Electrochemical Performance Of Cell Research Articles

Laser structuring of high mass loaded and aqueous acid processed Li(Ni0.6Mn0.2Co0.2)O2 cathodes for lithium-ion batteries

Aqueous processing of cathode is a practical method to achieve cost reduction for lithium-ion batteries and provide environmentally friendly production by avoiding the use of the state-of-the-art polyvinylidene fluoride binder and toxic N-methyl-2-pyrrolidone solvent. However, the reaction of cathode materials with water leads to lithium leaching and a slurry pH value larger than 8. This results in chemical corrosion on current collector during coating process, leaving cavities inside dried electrodes. In this work, different acid additions were applied during mixing process in order to adjust slurry pH value. Besides, thick-film Li(Ni0.6Mn0.2Co0.2)O2 cathodes were manufactured to achieve a high mass loading of about 35 mg/cm2. X-ray photoelectron spectroscopy and Raman spectroscopy were applied to characterize the electrodes. Meanwhile, three-dimensional (3D) structures were generated in aqueous processed thick-film electrodes by applying ultrafast laser patterning and the active mass loss was adjusted to 7.5 %. Rate capability analyses, long-term performance, impedance spectroscopy, and cyclic voltammetry measurements were conducted to compare the electrochemical performance of cells with different cathode types. Rate capability analyses reveal that cells with structured aqueous processed thick electrodes with phosphoric acid and acetic acid show higher discharge capacity at specific current >80 mA/g in comparison to ones with PVDF. Besides, cells containing structured high mass loaded electrodes with phosphoric acid maintain 72 % capacity, which is 15 % higher than the reference cells with PVDF.

An effective cellulose triacetate interlayer to construct a dendrite-free zinc anode for advanced aqueous zinc-ion batteries

For Zn anodes of aqueous rechargeable zinc-ion batteries, the poor electrochemical performance caused by undesirable zinc dendritic formation and side reactions limit their practical application. Herein, a Zn2+ redistributor is created to reduce dendrites growth by inserting a cellulose triacetate (CTA) film as an interlayer between the zinc anode and the separator. The zinc dendritic formation and side reactions can be suppressed by the CTA interlayer. Consequently, the Zn anode covered by CTA interlayer exhibits highly reversible plating/stripping behavior with lifetime exceeding 2500 h and 600 h at current densities of 1 and 5 mA cm−2, respectively. In particular, the electrochemical performance of the full cells is investigated by using VO2 as the cathode and the CTA as interlayer. The Zn + CTA||VO2 full cells exhibit superior performance including high reversible capacity (490.2 mAh g−1 at 0.2 A g−1), excellent cycle performance (60.2% and 71.5% capacity retention after 5000 cycles at 5 A g−1 and 10 A g−1) and superior rate performance. This work demonstrates that designing a CTA interlayer is considered a cost-effective strategy to light up the practical application of aqueous zinc-ion batteries.

Ultra‐High Capacity and Cyclability of β‐phase Ca0.14V2O5as a Promising Cathode in Calcium‐Ion Batteries

AbstractCrystalline water‐free β‐phase Ca0.14V2O5is reported for the first time as a viable cathode material for calcium‐ion batteries (CIBs). In contrast to layered α‐V2O5and δ‐CaxV2O5·nH2O, which have limited capacity, the β‐phase delivers a reversible capacity of ≈247 mAh g−1, which corresponds to the insertion/extraction of Ca2+between Ca0.14V2O5and Ca1.0V2O5. The process of Ca2+insertion process and the accompanying structural relaxation are theoretically and experimentally verified. The initial insertion of Ca2+into Ca0.14V2O5causes a slight shift of oxygen atoms surrounding hepta‐coordination sites, creating penta‐coordinated sites that are then partially filled up to Ca0.33V2O5. Further insertion occurs through the stepwise occupation of up to 50% of neighboring hexa‐ and tetra‐coordination sites to form Ca0.67V2O5and Ca1.0V2O5, respectively. The rearrangement of oxygen atoms in Ca0.14V2O5also minimizes dimensional changes, leading to high cyclic stability during repeated charge/discharge cycles. The remarkable electrochemical performance of full cells containing a Ca0.14V2O5cathode and a K metal anode in Ca2+/K+hybrid electrolytes, is also demonstrated, thanks to the inertness of K+insertion into Ca0.14V2O5and the absence of calcium plating/stripping. The cyclic stability and high capacity of Ca0.14V2O5is not compromised in hybrid electrolytes, making it a viable CIB cathode.

Solid electrolyte interphase-ization of Mg2+-blocking layers for lithium ions in anode-free rechargeable lithium metal batteries

A novel concept of solid electrolyte interphase (SEI)-ization of Mg2+-blocking layers for Li+ ions and its effect on their deposition in anode-free rechargeable Li-metal batteries (AFLMBs) has been introduced. The deposition quality of Li on Cu current collectors (CCs) has been improved by the addition of a moderate amount of Mg(N(CF3SO2)2)2 co-salt in Li+-containing carbonate-based electrolytes (Li–Mg electrolytes). Additional analyses revealed that thin, dense, and stable surface layers exhibiting permeability for Li+ and impermeability for Mg2+ ions were formed in Li–Mg electrolytes, significantly suppressing the Li dendrite growth and enhancing the deposited Li metal/Cu CC surface binding. As a result, the Mg2+-blocking layers acted as effective SEI layers from the perspective of Li+ ions, positively influencing the electrochemical performance of the AFLMB full cells.

Functional ceramic support as an independent catalyst layer for direct liquid fuel solid oxide fuel cells

A porous ceramic support is designed as a multi-functional independent catalyst layer for solid oxide fuel cells (SOFCs) running on liquid hydrocarbon fuel. The layer consists of a highly porous Ce_0.9Ca_0.1O_{2−<i>δ</i>} ceramic backbone and active NiMo catalysts, which could be integrated into the conventional Ni metal containing the anode for internal reforming of the hydrocarbon fuel. Compared to conventional catalyst layers sintered on the anodes, this independent catalyst layer could be simply assembled on top of the anode without additional sintering, thereby avoiding the mismatch of the thermal expansion coefficient between the catalyst layer and the anode and improving stability of a single cell. Moreover, a current collector layer could be inserted between the catalyst and the anode to enhance current collection efficiency and electrochemical performance of the single cell. At 750 ℃, the independent catalyst layer displays high activity towards the catalytic decomposition of methanol, and the single cell could achieve the maximum power density of 400–500 mW·cm⁻² in dry methanol. Furthermore, by employing the independent catalyst layer, the single cell offers additional <i>in-situ</i> catalyst regeneration capability under the methanol operation mode. Feeding 10 mL·min⁻¹ air into an anode channel for 5 min is found to be effective to burn out carbon species in the catalyst layer, which reduces the degradation rate of the cell voltage by orders of magnitude from 2.6 to 0.024 mV·h⁻¹ during the operation of 360 h in dry methanol. The results demonstrate the significance of the independent catalyst layer design for direct internal reforming methanol fuel cells.

A reversible perovskite air electrode for active and durable oxygen reduction and evolution reactions via the A-site entropy engineering

The performance of reversible solid oxide electrochemical cells (R-SOECs) is largely hindered by the insufficient electroactivity and poor durability of the bifunctional air electrodes, where the oxygen reduction and evolution reactions (ORR and OER) occur. Here, we report our findings in boosting the electrochemical activity and durability of an air electrode with Pr0.2Ba0.2Sr0.2La0.2Ca0.2CoO3-δ (PBSLCC) via an A-site entropy engineering. The PBSLCC electrode shows enhanced oxygen reaction activity and excellent durability compared to binary and ternary double perovskites (PrBaCo2O5+δ and Pr0.8Ba0.8Ca0.4Co2O5+δ, respectively). A low and nearly unchanged area-specific resistance of 0.042 Ω cm2 is achieved at 750 °C during the 225-h stability test. La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte-supported cells with the PBSLCC air electrode show remarkable performance at 800 °C, demonstrating a peak power density of 1.2 W cm−2 in the fuel cell mode, and a current density of −1.1 A cm−2 at 1.3 V in the electrolysis mode while maintaining the excellent cycling durability of 228 h at ±0.5 A cm−2 under humidified H2 (10% H2O). A bulk oxygen p-band center model is applied to verify that tailoring of the A-site entropy strongly influences the surface exchange coefficients (k*chem), leading to higher oxygen reaction activity of PBSLCC than the binary and ternary perovskites. This study opens a new class of high-entropy perovskites for the rational design of air electrodes for R-SOECs with high activity and durability.

Simultaneous characterizations of segmented electrochemical characteristics and temperature distribution in the hythane-fueled direct internal reforming solid oxide fuel cell

The solid oxide fuel cell with direct internal reforming is promising for cost-effective utilization of hythane produced by blending hydrogen in natural gas. Deep understanding of the inhomogeneous distributions of physiochemical processes is essential to assist in optimization of hythane-fueled fuel cell. In this work, the effects of H2 blending ratio and steam-to-carbon ratio on local electrochemical performance and temperature of a segmented cell are comprehensively examined. Local electrochemical processes are clarified by various electrochemical impedance spectroscopy investigation approaches including analysis of differences in impedance spectra, distribution of relaxation times, and equivalent circuit model fitting. H2 blending reduces the concentration overpotential significantly while also homogenizing the reforming distribution and promoting the anodic electrochemical process in all segments. H2 blending ratio above 20 % greatly reduces the cold spots induced by endothermic reforming but results in hot spots in the gas outlet when the voltage is below 0.7 V because of high electrochemical reaction heat. Regardless of the H2 blending or steam-to-carbon ratio, a nearly thermal neutral state is observed at current density of 300 mA cm−2. These findings demonstrate the potential of boosting performance and simultaneously maintaining homogeneous temperature in the direct internal reforming solid oxide fuel cells.

Stepwise optimization of single-ion conducting polymer electrolytes for high-performance lithium-metal batteries

Single-ion conducting polymer electrolytes (SIPEs) are promising candidates for high-energy and high-safety lithium-metal batteries (LMBs). However, their insufficient ionic conductivity and electrochemical stability hinder their practical application. Herein, three new SIPEs, i.e., poly (1,4-phenylene ether ether sulfone)-Li (PEES-Li), polysulfone-Li (PSF-Li), and hexafluoropolysulfone-Li (6FPSF-Li), all containing covalently tethered perfluorinated ionic side chains, have been designed, synthesized, and compared to investigate the influence of the backbone chemistry and the concentration of the ionic group on their electrochemical properties and cell performance. Especially, the trifluoromethyl group in the backbone and the concentration of the ionic function appear to play an essential role for the charge transport and stability towards oxidation, and the combination of both yields the best-performing SIPE with high ionic conductivity of ca. 2.5 × 10−4 S cm−1, anodic stability of more than 4.8 V, and the by far highest capacity retention in Li‖LiNi0.6Co0.2Mn0.2O2 cells.

Dynamic Multi-Dimensional Numerical Transport Study of Lithium-Ion Battery Active Material Microstructures for Automotive Applications

In support of GM’s traction battery efforts, we derived and implemented a method to describe the electrochemical performance of a battery cell considering the nuances of the electrode microstructure at the anode and the cathode and the corresponding impact on the electrochemical transport in the solid and liquid phases. To assess the capability of the method, we compared model results from the microstructure framework with the commonly used continuum-level porous electrode model, commonly referred to as the pseudo-2-dimensional model, or the Newman Model. The microstructure modeling framework was applied to simulate the electrochemical and transport processes within the battery cell to predict the concentration gradients, local state-of-charge distributions, reaction distributions, and the overall terminal voltage of the system. In this report, we provide a commentary on the validity and practicality of the microstructure approach to drive battery cell design.

Electrochemical Performance of Galvanic Cell with Silver Coated Cathode in One Compartment System Using Seawater as Electrolyte

This research was carried out to evaluate the electrochemical performance of a galvanic cell using seawater as an electrolyte. The cell was designed to have a volume of 200 mL and equipped with Zn as an anode and Ag-coated Cu as a cathode (Cu(Ag)-Zn system) in order to suppress the corrosion of Cu. As a comparison, the same experiment with the use of uncoated Cu as a cathode (Cu-Zn system) was also conducted. To conduct the experiment, a system was assembled by connecting 20 cells in series and placed in a closed container filled with seawater. The experiment was run for 72 hours, divided into three 24-hour cycles, by replacing the seawater every 24 hours. The performance of the system was evaluated in terms of open circuit voltage, close circuit voltage, current, light intensity, internal resistance, and power. The experimental results show that the corrosion rate of Cu coated with silver was smaller than that of uncoated Cu. Compared to the performance of the Cu-Zn system, it was also found that the Cu(Ag)-Zn system produced higher power and light intensity, which is in accordance with its smaller internal resistance. The overall experimental results indicate better performance of Cu(Ag)-Zn system and this better performance is attributed to the significantly lower corrosion rate of Cu(Ag) cathode which signifies the role of Ag layer to protect the Cu from attack by seawater. As a result, the Cu(Ag)-Zn system maintained the cathode corrosion rate with a ratio of 0.19. The percentage decrease of the OCV of the Cu(Ag)-Zn system was 6.14%, the CCV on the third day was 0.99%, the current was 36.68%, and the power was 37.83%.

Robust Cross‐Linked Na3V2(PO4)2F3 Full Sodium‐Ion Batteries

Sodium‐ion batteries (SIBs) have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium‐ion batteries (LIBs). Na3V2(PO4)2F3 (NVPF) as a common cathode of SIBs, features the merits of high operating voltage, small volume change and favorable specific energy density. However, it suffers from poor cycling stability and rate performance induced by its low intrinsic conductivity. Herein, we propose an ingenious strategy targeting superior SIBs through cross‐linked NVPF with multi‐dimensional nanocarbon frameworks composed of amorphous carbon and carbon nanotubes (NVPF@C@CNTs). This rational design ensures favorable particle size for shortened sodium ion transmission pathway as well as improved electronic transfer network, thus leading to enhanced charge transfer kinetics and superior cycling stability. Benefited from this unique structure, significantly improved electrochemical properties are obtained, including high specific capacity (126.9 mAh g−1 at 1 C, 1 C = 128 mA g−1) and remarkably improved long‐term cycling stability with 93.9% capacity retention after 1000 cycles at 20 C. The energy density of 286.8 Wh kg−1 can be reached for full cells with hard carbon as anode (NVPF@C@CNTs//HC). Additionally, the electrochemical performance of the full cell at high temperature is also investigated (95.3 mAh g−1 after 100 cycles at 1 C at 50 °C). Such nanoscale dual‐carbon networks engineering and thorough discussion of ion diffusion kinetics might make contributions to accelerating the process of phosphate cathodes in SIBs for large‐scale energy storages.

Novel macaroni‐sponge‐like pore structure biomass (Zingiber officinale Rosc. leaves)‐based electrode material for excellent energy gravimetric supercapacitor

AbstractBACKGROUNDBiomass‐based porous carbon as the basic component of electrodes has received wide interest as a renewable energy storage device with high chemical–physical stability and environmental friendliness. Therefore, novel biomass waste based on Zingiber officinale Rosc./red ginger leaves was synthesized as an electrode‐based carbon material with an abundance of unique macaroni‐sponge‐like hierarchical pore structure, as well as good chemical, physical and economic performance. Template/metal–organic framework‐free red ginger leaf‐based hierarchical porous carbon (RGPC) was prepared using a facile and zero‐residue technique as electrode material for supercapacitor application.RESULTSAdditionally, ZnCl2 impregnation with concentrations of 0.1, 0.3 and 0.5 mol L−1 was utilized for increasing the active sites between electrode and electrolyte ions through interconnecting microchannels. The combination of macaroni‐sponge‐like structure, amorphous nature, optimum specific surface area and availability of oxygen functional groups as a self‐doping heteroatom of RGPC‐0.3 greatly optimized the electrochemical performance of symmetric supercapacitor cells. The RGPC‐0.3 electrode had an ideal specific capacitance of 215.76 F g−1 with a specific energy of 29.966 Wh kg−1 and maximum specific power of 108 W kg−1 at 1 mV s−1 in a symmetric supercapacitor system. Furthermore, a relatively good coulombic efficiency of 71.01% was obtained with a low equivalent series resistance of 0.098 Ω.CONCLUSIONSThis study provides insight into the generation of unique hierarchical porous carbon as a basic component of electrodes for energy storage applications with high electrochemical performance through the utilization of waste red ginger biomass with a simple, facile and cost‐effective strategy. © 2022 Society of Chemical Industry (SCI).

Effect of Steam to Carbon Dioxide Ratio on the Performance of a Solid Oxide Cell for H2O/CO2 Co-Electrolysis

The mixture of H2 and CO, the so-called syngas, is the value-added product of H2O and CO2 co-electrolysis and the feedstock for the production of value-added chemicals (mainly through Fischer-Tropsch). The H2/CO ratio determines the process in which syngas will be utilized and the type of chemicals it will produce. In the present work, we investigate the effect of H2O/CO2 (steam/carbon dioxide, S/C) ratio of 0.5, 1 and 2 in the feed, on the electrochemical performance of an 8YSZ electrolyte-supported solid oxide cell and the H2/CO ratio in the outlet, under co-electrolysis at 900 °C. The B-site iron doped lanthanum strontium chromite La0.75Sr0.25Cr0.9Fe0.1O3-δ (LSCF) is used as fuel electrode material while as oxygen electrode the state-of-the art LSM perovskite is employed. LSCF is a mixed ionic-electronic conductor (MIEC) operating both under a reducing and oxidizing atmosphere. The cell is electrochemically characterized under co-electrolysis conditions both in the presence and absence of hydrogen in the feed of the steam and carbon dioxide mixtures. The results indicate that under the same concentration of hydrogen and different S/C ratios, the same electrochemical performance with a maximum current density of approximately 400 mA cm-2 is observed. However, increasing p(H2) in the feed results in higher OCV, smaller iV slope and Rp values. Furthermore, the maximum current density obtained from the cell does not seem to be affected by whether H2 is present or absent from the fuel electrode feed but has a significant effect on the H2/CO ratio in the analyzed outlet stream. Moreover, the H2/CO ratio seems to be identical under polarization at different current density values. Remarkably, the performance of the LSCF perovskite fuel electrode is not compromised by the exposure to oxidizing conditions, showcasing that this class of electrocatalysts retains their reactivity in oxidizing, reducing, and humid environments.

Robust NASICON-type iron-based Na4Fe3(PO4)2(P2O7) cathode for high temperature sodium-ion batteries

Iron-based mixed phosphates sodium ion batteries (SIBs) are promising sustainable storage devices due to the low-costing and non-toxicity characters. Whereas, their real application is seriously restricted by the sluggish Na+ diffusion and inferior intrinsic electronic conductivity. Herein, we propose mesoporous sponge-like structural Na4Fe3(PO4)2(P2O7) (NFPP) in-situ caged in carbon layer and cross-linked graphene nanosheets (NFPP@C@rGO), toward fast charging and highly stable sodium ion half/full cells in a wide temperature range. This rational strategy gives the cathode superior long-lasting cycling stability, specifically, 86.7 % capacity retention is retained at 20 C for over 30,000 cycles, displaying a capacity loss less than 0.00045 % per cycle. Notably, outstanding thermal stability at 60 °C is achieved and no obvious capacity degradation can be observed after cycling for 200 times at 1 C. Furthermore, the impressive electrochemical performances of full cells are determined, ascribed to the improved electronic conductivity and structural stability (e.g. a small volume change of ∼4.1 % during sodium ion insertion/deinsertion), which is confirmed by in-situ X-ray diffraction (XRD) and X-ray absorption near edge structure (XANES) measurements. All the results above prove that the NFPP@C@rGO is of high potential for advanced energy storage system based on its low costs, long-lasting cyclability and excellent thermal stability.

High-voltage electrochemical double layer capacitors enabled by polymeric ionic liquid

Improving the energy density of electrochemical double layer capacitors (EDLC) is an important but challenging research topic. Electrolytes with wide operating potential windows are key materials for current EDLC technology. In this work, an ether branch polymeric imidazole ionic liquid (PVEIm.TFSI) is synsthesized and served as an electrolyte additive in common electrolyte to optimize the working potential ranges of carbon-based EDLC. The addition of PVEIm.TFSI can improve the electrochemical stability of electrolytes and effectively adjust the upper limit potential (PU), lower limit potential (PL). Under the optimal addition ratio of 10%, the operational voltage of EDLC increases from 2.8 V to 3.2 V, which lead to an approximately 41.5% energy density increase compared with EDLC without additive. Cycling stabibity of EDLC containing 10% PVEIm.TFSI is significantly enhanced under both 3.0 V and 3.2 V. Furthermore, an equivalent circuit model and Bode plots are proposed from the electrochemical impedance spectroscopy (EIS) measurements. Both simulated and measured date dedicate that PVEIm.TFSI reduces each element of resistance, which result in more ions movement and smaller energy barrier for the diffusion processes, thereby improving the electrochemical performance of cells.

Perspective on high-temperature surface oxygen exchange in a porous mixed ionic-electronic conductor for solid oxide cells.

The surface exchange coefficient (k) of porous mixed ionic-electronic conductors (MIECs) determines the device-level electrochemical performance of solid oxide cells. However, a great difference is reported for k values, which are measured using presently available technologies of electrical conductivity relaxation (ECR), electrochemical impedance spectroscopy (EIS), and oxygen isotope exchange (OIE). In terms of this issue, this perspective paper estimates the possible physiochemical processes for the oxygen reduction reaction (ORR) in porous MIECs by comparing the oxygen supply/consumption fluxes through calculation. Then, the potential problems associated with ECR, EIS, and OIE for application in porous materials are discussed regarding theory, assumptions, sample requirements, and data processing. Finally, gas diffusion effects are revealed by comparing the simulated and measured ECR profiles, which show that the ORR process can be significantly delayed by gas diffusion. This perspective aims to recommend a reasonable method to characterize the true ORR kinetics of porous electrodes and quantify the effect of gas diffusion.

Research on SOFC Properties of Low Concentration Gas Fuel and SFM-GDC Reforming

When gas fuel is used in solid oxide fuel cells, methane cracking occurs at high temperature in the Ni-based anode, forming granular carbon deposition in the active site of the anode, and finally completely wrapped Ni metal, greatly losing the electrochemical performance. Therefore, it is very necessary to add a reforming catalytic layer in the anode of the battery. The methane is reformed into CO and H2 fuel before entering the anode, and the place where methane cracking occurs is mostly transferred to the reforming layer, which reduces the catalytic reforming burden of the Ni-based anode, so as to effectively improve the battery performance. In this paper, Sr2Fe1.5Mo0.5O6 with double perovskite structure was synthesized and prepared, which maintained very good stability in high temperature REDOX atmosphere and had high electrical conductivity. The combination of GDC and SFM can increase the reaction site of the three-phase interface of the reforming layer, and also help to improve the thermal expansion matching between the reforming layer and anode. In this paper, the electrochemical performance of straight cell coated with SSFM-GDC reforming layer has been studied. Low concentration gas in coal mine contains methane, oxygen, nitrogen, and water hydrogen sulfide, etc., and its reaction process in solid oxide fuel cells is complicated. Therefore, studying the reaction mechanism of low concentration gas in solid oxide fuel cells has important practical significance for promoting its application.

A review of progress in proton ceramic electrochemical cells: material and structural design, coupled with value-added chemical production

Improved performance of proton ceramic electrochemical cells (PCECs) through material development and structural design, and application of PCECs for efficient energy conversion render them promising for clean energy and sustainable development.

Development and implementation of in-line segmentation for continuous electrode production in lithium-ion battery cell manufacturing for traceability applications

One of the biggest challenges in battery cell production is reducing manufacturing costs. Production errors and manufacturing inaccuracies due to a complex process chain and cost-intensive material flows lead to high scrap rates and costs. In order to detect and eliminate production errors early in the manufacturing process, traceability approaches have been increasingly referred to in the literature. Here, process and product parameters are already assigned to the individual intermediate products and used to evaluate whether further processing is possible. When transferring traceability concepts to battery cell production, the challenge is to identify individual sections in the continuous processes of electrode production. These process steps have a decisive influence on the later electrochemical performance of the battery cells and have so far only been performed in batches to reduce possible defects. This paper presents two approaches to segmenting the produced electrodes in-line in the coating process to provide discrete sections for tracking and tracing applications. Production data are allocated to single electrodes instead of the entire electrode coil. Laser and ink marking systems are used to apply unique markings that are subsequently read out for product and process data assignment. Appropriate integration requirements must be met for both marking systems to apply readable markings. The requirements are derived for both marking systems from the respective mode of operation and compared with each other. It is shown that laser systems are more technically challenging and cost-intensive to integrate than ink systems but offer greater geometrical flexibility. Furthermore, it is shown how both marking technologies are integrated into the respective coating lines for lithium-ion battery electrodes within the pilot production lines at two research facilities. The traceability of product data to individual electrode sections is demonstrated using in-line and hand-measured electrode areal mass loading data.

Annealing‐Free Thioantimonate Argyrodites with High Li‐Ion Conductivity and Low Elastic Modulus

AbstractAlthough Li‐ion superconducting sulfides have been developed as solid electrolytes (SEs) in all‐solid‐state batteries, their high deformability, which is inherently beneficial for room‐temperature compaction, is overlooked and sacrificed. To solve this dilemmatic task, herein, highly deformable Li‐ion superconductors are reported using an annealing‐free process. The target thioantimonate, Li5.2Si0.2Sb0.8S4Br0.25I1.75, comprising bimetallic tetrahedra and bi‐halogen anions is synthesized by two‐step milling tuned for in situ crystallization, and exhibits excellent Li‐ion conductivity (σion) of 13.23 mS cm−1 (averaged) and a low elastic modulus (E) of 12.51 GPa (averaged). It has a cubic argyrodite phase of ≈57.39% crystallinity with a halogen occupancy of ≈90.67% at the 4c Wyckoff site. These increased halogen occupancy drives the Li‐ion redistribution and the formation of more Li vacancies, thus facilitating Li‐ion transport through inter‐cage pathway. Also, the facile annealing‐free process provides a unique glass‐ceramic structure advantageous for high deformability. These results represent a record‐breaking milestone from the combined viewpoint of σion and E among promising SEs. Electrochemical characterization, including galvanostatic cycling tests for 400 h, reveals that this material displays reasonable electrochemical stability and cell performance (150.82 mAh g−1 at 0.1C). These achievements shed light on the synthesis of practical SEs suffice both σion and E requirements.