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The dry-process is a sustainable and promising fabrication method for all-solid-state batteries by eliminating solvents. However, a pragmatic fabrication design for thin and robust solid-state electrolyte (SSE) layers has not been established. Herein, we report a dry-process approach that enhances mechanical stability of SSE layers from film fabrication to cell operation. By co-rolling thick SSE and positive electrode feeds, a uniform, thin SSE layer (50 µm) and a high loading positive electrode layer (5 mAh cm −2 ) with high active material ratio (80 wt%) are simultaneously achieved. This SSE-positive electrode integrated film exhibits enhanced physical properties and cyclability (> 80% retention after 500 cycles) at low stack pressure (2 MPa) compared to the freestanding counterparts, attributed to reinforced and intimate SSE-positive electrode interface constructed during co-rolling process. Additionally, an all-solid-state pouch cell with high stack-level specific energy (310 Wh kg −1 ) and energy density (805 Wh L −1 ) operating at 30 °C and 5 MPa is demonstrated. All-solid-state batteries face practical challenges such as sustainable fabrication and low-stack pressure operation. Here, authors develop a modified dry-process technique to yield robust solid electrolyte-electrode interface for practical fabrication and operation of all-solid-state batteries.

All-solid-state batteries using sulfur-based positive electrodes (cathodes) offer a cost-effective route to achieve high specific energy. However, low active material utilization and cycle life hinder performance. Here, we demonstrate a positive electrode design that employs sulfide solid-state electrolytes, where a high energy synthesis approach forms a metastable and ionically conductive interphase on the active material surface. This interphase facilitates high active material utilization and contributes capacity with cycling. We also show that tailoring active material particle sizes to the micron-scale improves rate performance and cycling stability. Structural analysis reveals that the substantial volume change of sulfur-based positive electrodes during operation can partially offset that of the negative electrodes, thereby mitigating internal mechanical stress. The combined design principles enable sulfur areal capacities up to 11 mAh cm -2 while maintaining stable cycling at 25 °C. We further demonstrate several specific-energy-focused cell architectures, particularly a Li 2 S anode-free pouch cell that operates under “low stack pressure” of 10 MPa. This work outlines practical design strategies for constructing high-specific-energy all-solid-state batteries for a broad range of emerging applications. Solid-state lithium-sulfur batteries face practical challenges such as low utilization and cycle life. Here, authors introduce design strategies that enable practical operation, leading to the demonstration of a high loading Li 2 S-anode free pouch cell that operates under “low stack pressure” of 10 MPa.

The growth of the semiconductor and solar industry has been exponential in the last two decades due to the computing and energy demands of the world. Silicon (Si) is one of the main constituents for both sectors and, thus, is used in large quantities. As a result, a lot of Si waste is generated mainly by these two industries. For a sustainable world, the circular economy is the key; thus, the waste produced must be upcycled/recycled/reused to complete the circular chain. Herein, we show that an upcycled/recycled Si can be used with carbon as a composite anode material, with high Si content (~40 wt.%) and loading of 3-4 mAh/cm^2 for practical use in lithium-ion batteries. The unique spherical jackfruit-like structure of the Si-C composite can minimize the total lithium inventory loss compared to the conventional Si-C composite and pure Si, resulting in superior electrochemical performance. The superior electrochemical performance of Si-C composites enables the cell energy density of ~325 Wh/kg (with NMC cathode) and ~260 Wh/kg (with LFP cathode), respectively. The results demonstrate that Si-based industrial waste can be upcycled for high-performance Li-ion battery anodes through a controllable, scalable, and energy-efficient route.

All-solid-state batteries are emerging as potential successors in energy storage technologies due to their increased safety, stemming from replacing organic liquid electrolytes in conventional Li-ion batteries with less flammable solid-state electrolytes. However, All-solid-state batteries require precise control over cycling pressure to maintain effective interfacial contacts between materials. Traditional uniaxial cell holders, often used in battery research, face challenges in accommodating electrode volume changes, providing uniform pressure distribution, and maintaining consistent pressure over time. This study introduces isostatic pouch cell holders utilizing air as pressurizing media to achieve uniform and accurately regulated cycling pressure. LiNi0.8Co0.1Mn0.1O2 | Li6PS5Cl | Si pouch cells were fabricated and tested under 1 to 5 MPa pressures, revealing improved electrochemical performance with higher cycling pressures, with 2 MPa as the minimum for optimal operation. A bilayer pouch cell with a theoretical capacity of 100 mAh, cycled with an isostatic pouch cell holder, demonstrated a first-cycle Coulombic efficiency of 76.9% and a discharge capacity of 173.6 mAh g-1 (88.1 mAh), maintaining 83.6% capacity after 100 cycles. These findings underscore the effectiveness of isostatic pouch cell holders in enhancing the performance and practical application of All-solid-state batteries.