Scaling up high-energy-density sulfidic solid-state batteries: A lab-to-pilot perspective

Organic‐Additive‐Derived Cathode Electrolyte Interphase Layer Mitigating Intertwined Chemical and Mechanical Degradation for Sulfide‐Based Solid‐State Batteries

“…To alleviate the mechanical degradation for securing the ionic and electronic percolation path in the cathode composite, high stack pressure (tens or hundreds of MPa) is generally applied in the operation of an SSB. [56][57][58] Therefore, to elucidate the function of the LiDFBOP-derived CEI layer in mitigating mechanical degradation, we investigated the cathode-solid electrolyte interfacial resistance change as the state of charge (SOC) at low stack pressure below 1 MPa (Figure 3a,b). At a low stack pressure of 0.75 MPa, a larger overpotential was observed at the bare NCM compared with the LiDFBOP-coated NCM, where more than 0.45 lithium was extracted from the NCM cathode (SOC 55).…”

Current Status of Formulations and Scalable Processes for Producing Sulfidic Solid‐State Batteries

“…While this publication is limited to sulfidic SEs and focuses on the process engineering implementation of the steps from synthesis to calendering, the works of Schnell et al., [1] Duffner et al [147] . and Tan et al [148] . are recommended for the study of alternative SSB concepts, as well as economic perspectives.…”

“…[145,146] According to Jung et al, the current collector acts both as positive and negative pole, unit cells do not have to be packed and sealed individually and cell modules can be achieved by sequentially stacking or laminating of the cathode, current collector, anode and separator without external wiring. [146] While this publication is limited to sulfidic SEs and focuses on the process engineering implementation of the steps from synthesis to calendering, the works of Schnell et al, [1] Duffner et al [147] and Tan et al [148] are recommended for the study of alternative SSB concepts, as well as economic perspectives.…”

Liquid‐Phase Synthesis of Highly Deformable and Air‐Stable Sn‐Substituted Li3PS4 for All‐Solid‐State Batteries Fabricated and Operated under Low Pressures

“…[1][2][3][4][5][6][7][8][9][10][11] In particular, highly conductive sulfide solid electrolytes (SEs) are mechanically deformable, which allows for scalable fabrication of practical all-solid-state Li batteries (ASLBs) by simple cold-pressing processes, such as isostatic pressing, areal pressing, and roll-pressing. [3,7,12,13] A critical drawback of sulfide SEs is their poor chemical stability toward atmospheric air; upon exposure to atmospheric air, they are degraded with the release of toxic H 2 S. [3,14] The substitution of phosphorus with metals, such as Sn and Sb, has been effective in alleviating the reactivity of sulfide SEs with air (Table S1, Supporting Information), which can be explained via hard and soft acid and base theory. [15][16][17][18][19][20] Similar to other types of ceramic electrolytes, solid-state syntheses (SS), such as mechanochemical methods, hightemperature solid-state reactions, and meltquenching methods, are also commonly used for the preparation of sulfide SEs.…”

“…Although sulfide SEs are mechanically sinterable, the extremely high pressure required for compaction (e.g., above 300 MPa) remains a technical challenge for the mass production of ASLBs. [ 13,42,43 ] Moreover, most lab‐scale ASLB cells have been tested under unrealistically high operating (or stack) pressures (e.g., ≈70 MPa), which blurs serious electrochemo‐mechanical degradation. [ 43–45 ] In this regard, the material design of SEs for controlling their mechanical properties is imperative for practical ASLBs.…”