute in iterative explorations of several stances and action possibilities. Secondly, they promote change of awareness through increasing understanding of diverse user experiences and social exclusion, and thirdly, they contribute both in thinking new about what is and what might be, thereby affording innovative prospects. Tactics for norm-creative innovation can for these reasons be one way of raising awareness and contributing to social sustainability through design. Keywords: Norm-creative innovation tactics, Design methods, Social sustainability

Non-centrosomal microtubule bundles play important roles in cellular organization and function. Although many diverse proteins are known that can bundle microtubules, biochemical mechanisms by which cells could locally control the nucleation and formation of microtubule bundles are understudied. Here, we demonstrate that the concentration of tubulin into a condensed, liquid-like compartment composed of the unstructured neuronal protein tau is sufficient to nucleate microtubule bundles. We show that, under conditions of macro-molecular crowding, tau forms liquid-like drops. Tubulin partitions into these drops, efficiently increasing tubulin concentration and driving the nucleation of microtubules. These growing microtubules form bundles, which deform the drops while remaining enclosed by diffusible tau molecules exhibiting a liquid-like behavior. Our data suggest that condensed compartments of microtubule bundling proteins could promote the local formation of microtubule bundles in neurons by acting as non-centrosomal microtubule nucleation centers and that liquid-like tau encapsulation could provide both stability and plasticity to long axonal microtubule bundles.