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The Role of Isostatic Pressing in Large-Scale Production of Solid-State Batteries

Cite this: ACS Energy Lett. 2022, 7, 11, 3936–3946
Publication Date (Web):October 18, 2022
https://doi.org/10.1021/acsenergylett.2c01936

Copyright © 2022 The Authors. Published by American Chemical Society. This publication is licensed under

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Abstract

Scalable processing of solid-state battery (SSB) components and their integration is a key bottleneck toward the practical deployment of these systems. In the case of a complex system like a SSB, it becomes increasingly vital to envision, develop, and streamline production systems that can handle different materials, form factors, and chemistries as well as processing conditions. Herein, we highlight isostatic pressing (ISP) as a versatile processing platform for large-scale production of the currently most promising solid electrolyte materials. We briefly summarize the development of ISP techniques as well as the processing methods and windows accessible. Subsequently, we discuss recent reports on SSBs that leverage ISP techniques and their impact on the electrochemical performance of the systems. Finally, we also provide a techno-economic analysis for implementing ISP at scale along with some key perspectives, challenges, and future directions for large-scale production of SSB components and integration.

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Solid-state batteries (SSBs) are promising energy storage alternatives that can achieve high energy densities by enabling Li metal anodes and high-voltage cathodes. (1,2) When combined with long cycle life, improved safety, and low cost (<$100/kWh), the value proposition of solid-state lithium metal batteries becomes more and more relevant. There are, however, significant materials and processing challenges that disrupt the materialization of working SSBs at present. (3−5) Recent reviews make it clear that the energy and power densities of the reported SSBs fall short in comparison with those of the state-of-the-art Li-ion batteries. The technical barriers to be addressed in the long term include achieving areal capacities in the range of 3–10 mAh cm–2, with less than 10% excess Li anode and more than 70% active material loading, in solid-state composite cathodes that are assembled against thin electrolytes which can withstand current densities higher than 1 mA cm–2 and yet enable higher Coulombic efficiencies. Cell design calculations show that solid electrolytes with <100 μm thicknesses and Li metal anodes with <50 μm thickness are necessary to achieve energy densities comparable to or higher than those of the state-of-the-art lithium-ion batteries. (4−6) The processability and integration of thick composite cathodes, thin solid electrolytes, and thin lithium metal anodes into cell configurations in scalable fashions are of utmost significance to improve the value proposition of near-market SSBs.
An ideal SSB cell is a dense, thin, tri-layer assembly with conformal interfaces. (1,3) Generating these dense, thin multi-layer systems required for practical SSBs is typically not possible with conventional processing approaches for a variety of reasons. (7−9) Indeed, each component of the SSB has a multitude of issues that need to be tackled to engineer high-performance cells (Figure 1a). (4,10,11) The sheer variety of materials and their properties independent of the solid electrolytes make development of a consistent processing platform almost impossible to achieve. (2,12,13) For example, garnet solid electrolytes typically undergo dual-step sintering for achieving the cubic phase and densification of the pellets along with an additional sintering step in Ar to remove the Li2CO3 impurities. (14,15) The sintering temperatures for garnets are typically in excess of 1000 °C, with hold-times of 10 h or longer. In contrast, sulfide, argyrodites, and anti-perovskite materials are synthesized at lower temperatures of 100–400 °C and are generally processed into cells at room temperature and under uniaxial loading. (16−19) Most of the processing routes described are strictly for small-scale pellet preparation. So far, a large-scale roll-to-roll kind of processing is typically only demonstrated on hybrid electrolytes that leverage the slot-die processing of polymer dispersions to make larger form factor materials. (20,21,37)

Figure 1

Figure 1. (a) Current challenges in processing and integration of solid-state batteries. (b) Uneven density distribution by single uniaxial pressing in rigid die for cylinder. (c) Schematic diagram of a pressure vessel cavity into which the sample is inserted and subjected to isostatic pressure and temperature conditions, and temperature and pressure ranges for CIP (blue), WIP (green), and HIP (orange) techniques.

Conventional pressing methods are used for a broad number of applications to compact, form, integrate, and densify materials for further fabrication and use. (22) Powder metallurgy processing commonly applies conventional pressing methods consisting of uniaxial press-and-sinter to create solid parts of various geometries from raw powder. (23,24) Most solid electrolyte (SE) materials and components are processed using these approaches. The compaction mechanisms are material and process dependent but typically consist of loose particle restacking and deformation at points of contact as pressure increases. This method poses significant challenges for SSB materials and components as it invariably leads to high variation in density throughout the compact due to friction at die walls resulting in non-uniform properties (Figure 1b). (25,26) Although improved density uniformity is possible with use of lubricants and additional punches, the application window is limited.

The solid-state battery community needs to start envisioning pathways to streamline and scale-up the processing of promising solid electrolytes from pellet scale to form factors that are more practical.

The SSB community needs to start envisioning pathways to streamline and scale-up the processing of promising solid electrolytes from pellet scale to form factors that are more practical. Application of high formation pressures and temperatures over sustained time is an underlying requirement for processing most materials under study. In this regard, isostatic pressing (ISP) is a technique that has inherent versatility to cover the processing conditions required for most promising SE materials as well as the capability to achieve large-scale production. ISP can be employed for generating the thin, dense SE layers needed for practical SSBs. Furthermore, it can also provide a pathway toward integration of the cathode, solid electrolyte, and anode layers into a dense, tri-layer system for practical applications. Herein, we discuss an overview of the ISP technology along with recent experimental results in the SSB domain that leverage ISP techniques to achieve superior electrochemical performance. We also provide a techno-economic analysis to evaluate the viability of using ISP for large-scale production of SSB components and assemblies. Finally, we provide some perspectives from the research and instrumentation viewpoints for increasing the penetration of ISP in the SSB manufacturing ecosystem.

ISP Processing Pathways and Their Application to SSBs

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Isostatic pressing is a technique that applies pressure uniformly in all directions on the compact or container being pressed. (27,28) The process fundamentals are based on Pascal’s law, in which a pressure change exerted on a fluid in an enclosed vessel will be transmitted undiminished to all portions of the fluid, surfaces, and walls within the vessel. Depending on the processing parameters, the fluid can be a gas or liquid. This processing route provides a path to eliminate the frictional forces hindering conventional pressing techniques due to die wall interaction thereby improving the average density for a given applied pressure as well as the uniformity that can be achieved. (29−31) The resultant density and uniformity of the sample depend on the optimization of three key variables: time, temperature, and pressure of the ISP cycle. (27)
There are three main categories of isostatic pressing: (1) cold isostatic pressing (CIP), (2) warm isostatic pressing (WIP), and (3) hot isostatic pressing (HIP), with a common thread between these techniques being the use of a pressure vessel. A typical ISP process involves loading of the sample inside the pressure vessel, which is then elevated to the required process temperature and pressure using appropriate process control systems followed by a hold and a relaxation process to ambient conditions (Figure 1c). CIP, WIP, and HIP are primarily differentiated by the process conditions (T and P) that are accessible within the technique (Figure 1c, Table 1). Beyond the pressure vessel, CIP and WIP are relatively simple systems consisting of various valves, intensifiers, pumps, and a control panel. Due to the elevated temperatures involved in HIP, the equipment is more complex, requiring additional subsystems to ensure safe and reliable operation. CIP can offer ISP capabilities up to 600 MPa (87 000 psi) dependent on equipment design and size. (27) Liquid consisting of water and an additive such as oil is generally used as the pressure medium. WIP can be performed in standard CIP vessels offering similar pressing capabilities (Figure S2). The pressurizing medium is heated externally and circulated into the pressure vessel. Elevated temperatures up to 150 °C (302 °F) with good temperature uniformity are possible with utilizing high-temperature oil and compatible bag material. WIP cycle time is extended relative to that of CIP due to the heating of the circulating media, with one cycle every 10–20 min being feasible, dependent on temperature uniformity requirements. It is important to note here that handling of reactive materials like Li metal, sulfides, and argyrodites requires careful selection of the pressure medium to eliminate any potential chemical reactivity. Also, handling of Li metal within ISP equipment is not established; however, it is expected that, with proper optimization of the experimental conditions, Li metal anodes can be processed using CIP/WIP techniques. Standard HIP processing equipment offers capabilities up to 200 MPa (30 000 psi) and high temperatures up to 2000 °C with great temperature uniformity and accuracy. Due to the elevated temperatures required, inert argon gas is commonly used as the pressure medium to protect both the workpieces and the furnace during operation. The gas is supplied to the HIP vessel from a gas storage system and delivered from a compressor(s) through a series of valves under high pressure. (28,32) Due to the high compressibility of gas relative to liquid, processing time is significantly increased, typically requiring hours instead of minutes. However, recent advancements in vessel design and cooling strategies have enabled uniform rapid cooling (URC), significantly reducing process time. Production rates are dependent on several factors such as applied pressure, vessel size, level of automation, and pump capacity but can achieve one operation cycle per minute or faster. The size of the vessel is dependent on product size and volume needs, with an vessel inner diameter of up to 3 m and length up to 5 m (Figure S1).
Table 1. Standard Processing Capabilities of Isostatic Pressing Equipmenta
ISP techniqueCIPWIPHIP
pressure mediumliquid - waterliquid - oil/watergas - argon/nitrogen
standard temperature rating (°C/°F)20/68150/3022000/3632
standard pressure rating (MPa/ksi)600/87500/72.5207/30
cycle timeo++++
equipment costo++++
a

Qualitative values are represented by o, +, and +++, where o < + < +++.

Currently, there is an absence of consensus with regard to how SSBs are going to be scaled up for production due to the variety of materials, architectures, and components as well as design philosophies. Primarily, the form factors prevalent in the literature are pouch cells, cylindrical cells, and prismatic cells (Figure 2a). Within these cell configurations, the underlying architectures are identical: the tri-layer anode|solid electrolyte|cathode films supported on current collectors. We anticipate that ISP will primarily be used for compaction of densification of individual components, viz. thin SE films as well as these tri-layer cell assemblies, to enable improved performance.

Currently, there is an absence of consensus with regard to how solid-state batteries are going to be scaled up for production due to the variety of materials, architectures, and components as well as design philosophies.

It is anticipated that batch processing of stacked sheets of solid electrolyte or wound spools of the SE films can be processed using ISP to generate the required dense thin films (Figure 2b). For full cells, we anticipate that tri-layer assemblies and pouch cells as well as cylindrical geometries are compatible for ISP, with the latter preferred as this ensures pressure uniformity across all the surfaces of the samples undergoing the ISP treatment as well as allows for higher packing fraction of the container volume resulting in higher throughput. Ultimately, ISP offers a more efficient and effective alternative to consolidate internal voids and defects for maximum uniformity and density, achieving intimate contact between particles without geometrical limitations, all while preserving the shape of an object. Over conventional routes, ISP enables the production of larger components, increases allowable length–diameter ratios, and provides superior material properties.

Figure 2

Figure 2. ISP integration pathways into SSB manufacturing. (a) Possible packaging of SSB systems and the underlying tri-layer architectures. (b) ISP configurations of the components and assemblies envisioned for large-scale production.

Critical Survey of ISP Implementations in SSB Field

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Isostatic pressing has seen limited application in the SSB field thus far. To date, the majority of the implementation of ISP techniques is for densification of green pellets prior to their sintering (Supporting Information). As discussed earlier, for a given material system, high densities can only be achieved through careful optimization of the time–temperature–pressure dependence of the ISP cycle. However, no such study is reported for any SE material in the literature. In contrast, most reports utilize an average isostatic pressure of 200–250 MPa for the CIP cycle. The choice of this processing pressure is most likely arbitrary. As such, there is no correlation between the reported density of the pellet and the ISP conditions (Figure S3). This primarily indicates that the ISP conditions that are being used are largely un-optimized. No reports of WIP for SE densification were available to the best of the authors’ knowledge, while only a few reports of HIP treatment were identified (Figure 3a). The phase purity of the solid electrolytes is typically not impacted by the ISP treatments (Figure 3b) as no additional peaks from decomposition products or Li loss are seen for LLZO, even after a HIP treatment. (33) Additionally, carefully tuning the processing conditions with garnets can help minimize/eliminate the need for mother powder during sintering that currently constitutes a significant amount of material waste for LLZO materials. (34) After the HIP treatment, the opaque pellet turns translucent, as shown in the inset in Figure 3b. (33) This typically is indicative of larger grain sizes and high densities, both of which result in improved transport and electrochemical properties. It should be noted that the relative intensities of certain reflections are modulated after the HIP process. This suggests that the grain growth during ISP might lead to certain preferred orientations.

Overall, the demonstrations here showcase that the application of isostatic pressing to the soft solid electrolyte material families can enable processing of these materials with a high degree of local microstructural control that is imperative for durable solid-state batteries.

Recent work has shown that cathode particles with certain crystallographic orientations perform better compared to polycrystalline counterparts in SSBs. (35) The ability to control and grow preferred orientations during the sintering/integration process can have significant benefits for the performance of batteries. This aspect of ISP has not been utilized by the community thus far but is expected to yield high-performance battery systems. It should be noted here that the available literature data suggests almost all the SE densification work with ISP is carried out for garnet or NASICON-type crystalline materials. This is counter-intuitive, as one would assume that softer electrolytes like sulfide and argyrodites can benefit enormously from these densification strategies. Further work is needed to explore ISP processing techniques for materials like sulfides and halides. Earlier work has conclusively shown that local microstructural differences occurring in the solid electrolyte due to uniaxial pressing can catastrophically impact the SSB cell. (17,57) As a proof of concept on the applicability of ISP techniques to these electrolytes, CIP and WIP processing was carried out on anti-perovskite solid electrolytes (Figure 3). As can be seen from the scanning electron microscopy (SEM) images (Figure 3c–e), the cross-sectional morphologies of the anti-perovskite materials processed with conventional uniaxial pressing and ISP techniques are completely distinct. Uniaxial pressing leads to materials with some porosity and distinct grain boundaries, both of which can limit the electrochemical performance of the material. (58−63) Overall, both ISP techniques lead to improved density compared to the green pellet; however, WIP shows additional formation of small rod-like crystals (Figure 3d,e). We also carried out synchrotron tomography on the CIP and WIP processed materials. From the synchrotron tomography data sets, it was observed that the uniaxially pressed pellet results in a porosity of ∼12%, while the CIP pellet shows an average porosity of ∼1.8% and the WIP pellet shows a porosity of 0.15%. CIP and WIP, therefore, lead to an order of magnitude reduction of porosity and highly dense solid electrolytes that are vital for high-performance SSBs. Overall, the demonstrations here showcase that the application of ISP to the soft SE material families can enable processing of these materials with a high degree of local microstructural control that is imperative for durable SSBs. It should be noted that the densification mechanism in ISP is strongly dependent on the materials’ properties. For metallic-like components, ISP relies on creep diffusion to achieve high density, while for polycrystalline ceramic-like materials the densification is governed by the grain growth mechanism. As such, there is no strict definition of a “critical temperature” at/above which densification occurs. However, it is necessary to carefully optimize the time–temperature–pressure correlation for each material system to optimize the densification process. Further, some studies have also indicated that ISP treatment of the solid electrolytes can improve their mechanical properties. (64) HIP-processed LLTO showed an average Young’s modulus of ∼223 MPa, compared to 192 MPa obtained by conventional sintering approaches. Further work on the impact of ISP processing conditions on the surface mechanics of the solid electrolyte is going to be vital toward designing resilient interfaces for SSBs.

Figure 3

Figure 3. (a) Compilation of isostatic pressing parameters used in the SSB literature for densification and integration of solid electrolytes and cells, respectively. Largely CIP is the primary technique that is leveraged within the SSB community. Shaded markers indicate either HIP or WIP cycles. The color of the markers indicates the solid electrolyte material family (pink markers, LLZO; yellow markers, Na-based NASICONs; green markers, sulfides; gray marker, hybrid electrolyte). The data for this figure are collected from refs (33,34,36−56). (b) XRD patterns and optical images of LLZO before and after the HIP treatment. The scale bars represent 10 mm. Data adapted from ref (33). SEM images of anti-perovskite solid electrolytes processed under (c) uniaxial loading conditions, (d) CIP conditions, and (e) WIP conditions. The scale bars in all the SEM images are 10 μm. (f, g) Tomographic reconstruction slices and pore volume visualization of the anti-perovskites processed under CIP and WIP conditions along with the measured porosity. The sub-volume investigated for porosity evaluation and visualized here is 300 × 300 × 300 μm3.

We also looked at the available literature in terms of ionic conductivities as well as full cells and symmetric cells that were processed using ISP. We note that the aim of this compilation is (1) to showcase that ISP techniques can be used for multiple material systems and (2) to visualize the spread of the data set when it comes to transport properties and cycling behavior when ISP techniques are employed. The literature data does not always report the impact of ISP versus standard conditions, which makes it difficult to provide an explicit comparison for each case. Figure 4a displays the compilation of ionic conductivities of solid electrolytes that underwent cold isostatically pressed (CIP) or hot isostatically pressed (HIP) pelleting as a function of inverse temperature. As mentioned above, most of the pellet densification processes are carried out for garnet and NASICON-type materials. It is discernible from Figure 4a that the conductivity data are very promising in terms of the magnitude of conductivity. However, even within the same material family, there is a large variance in the reported conductivity data due to the lack of optimization of the CIP and HIP processes. Apart from the intrinsic crystal structure and defect chemistry, the practical ionic conductivity of a particular solid electrolyte depends on the pressure, temperature, and time involved in densification. These three parameters need to be optimized to get optimum sample density. It is anticipated that the conductivity variance reported in Figure 4a is probably due to non-optimization of sample processing parameters and thereby sub-optimal densification.

Figure 4

Figure 4. (a) Compilation of ionic conductivity data sets from literature that leveraged ISP processing methods for solid electrolyte densification. The marker colors represent different material families (garnet, Na-solid electrolytes, and Li-based NASICONs). The data are adapted from refs (33,38,39,41,43,51,53,55,65−67). (b) Discharge polarization curves and (c) capacity retention profiles from solid-state battery cells that were integrated into tri-layer configurations using ISP processes. The corresponding solid electrolyte system is indicated in the legend. The data for (b) and (c) are adapted from refs (37,43,44,50,56,68−71).

The reported data shows pellet densities ranging from 85 to 100%, formed using ISP techniques for a range of processing pressures (Figure S3). Figure 4b exhibits the discharge profiles of various solid electrolyte|electrode assemblies integrated using an ISP process. The reports are promising in terms of interfacial resistances and the discharge capacity. Most of the cells exhibit practical discharge capacity as obtained from the conventional liquid electrolyte-based cell. Apart from the densification of electrolyte pellet/film, CIP/HIP helps to form a better interfacial contact between the electrolyte and electrode interfaces. The reduced contact impedance assists in obtaining practical discharge capacity. The discharge polarization curves also indicate that ISP processes do not generate secondary phases, indicating minimal reactivity between the electrolyte and electrode due to the high pressures. The retention behaviors of various SSB full cells that were integrated using ISP processes are shown in Figure 4c. The full cell and symmetric cells are processed with a comparatively wider range of materials. The reported data display excellent cycling stability, in some cases for close to 1000 cycles. (69) This work also highlighted the ameliorating influence of WIP in enhancing the density of the layers, interfacial adhesion of the cathode|solid electrolyte, uniformity of lithium deposition, and structural integrity of the solid electrolyte. Compared to this, uniaxial pressing would result in non-uniform density that would contribute to accelerated failures of solid electrolyte. Overall, the results thus far indicate that an optimized ISP process would be a great tool for the fabrication of high-performance and durable SSB components and cells.

Technoeconomic Analysis for Large-Scale Production of SSB Materials and Assemblies

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Large-scale adoption and production are crucial to drive SSB to a cost basis that is feasible when compared to that of conventional Li-ion batteries. (4) However, at the current nascent stage of manufacturing readiness level for most of the SE material families, it is difficult to accurately predict the techno-economics of a given processing pathway. (8,11) We carry out a preliminary analysis for processing costs associated with ISP considering its employment in two distinct stages of the SSB manufacturing process: (1) SE laminate formation and (2) tri-layer cell integration. Several projections of anticipated electric vehicle (EV) sales in the coming two decades suggest over 50 million EVs coming to the world market by 2040 (Figure S4). (72) The techno-economic projections included here assume that all those EVs are built with solid-state battery packs (Figure 5a). Additionally, we assume that all SE fabrication and cell integration are carried out using ISP processing. Assuming a pack and cell configuration (4 mAh cm–2 cathode loading, N/P ratio 0.2, SE thickness 75 μm, cell thickness 500 μm), we projected the required SE volume as well as the tri-layer cell volume for meeting the requirements of the expected EVs up to 2040 (Figure 5c). Detailed information regarding the projection calculation is available in the Excel sheet included in Supporting Information. It should be noted here that due to the inherent process of ramp–hold–release in all the ISP configurations (CIP/WIP/HIP), these are essentially batch processes. The typical configurations and costs of the CIP/WIP/HIP instruments are highlighted in Figure 5b. The metrics for the dimensions and cycle times as well as costs are adapted from Quintus’ internal design parameters which they envision for the SSB processing equipment. Further details on the metrics can be found in the Supporting Information. These metrics represent the state-of-the-art instruments with the largest sample handling volumes for large-scale production. Due to the geometry of the instruments, cylindrical form factors are preferred compared to planar configurations. For this analysis, we assume spools/rolls of SE films and/or tri-layer films on some backing substrate being fed to the ISP instrument for processing. The volume available for actual materials is defined by the product of packing fraction and the total volume measured from the dimensions. The packing fraction considers the volume taken up by the sealing/backing/holding materials and is assumed to be 0.6. Note that this packing fraction is a conservative estimate and there is an opportunity for significant improvement. Cost per cycle mentioned in Figure 5 reflects a number that incorporates capital expenditure over a 10-year time frame. Correspondingly, we calculate the cost of processing solid electrolyte (Figure 5c) as well as of cell integration (Figure 5d) considering various ISP cycle and their combinations. Based on the cycles/year metric, we also predicted that roughly 8–15 HIP/WIP/CIP units will be required to handle the SE processing and cell integration. Based on these calculations, it is estimated that the running cost of ISP for cell integration is ∼$1–20K/GWh based on the type of technique used. We understand that very different ISP cycles might be required depending on the materials chemistry involved, which can influence these results. However, these calculations provide an initial estimate of the scale of processing costs to meet the EV demands in the near future.

Figure 5

Figure 5. (a) Overview of the protocol used for techno-economic analysis carried out here. (b) Typical features of a state-of-the-art CIP/WIP/HIP instrument commercially available today. Dimensions reflect the volume of the largest sample that can be accommodated within the instrument. Packing fraction represents the fraction of the available volume which will occupied by the material of interest. Cycles assumed are detailed in the Supporting Information. Cost per cycle and cost per volume are in U.S. dollars. (c) Projected volumes of solid electrolyte and cells that need to be processed to cater to the expected EV demands in the next 20 years. For details see the Supporting Information. Projected processing cost for (d) solid electrolyte processing and (e) cell integration considering different ISP protocols.

Perspectives and Future Directions

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As discussed earlier, the major roadblock in the successful commercial deployment of all-solid-state batteries is the availability of a reliable, adaptable, and versatile large-scale manufacturing approach for solid-state architectures. Effectively addressing this challenge would leapfrog present-day battery technology into the next decades by enabling energy-dense SSBs to meet the burgeoning demands of portable electronics, grid storage, EV, and even eVTOL applications. Herein, our team comprehensively discussed and highlighted isostatic pressing as a potential pathway toward this goal of large-scale production of SSBs and their components.

As we continue to innovate on materials and interfaces within the solid-state battery, it is crucial to keep a lens on the manufacturing aspects of these systems.

Despite the versatility and easy adaptability of this manufacturing approach to cater to the needs of SSBs with varying form factors, battery chemistries, and configurations, continuous R&D efforts to address several underlying challenges in implementation of ISP have to be systematically undertaken to realize the true potential of this manufacturing approach. To this extent, we have also summarized some key perspectives, challenges, and future directions in ISP for SSB manufacturing as follows: (i) Employing and optimizing ISP techniques for SSB components and cells will not only be crucial for large-scale production but also afford key technological advantages that can improve the performance of SSBs. Briefly, this was highlighted by the ability to achieve high-density materials (>99%), the ability to control crystallographic orientations, and the ability to achieve conformal and resilient interfaces. (ii) We have shown the characteristic differences between key ISP processes─CIP, WIP, and HIP─and their application to SSB materials and cell integration. (iii) The techno-economic model discussed here provides a reference point for the scale of processing costs associated with SSB components and cells to meet the future EV demands. It drives home the crucial point that component and cell productions for SSBs become viable only with economies of scale. As we continue to innovate on materials and interfaces within the SSB, it is crucial to keep a lens on the manufacturing aspects of these systems. ISP processing is one of the key avenues toward achieving this goal.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.2c01936.

  • Anti-perovskite solid electrolyte preparation and characterization details, including Figures S1–S5 (PDF)

  • Excel sheet summarizing the referenced experimental data from literature (XLSX)

  • Excel sheet that includes the techno-economic model for ISP (XLSX)

Terms & Conditions

Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Author Information

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  • Corresponding Authors
  • Authors
    • Marm Dixit - Electrification & Energy Infrastructure Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesOrcidhttps://orcid.org/0000-0002-9599-9288
    • Ruhul Amin - Electrification & Energy Infrastructure Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesOrcidhttps://orcid.org/0000-0002-0054-3510
    • James Shipley - Quintus Technologies AB, Quintusvägen 2, SE-721 66 Västerås, Sweden
    • Richard Eklund - Quintus Technologies AB, Quintusvägen 2, SE-721 66 Västerås, Sweden
    • Nitin Muralidharan - Electrification & Energy Infrastructure Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesOrcidhttps://orcid.org/0000-0001-6042-5295
    • Lisa Lindqvist - Quintus Technologies, Lewis Center, Ohio 43035, United States
    • Anton Fritz - Quintus Technologies AB, Quintusvägen 2, SE-721 66 Västerås, Sweden
    • Rachid Essehli - Electrification & Energy Infrastructure Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    • Mahalingam Balasubramanian - Electrification & Energy Infrastructure Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesOrcidhttps://orcid.org/0000-0002-3988-3125
  • Author Contributions

    M.D. and C.B. contributed equally.

  • Notes
    The authors declare no competing financial interest.

Biographies

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Marm Dixit

Marm Dixit is a Weinberg Distinguished Staff Fellow at the Oak Ridge National Laboratory. Marm was awarded the ECS Toyota Young Investigator Fellowship 2021, and ECS student travel grant on two occasions. He received his Ph.D. in Mechanical Engineering from Vanderbilt University.

Chad Beamer

Chad Beamer has a M.S. from The Ohio State University in material science. He spent time with GE Aviation and Bodycote early in his career and currently works for Quintus Technologies. There he manages the Application Center, educates on isostatic pressing technologies, and leads development efforts within both academia and industry.

Ruhul Amin

Ruhul Amin is a staff scientist at ORNL with expertise in simulation and experimental studies on transport properties and interfacial kinetics with more than 18 years of experience in the battery field. He is a recipient of several awards and has published over 80 peer-reviewed articles and several patents.

James Shipley

James Shipley is Manager for Business Development at Quintus Technologies, working with isostatic processing with a focus on additive manufacturing, castings, powder near net shape, and metal injection molding for all manner of alloys and materials.

Richard Eklund

Richard Eklund has been managing applied product development and manufacturing of heavy engineered equipment for over 30 years. At Quintus Technologies he is responsible for the development of the product program for warm isostatic pressing.

Nitin Muralidharan

Nitin Muralidharan is currently a R&D Associate Staff Scientist in the Emerging and Solid-State Batteries Group. His research portfolio includes development of cobalt-free cathodes, solid-state batteries, and mechano-electrochemistry. He received his Ph.D. in Interdisciplinary Materials Science from the Vanderbilt University, Nashville, Tennessee.

Lisa Lindqvist

Lisa Lindqvist has a M.S. in computational mechanics from Luleå University of Technology in Sweden. She joined Quintus Technologies after graduating in 2021 and works with stress analyses of the equipment at the time of writing.

Anton Fritz

Anton Fritz has a M.S. from Luleå University of Technology in Aerospace Engineering. In 2018 he started his career at Quintus Technologies as a young graduate. Today his main topics are fluid mechanics and CFD simulation. He is also involved in several R&D projects.

Rachid Essehli

Rachid Essehli is a R&D Staff with 15 years of experience in synthesis of new compounds, both glassy and crystalline forms, and a strong background in characterization of materials by X-ray diffraction. He works on the material synthesis, engineering and characterization of materials for Li-ion, beyond Li-ion, and solid-state batteries.

Mahalingam Balasubramanian

Mahalingam Balasubramanian received his Ph.D. in physics from the University of Connecticut. He is currently a Distinguished Scientist and Lead of the Emerging and Solid-State Battery Group in the Electrification and Energy Infrastructures Division at Oak Ridge National Laboratory.

Ilias Belharouak

Ilias Belharouak is a Distinguished Scientist and the Head of Electrification and Energy Storage at the Oak Ridge National Laboratory and an Adjunct Professor at the University of Tennessee Knoxville. He holds Ph.D. and M.S. degrees in Materials Science and Solid-State Chemistry from the Bordeaux 1 University, Bordeaux, France.

Acknowledgments

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This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by Laboratory Directed Research and Development (LDRD) Program at Oak Ridge National Laboratory, and the Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO) (Director: David Howell) Applied Battery Research subprogram (Program Manager: Peter Faguy). M.D. was also supported by Alvin M. Weinberg Fellowship at the Oak Ridge National Laboratory. SEM micrography and EDS work reported here was conducted at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE, Office of Science User Facility at Oak Ridge National Laboratory. This research also used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. The authors would like to thank Pavel Shevchenko and Francesco de Carlo for their help with the tomography experiments.

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  • Abstract

    Figure 1

    Figure 1. (a) Current challenges in processing and integration of solid-state batteries. (b) Uneven density distribution by single uniaxial pressing in rigid die for cylinder. (c) Schematic diagram of a pressure vessel cavity into which the sample is inserted and subjected to isostatic pressure and temperature conditions, and temperature and pressure ranges for CIP (blue), WIP (green), and HIP (orange) techniques.

    Figure 2

    Figure 2. ISP integration pathways into SSB manufacturing. (a) Possible packaging of SSB systems and the underlying tri-layer architectures. (b) ISP configurations of the components and assemblies envisioned for large-scale production.

    Figure 3

    Figure 3. (a) Compilation of isostatic pressing parameters used in the SSB literature for densification and integration of solid electrolytes and cells, respectively. Largely CIP is the primary technique that is leveraged within the SSB community. Shaded markers indicate either HIP or WIP cycles. The color of the markers indicates the solid electrolyte material family (pink markers, LLZO; yellow markers, Na-based NASICONs; green markers, sulfides; gray marker, hybrid electrolyte). The data for this figure are collected from refs (33,34,36−56). (b) XRD patterns and optical images of LLZO before and after the HIP treatment. The scale bars represent 10 mm. Data adapted from ref (33). SEM images of anti-perovskite solid electrolytes processed under (c) uniaxial loading conditions, (d) CIP conditions, and (e) WIP conditions. The scale bars in all the SEM images are 10 μm. (f, g) Tomographic reconstruction slices and pore volume visualization of the anti-perovskites processed under CIP and WIP conditions along with the measured porosity. The sub-volume investigated for porosity evaluation and visualized here is 300 × 300 × 300 μm3.

    Figure 4

    Figure 4. (a) Compilation of ionic conductivity data sets from literature that leveraged ISP processing methods for solid electrolyte densification. The marker colors represent different material families (garnet, Na-solid electrolytes, and Li-based NASICONs). The data are adapted from refs (33,38,39,41,43,51,53,55,65−67). (b) Discharge polarization curves and (c) capacity retention profiles from solid-state battery cells that were integrated into tri-layer configurations using ISP processes. The corresponding solid electrolyte system is indicated in the legend. The data for (b) and (c) are adapted from refs (37,43,44,50,56,68−71).

    Figure 5

    Figure 5. (a) Overview of the protocol used for techno-economic analysis carried out here. (b) Typical features of a state-of-the-art CIP/WIP/HIP instrument commercially available today. Dimensions reflect the volume of the largest sample that can be accommodated within the instrument. Packing fraction represents the fraction of the available volume which will occupied by the material of interest. Cycles assumed are detailed in the Supporting Information. Cost per cycle and cost per volume are in U.S. dollars. (c) Projected volumes of solid electrolyte and cells that need to be processed to cater to the expected EV demands in the next 20 years. For details see the Supporting Information. Projected processing cost for (d) solid electrolyte processing and (e) cell integration considering different ISP protocols.

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    • Anti-perovskite solid electrolyte preparation and characterization details, including Figures S1–S5 (PDF)

    • Excel sheet summarizing the referenced experimental data from literature (XLSX)

    • Excel sheet that includes the techno-economic model for ISP (XLSX)


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