Solid-state Lithium-sulfur Batteries Research Articles

Lithium-rich high entropy oxide with abundant oxygen vacancies for composite polymer all-solid-state Li-S batteries

Poly(ethylene-oxide) (PEO)-based all-solid-state lithium-sulfur (Li-S) batteries simultaneously possess the advantage of extraordinary theoretical energy density and high safety, high machinability. However, the challenges of lithium polysulfide (LiPS) shuttling and insufficient Li+ conductivity hinder the batteries from practical application. In this work, a lithium-rich high entropy oxide with abundant oxygen vacancies (HL30) is developed as an active filler in PEO to concurrently address the two issues. Specifically, the addition of HL30 promotes the mobility of Li+ in PEO electrolyte as well as provides an extra high-efficiency pathway for Li+ transport, leading to large enhancement of the Li+ ionic conductivity. The metal species in HL30 could anchor the LiPS via bonding interaction while the surface oxygen vacancies further increase the bonding energy. As a result, the ionic conductivity of HL30-containing electrolyte reaches 5.06 × 10−4 S cm−1 at 60 °C, exceeding that of pure PEO electrolyte (2.45 × 10−4 S cm−1) to a considerable extent. The coulombic efficiency of Li-S full battery decreases from 113 % to 103 %, revealing an efficient restriction of shuttling effect. This work provides a novel method of composite polymer electrolyte design to achieve the practical application of high-performance solid-state Li-S batteries.

Efficient Co-ZrO2 electrocatalyst achieves high-performance solid-state lithium-sulfur batteries

Abstract Li-S batteries are recognized as a promising secondary battery system because of their high energy density, low cost, and environmental friendliness. However, the development of Li-S batteries is mainly limited by issues such as electrode volume expansion, lithium polysulfide (LiPSs) shuttle, and slow redox reaction kinetics of sulfur. Here, a kind of solid-state Li-S battery with in situ solidified solid-state electrolytes (SSEs) is reported, which dramatically reduces the electrode/electrolyte interfacial impedance. In addition, electrospinning is used to fabricate a macroporous carbon nanofibers film (MP-CNFs) loaded with dispersed Co-ZrO2 nanodot electrocatalyst as the cathode host. The in-situ gel electrolyte can be easily infiltrated into the porous carbon nanofibers and contact the Co-ZrO2 catalyst, thus fully exerting its catalytic and conversion effects on LiPSs. The results indicate that solid-state Li-S batteries exhibit a high initial capacity of 795.5 mA h·g−1 and a capacity retention rate of ∼100% after 200 cycles at 1 C.

High-Electrochemical-Activity Composite Cathode Enabled by Fast Segmental Relaxation for Solid-State Lithium-Sulfur Batteries.

Solid-state lithium-sulfur batteries (SSLSBs) have attracted a great deal of attention because of their high theoretical energy density and intrinsic safety. However, their practical applications are severely impeded by slow redox kinetics and poor cycling stability. Herein, we revealed the detrimental effect of aggregation of lithium polysulfides (LiPSs) on the redox kinetics and reversibility of SSLSBs. As a paradigm, we introduced a multifunctional hyperbranched ionic conducting (HIC) polymer serving as a solid polymer electrolyte (SPE) and cathode binder for constructing SSLSBs featuring high electrochemical activity and high cycling stability. It is demonstrated that the unique structure of the HIC polymer with numerous flexible ether oxygen dangling chains and fast segmental relaxation enables the dissociation of LiPS clusters, facilitates the conversion kinetics of LiPSs, and improves the battery's performance. A Li|HIC SPE|HIC-S battery, in which the HIC polymer acts as an SPE and cathode binder, exhibits an initial capacity of 910.1 mA h gS-1 at 0.1C and 40 °C, a capacity retention of 73.7% at the end of 200 cycles, and an average Coulombic efficiency of approximately 99.0%, demonstrating high potential for application in SSLSBs. This work provides insights into the electrochemistry performance of SSLSBs and provides a guideline for SPE design for SSLSBs with high specific energy and high safety.

High-Temperature Lithium-Sulfur Batteries with Commercial Paper-Derived Solid-State Electrolyte

Solid-state lithium-sulfur (Li-S) battery technologies could power future electric mobility due to their potential high energy density. However, the current solid-state Li-S batteries face several challenges, such as high internal impedance at the electrode/electrolyte interfaces, shuttling of lithium polysulfides, and Li dendrite formation. Herein, we introduced a novel Li-rich cellulose-based solid-state electrolyte in combination with sulfurized polyacrylonitrile (SPAN, 36.5 wt.% S) cathode, leading to durable Li-S batteries for high-temperature applications. We utilized SPAN due to its reasonable conductivity, high reversible capacity, and stable cycling performance. The solid-state electrolyte in this study was prepared by infusing Li ions (Li+) into a copper-coordinated cellulosic paper. The infusion of Li+ was carried out by soaking the copper-treated paper in a 1 M LiTFSI in EC0.5DME0.25DOL0.25 solution (where subscripts indicate the volume fraction), followed by complete evaporation of the solvents. Three types of cellulosic paper were explored, from which the commercial copy paper resulted in the highest area-normalized conductance of 24.4 mS cm-2 and Li-ion transference number of 0.76 at 50 °C. At this temperature, the Li-SPAN cells with paper-based electrolyte delivered an initial reversible capacity of 1536 mAh gs -1 at 168 mA gs -1 (0.1C). After high-temperature cycling for 150 cycles at 0.5C, the Li-SPAN cells exhibited an exceptional capacity retention of 82.2% (from 982 to 807 mAh gs -1). The conformability of the paper-based electrolyte ensures good interfacial contact with the SPAN and Li electrodes. As a result, when this solid-state Li-S battery was subjected to fast charging/discharging (1C) at 50 °C, it delivered a reversible capacity of 670 mAh gs -1. In this talk, we will outline the results from our electron microscopy, X-ray diffraction measurements, electrochemical impedance spectroscopy, and cyclic voltammetry studies on Li-S cells to unravel the superior performance of paper-based Li-S batteries at high temperatures. Figure 1

Ion Conduction Mechanism and Interfacial Stability in Fluorine Containing Lithium Argyrodite Electrolytes for Solid-State Lithium-Sulfur Batteries

Solid-state lithium-sulfur batteries (SSLSBs) hold great potential as a safe and energy-dense storage technology for wide variety of applications. Among solid-state electrolytes, halogen-doped lithium argyrodites have become an attractive category. This is attributed to their notable features, including high lithium-ion conductivity (~10-3 S/cm), favorable elastic stiffness (~ 30 GPa), and low flammability, making them promising candidates for enhancing the performance of SSLSBs.Despite their potential, SSLSBs based on sulfide faces challenges due to a limited atomic-scale understanding of ion-conduction, charge transport, structural evolution, and interfacial reactions such as dendrite growth, electrolyte decomposition. Here we employ a combination of density functional theory calculations, and ab initio molecular dynamics simulations to address this challenge for fluorinated argyrodites. Specifically, using accurate materials modeling, we design fluorine-containing argyrodite electrolytes that simultaneously offer enhanced (a) Li-ion conduction facilitated by unique Li-disorder induced by fluorine and other halogen co-dopants, and (b) stability against Li-anode owing to formation of a stable solid-electrolyte interface containing conductive species (Li3P), alongside LiCl and LiF. We will discuss these results in the context of accelerating design of novel solid-state electrolytes for long-lived, stable, and high-energy density SSLSBs.

Disruptive Semi-Solid Lithium Sulfur Battery Cell Design with Fully Separated Anolyte and Catholyte

Lithium-Sulfur-Batteries (LSBs) have been discussed as one of the most promising post-lithium-ion-battery technologies in literature for the last decade due to their high theoretical specific energy of 2600 Wh/kg. However, several drawbacks still exist in case of liquid LSB-concepts, especially cycling stability with low electrolyte excess in combination with a reasonable sulfur utilization plus cycle stability still hinders the commercial breakthrough of this battery technology. One main reason for both issues is the dissolution of the active material, sulfur, as polysulfides in the electrolyte, which leads to the so-called polysulfide shuttle that comprises polysulfide diffusion through the cell to the lithium metal anode resulting in decomposition reactions, and therefore, loss of active material. Several electrolyte approaches in order to limit polysulfide dissolution have been developed over the last 5-10 years, however, those electrolyte formulations usually lead to a strong lithium metal corrosion. Electrolytes that enable stable cycling of lithium metal batteries in combination with a nickel manganese cobalt oxide cathode have been successfully developed, however, they are ususally not compatible with the polysulfides of Li-S batteries. Hence, decoupling the anolyte from the catholyte has been much desirable. Recently introduced solid-state lithium sulfur batteries based on sulfidic solid electrolytes might overcome some challenges of conventional liquid LSBs since no formation or diffusion of polysulfide species can take place, and very high sulfur utilization have been already reached. However, solid-state LSBs have not been cycleable so far when a thin layer of solid electrolyte and lithium metal anode (without indium) were employed, especially in pouch cells, due to the formation of lithium dendrites, resulting in short circuits.Herein, a completely new battery design, a “semi-solid”-LSB, is presented. The concept combines the advantages of liquid and solid state LSBs. On the cathode side, an electrode comprising carbon, sulfur and sulfidic solid electrolyte (argyrodite) enables a solid to solid conversion of sulfur resulting in a complete suppression of the polysulfide shuttle.On the anode side, a liquid electrolyte enabling stable cycling of a lithium metal anode is employed. A careful design of the liquid electrolyte is crucial in order to obtain high stability of the liquid electrolyte against the lithium metal anode as well as to avoid side reaction between the solid electrolyte of the cathode and the liquid electrolyte. Different electrolytes are discussed for the new cell design and proof of concept was successfully reached in coin cells leading to 100 cycles with a stable coulombic efficiency of over 99 % which outperforms the majority of previously published Li-S cycling data. In addition, the concept was also transferred into first semi-solid lithium sulfur-pouch cells which is an important step in the direction of practical applications.

Enhanced performance of graphene-incorporated electrodes for solid-state lithium-sulfur batteries through facilitated ionic diffusion pathways

Significant progress has been achieved in advancing all-solid-state lithium-sulfur batteries through the development of sulfide solid electrolytes. Nonetheless, a challenge lies in creating a percolated ion–electron conduction path with intimate contact between charge carriers throughout the cathode which is crucial for enhancing overall efficiency and addressing issues related to slow kinetics and impedance during battery operation. This study introduces a framework elucidating how the integration of graphene enhances electrode performance by refining ionic diffusion pathways. An idealized ionic diffusion pathway characterized by a continuous ionic network, facilitating minimum diffusion distances, is proposed. Through a parametric study substituting portions of ionic and electronic conductive agents with graphene, the impact on total ionic and electronic conductivity of positive electrodes was comprehended. The findings underscore the critical role of optimum graphene content, which fills the gaps between ionic conductive materials and creates the shortest diffusion paths for ions and electrons. While incorporating graphene into cathode electrodes is not novel, it is noteworthy that graphene, as a mixed ion–electron conductive material, significantly enhances ion mobility due to its 2D structure, addressing a crucial aspect of cathode performance. Upon achieving optimum composite formulation, empirical findings demonstrate substantial performance improvement, including a 17.7% increase in initial capacity and a remarkable 21% enhancement in capacity retention compared to electrodes without graphene.

Unlocking high-energy solid-state lithium-sulfur batteries with an innovative double-layer hybrid solid electrolyte

This study developed a novel double-layer hybrid solid electrolyte (DLHSE) to address the limitations of solid-state lithium–sulfur (Li–S) batteries, which include poor electronic/ionic conductivity, interfacial chemical/electrochemical instability, and substantial interfacial resistance between the solid electrolyte and electrodes. The DLHSE comprises an ion-conducting ceramic, electrochemically stable polymer, and ether-based liquid electrolyte. Specifically, the dual-layer ceramic skeleton comprises an inorganic NASICON-type Li1+xAlxTi2-x(PO4)3 (LATP) layer facing the cathode to facilitate Li+ migration at the interface and a garnet-type Li7La3Zr2O12 (LLZO) layer facing the anode to suppress Li dendrite formation and mitigate the “shuttle effect”. The polymer binder (PVDF–TrFE) can create a three-dimensional network to enhance structural compactness and stability. The penetrating ether-based electrolyte can facilitate Li+ transfer and reinforce the interfacial contact. Furthermore, a well-designed porous carbon rod/sulfur (PCR/S) composite with an ultrahigh sulfur content of 80 wt% was prepared as the cathode. Consequently, the novel structural configuration with PCR/S cathode and DLHSE, not only demonstrated excellent coin-cell performance with a capacity retention of 802 mAh g−1 after 500 cycles at 0.2C, but also an outstanding A-h-level pouch cell with an impressive discharge capacity of 7 Ah at 0.1C.

Modulating Ionic Conduction and Accelerating Sulfur Conversion Kinetics through Oxygen Vacancy Engineering for High‐Performance Solid‐State Lithium‐Sulfur Batteries

AbstractPoly(ethylene oxide) (PEO)‐based solid‐state lithium‐sulfur batteries (SSLSBs) have garnered considerable attention as potential energy storage solutions owing to their exceptional specific energy, ease of processing, and economic viability. Nevertheless, the inherently low Li+ conductivity of the PEO electrolyte and the inevitable dissolution of lithium polysulfides (LiPSs) within the sulfur cathode hinder the solid‐state sulfur conversion kinetics and lead to significant loss of active materials, thus posing challenges for practical applications. Herein, these concerns are addressed by incorporating oxygen vacancy enriched‐Nb22W20O102‐x (NWOx) nanorods as cathode additives in high‐performance PEO‐based SSLSBs. The uniformly dispersed NWOx nanorods effectively modify the coordination environment of Li ions by increasing the concentration of free Li ions in the PEO catholyte and alleviating the shuttle effect of dissolved LiPSs. Consequently, the developed SSLSB demonstrates excellent cyclic stability and rate capability. Specifically, it achieves a high discharge capacity of 1208.6 mAh g−1 during the initial cycle and maintains 927.8 mAh g−1 after 200 cycles at 0.1 C. Moreover, such a configuration can accommodate a high loading of active materials with stable capacity retention. Overall, this study presents an effective approach for developing solid‐state sulfur cathodes in PEO‐based SSLSBs.

The role of nanoporous carbon materials for thiophosphate-based all solid state lithium sulfur battery performance

Due to their high theoretical energy density, all solid state lithium sulfur batteries (LS-SSB) represent one of the most promising candidates for next-generation energy storage systems. Whilst high sulfur utilizations have been published for several cathode compositions and preparation methods in recent years, there is still a lack of clarity regarding the influence of the used carbon. Furthermore, LS-SSBs face challenges in up-scaling as the common preparation methods including high energy ball milling are time consuming, batch-wise and need high energy impact. In this study, high sulfur utilization >1600 mAh gS−1 and reversibility with 80 % of initial discharge capacity after 60 cycles is achieved, using a more time-efficient preparation method with drastically lowered energy impact by selecting a suitable carbon. Additionally, the influence of the carbon nanostructure on the electrochemical performance is discussed. This study provides guidance in selecting nanostructured carbon materials to enable cost-efficient, up-scalable preparation methods for LS-SSBs without compromising on the excellent electrochemical performance.

Selenium-Doped Sulfurized Polyacrylonitrile Hybrid Cathodes with Ultrahigh Sulfur Content for High-Performance Solid-State Lithium Sulfur Batteries.

The solid-state lithium sulfur battery (SSLSB) is an attractive next-generation energy storage system by reason of its remarkably high energy density and safety. However, the SSLSB still faces critical challenges, such as sluggish reaction kinetics, mismatched interface, and undesirable reversible capacity. Herein, a high-performance SSLSB is reported using sulfurized polyacrylonitrile with rich selenium-doped sulfur (Se/S-S@pPAN) as a cathode and poly(ethylene oxide)/Li7La3Zr1.4Ta0.6O12 (PEO-LLZTO) as an electrolyte. The sulfur content of the cathode up to 60.9 wt % can be achieved by dispersing selenium sulfide (SeSx) species in the sulfurized polyacrylonitrile (S@pPAN) skeleton at a molecular level. Selenium as a eutectic accelerator can be uniformly distributed in the composite through the Se-S bond and can accelerate the reaction kinetics. The PEO-LLZTO hybrid solid-state electrolyte (SSE) displays an attractive electrochemical performance and provides an intimate contact with electrodes. At 60 °C, Se/S-S@pPAN delivers an impressive discharge capacity of 1042 mAh g-1 at 0.1C and 445 mAh g-1 at 1C. Additionally, the LiFePO4 cathodes combined with PEO-LLZTO deliver a high reversible capacity (158.9 mAh g-1, 1C) and an ultralong lifespan (a capacity retention of 80%, 1000 cycles) at 1C. The synergetic design of the high-performance sulfur cathode and the organic/inorganic hybrid electrolyte is crucial for enabling the high-performance SSLSB.

Laminar Composite Electrolytes with Nanoporous Sulfonated Covalent Organic Framework-Confined Crown Ether for Solid-State Lithium–Sulfur Batteries

Laminar Composite Electrolytes with Nanoporous Sulfonated Covalent Organic Framework-Confined Crown Ether for Solid-State Lithium–Sulfur Batteries

Interfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries

Coupling high-capacity cathode and Li-anode with solid-state electrolyte has been demonstrated as an effective strategy for increasing the energy densities and safety of rechargeable batteries. However, the limited ion conductivity, the large interfacial resistance, and unconstrained Li-dendrite growth hinder the application of solid-state Li-metal batteries. Here, a poly(ether-urethane)-based solid-state polymer electrolyte with self-healing capability is designed to reduce the interfacial resistance and provides a high-performance solid-state Li-metal battery. With its dynamic covalent disulfide bonds and hydrogen bonds, the proposed solid-state polymer electrolyte exhibits excellent interfacial self-healing ability and maintains good interfacial contact. Full cells are assembled with the two integrated electrodes/electrolytes. As a result, the Li||Li symmetric cells exhibit stable long-term cycling for more than 6000 h, and the solid-state Li-S battery shows a prolonged cycling life of 700 cycles at 0.3 C. The use of ultrasound imaging technology shows that the interfacial contact of the integrated structure is much better than those of traditional laminated structure. This work provides an interesting interfacial dual-integrated strategy for designing high-performance solid-state Li-metal batteries.

An artificial cathode-electrolyte interphase enabling one-step sulfur transition in polyethylene oxide-based solid-state lithium–sulfur batteries

An artificial CEI is developed for PEO-based solid-state Li–S batteries, which inhibits the cohesion and dissolution of polysulfides in PEO and enables a one-step solid-state transition of sulfur.

Novel PEO-based composite solid electrolytes for All-Solid-State Li-S battery

Solid polymer electrolytes (SPEs) were investigated for several decades due to their good compatibility with electrodes. However, meeting the essential requirements for solid polymer electrolytes, including enhanced ionic conductivity, superior solubility with conductive lithium salts, and robust interface stability when in contact with a Li anode, remains a formidable challenge. In our work, we found that transition metal carbides (NiNbCeC) over mesoporous silica (SBA-15) can be filled into the Polyethylene Oxide (PEO) matrix to form composite solid electrolytes which can greatly improve the ionic conductivity of PEO. We investigate a series of transition metal carbides with varying mass ratios of Cerium (5%, 10%, and 20%) to fabricate All-Solid-State Li-S batteries (ASSLi-S). Our results demonstrate that different mass ratios of Cerium play a pivotal role in enhancing the ionic conductivity of the composite solid electrolytes, reducing impedance levels from 9150 O (20% Ce) to 4000 O (5% Ce) to 1730 O (10% Ce). At room temperature, the high initial specific capacity at 1C and reversible specific capacity after 100 cycles are 525 and 363 mAh/g, 605 and 403 mAh/g, 246.3 mAh/g and 63.28 mAh/g for 5% Ce, 10%, and 20%, respectively. Furthermore, long-term cycling tests of ASSLi-S cells at 0.5C reveal promising performance, with the cell containing 10% Ce solid electrolytes delivering an initial specific capacity of 1165.7 mAh/g and maintaining 335 mAh/g after 200 cycles. This represents a significant breakthrough, demonstrating that PEO-based solid electrolytes can achieve impressive electrochemical results at room temperature. SEM characterization was employed to assess the volume change in the solid electrolyte layer and elemental distribution of solid electrolyte materials through cross-sectional analysis. This analysis revealed that the failure modes of solid-state Li-S cells can also be attributed to the migration of sulfur elements from the cathode to the solid electrolyte layer during the cycling process. XRD was utilized to study the crystallinity of composite solid electrolytes. This study represents a significant stride in the progress of high-performance solid polymer electrolytes for All-Solid-State Li-S batteries, shedding light on the failure modes of such batteries. It underscores the potential of composites based on transition metal carbides in addressing crucial challenges for their practical implementation in Solid-State Lithium-Sulfur Batteries.

A Fully Amorphous, Dynamic Cross-Linked Polymer Electrolyte for Lithium-Sulfur Batteries Operating at Subzero-Temperatures.

Solid-state lithium-sulfur batteries have shown prospects as safe, high-energy electrochemical storage technology for powering regional electrified transportation. Owing to limited ion mobility in crystalline polymer electrolytes, the battery is incapable of operating at subzero temperature. Addition of liquid plasticizer into the polymer electrolyte improves the Li-ion conductivity yet sacrifices the mechanical strength and interfacial stability with both electrodes. In this work, we showed that by introducing a spherical hyperbranched solid polymer plasticizer into a Li+ -conductive linear polymer matrix, an integrated dynamic cross-linked polymer network was built to maintain fully amorphous in a wide temperature range down to subzero. A quasi-solid polymer electrolyte with a solid mass content >90 % was prepared from the cross-linked polymer network, and demonstrated fast Li+ conduction at a low temperature, high mechanical strength, and stable interfacial chemistry. As a result, solid-state lithium-sulfur batteries employing the new electrolyte delivered high reversible capacity and long cycle life at 25 °C, 0 °C and -10 °C to serve energy storage at complex environmental conditions.

G-C3N4 Boosting the Interfacial Compatibility of Solid-State Lithium-Sulfur Battery

The poor interfacial compatibility between solid electrolyte and lithium metal anode is one of the main obstacles to the development of solid lithium metal battery. Herein, the poly (1,3-dioxolane) (PDOL) polymer is combined with g-C3N4 powders to form a flexible and dense composite solid electrolyte film, which not only possesses high ionic conductivity of 3.7 × 10−4 S·cm−1, high ion migration number up to 0.86, and wide electrochemical stability window of 5.0 V, but also is helpful for inhibiting the growth of lithium dendrites to improve the interfacial stability of the lithium anode and close contact with cathode. The prepared S/g-C3N4-PDOL/Li battery exhibits good rate and cycle performances with a capacity of 550 mAh g−1 at 1 C, and 1150 mAh g−1 at 0.1 C with a capacity retention rate of 83% after 100 cycles. The dense Li3N layer generated by the reaction between g-C3N4 and Li gives g-C3N4/PDOL composite electrolyte a high inhibition ability of lithium dendrites. This composite solid electrolyte film with an interface modification function has good practical application prospects in lithium-sulfur batteries.

A high ion conductive solid electrolyte film and interface stabilization strategy for solid-state Li-S battery

Lithium-sulfur (Li-S) batteries are regarded as a potential next-generation electrochemical energy storage technology. However, polysulfide shuttle effect and lithium dendrite growth always worsen the battery's cycling performance, especially, the safety problem of liquid electrolyte has also become a major challenge to the development and application of Li-S batteries. Herein, a high ion conductive poly(1,3-dioxolane) solid electrolyte film (PDOL) was introduced in Li-S battery, which hinders the shuttle of polysulfides, and forms a uniform LiF protective layer on the lithium metal contact surface to inhibit the growth of lithium dendrites. Meanwhile, the problem of high interfacial impedance in solid-state Li-S batteries was also solved by adding a trace amount of flexible organic ether electrolyte to the solid electrolyte/electrode interface. The assembled quasi-solid-state S/PDOL/Li cell shows low interfacial impedance less than 75 Ω and can be stably cycled over 500 times at 0.1 C. This rigid-flexible solid electrolyte design method provides a practical idea for the development of high-performance solid-state Li-S batteries.

High energy and sustainable solid-state lithium-sulfur battery enabled by the force-bearing cathode and multifunctional double-layer hybrid solid electrolyte

High energy and sustainable solid-state lithium-sulfur battery enabled by the force-bearing cathode and multifunctional double-layer hybrid solid electrolyte

Optimizing Sulfur Utilization in High Loading Cathode for All-Solid-State Lithium-Sulfur Battery

All Solid-state Lithium-Sulfur battery (ASSLSB) possesses a great promise in providing a safe, high energy density, and low cost battery technology for vehicle electrification and grid energy storage. To achieve practically high specific energy in ASSLSB (e.g., >400 Wh/Kg), sulfur cathodes with high areal capacity (>6 mAh cm-2) are essentially needed to offset the relatively low working voltage of elemental sulfur cathode (1.9 V vs. Li). This requires high mass loading sulfur cathodes by maximizing both sulfur content in the whole electrode and sulfur utilization rate to reduce the parasitic weights. An optimal electrode architecture featuring sufficiently connected sulfur/solid electrolyte/carbon triple interfaces is desired to enable sulfur’s fast accessibility to electron and Li-ion simultaneously. Due to the non-flowability of those three solid components, however, it is very hard to maximize the contact of trip solid phases, which need new insights of the materials design and processing technology.This work looks at carbon microstructures and their impact on triple-point contact between electrochemically active sulfur, carbon, and the solid-state electrolyte (SSE) that comprises most composite cathodes in ASSLSB systems. While significant work has gone into understanding and developing novel carbon host structures for liquid Li-S cells for improving sulfur utilization, polysulfide trapping, better understanding is needed for ASSLSBs. Specifically, how sulfur infiltration, loading, and spatial distribution within the porous carbon host impacts sulfur utilization. Understanding how the infiltrated sulfur that resides in the porous carbon host connects with both carbon and solid electrolyte networks across the whole electrode structure and maintains its robustness during the repeated cell cycling is needed to achieve full utilization in high sulfur loading electrodes. The solid sulfur cathode system examined in the present study is a composite of porous carbon, sulfur, and a sulfide-based solid electrolyte. A combination of porous carbon hosts is investigated and correlated to the cell performance at practical conditions. Advanced characterization and computational tools are used to further elucidate the key parameters for high sulfur utilization in ASSLSBs with high sulfur loading cathodes. Details of the study will be presented and discussed at the meeting.Reference:(1) Nagata, H. and Y. Chikusa (2016). "All-Solid-State Lithium–Sulfur Battery with High Energy and Power Densities at the Cell Level." Energy Technology 4(4): 484-489(2) Banerjee, A., et al. (2020). "Interfaces and Interphases in All-Solid-State Batteries with Inorganic Solid Electrolytes." Chemical Reviews 120(14): 6878-6933.