Scalable Processing Routes for the Production of All‐Solid‐State Batteries—Modeling Interdependencies of Product and Process

Abstract

The expansion of renewable energies and the enactment of laws to reduce emissions are encouraged by climate policies. As part of this, the electrification of the global automotive market is progressing but still suffers from customer unacceptance. [1,2] In the future, the usage of electric vehicles will highly depend on the progress of associated technical core components such as the lithium-ion battery (LIB). [3] The development of energy storage, therefore, is of decisive importance to optimize sustainable energy systems and to mitigate environmental pollution. [4,5] LIBs are the key technology in electric vehicles to accomplish market and customer requirements. [6] These relate especially to the driving range and the charging time [7] throughout operational safety. [8] The main proposed advantage of the all-solid-state batteries (ASSBs) is their increased safety, which results from replacing the flammable and toxic liquid electrolyte in LIBs with a solid ion conductor. Furthermore, the application of metal anodes, e.g., pure lithium, to enhance the energy and power density is discussed to be most likely achieved by the use of a dense and mechanically stable solid electrolyte. [9] Although polymers, sulfidic, ceramic oxide-based and halide materials are identified as promising solid-state electrolytes, [10] challenges arise in the identification of material compatibilities, suitable cell designs, and production technologies. [11] Yet, the development of production processes for thin-layer [12] and large-format ASSBs is crucial for successfully bridging the gap between laboratory research and the industrial market. [13,14] The production of ASSB cells for electrochemical research purposes and first process sequences of different technologies are described in various publications. [11,15-24] However, a systematic study on processing routes considering every value-adding production step and related parameters in dependence of the cell design is omitted. Novel materials and components of ASSBs are characterized by interdependencies among each other, [25] which in turn are affecting the respective production steps. [19] (Electro-)chemical obstacles regarding the choice of materials, blocking interfaces, and instabilities influence the scalability of processes. The high uncertainty about a suitable production line, therefore, has a major impact on impeding the industrial application. [21] In this article, a detailed system model for ASSBs and scalable production technologies is presented. Interdependencies between the processes and the product structure of ASSBs are considered. The method consists of five sub-models, which

Enhanced Room-Temperature Ionic Conductivity of NaCB11H12 via High-Energy Mechanical Milling

“…In the past years, both Li-and Na-based solid ionic conductors have been developed that rival, and in some cases beat, the ionic conductivity of current liquid electrolytes. 12−15 Other drawbacks plaguing SSBs that need to be urgently tackled are the narrow electrochemical voltage window, 7 limited chemomechanical stability, 6,16 poor compatibility with electrodes, 17,18 and a thorough determination of the stack pressure. 19,20 Focusing on Na-ion conductors, several classes of chemical compounds acting as SEs have been investigated, e.g., β-Al 2 O 3 and NASICON, that despite their good chemical stability require harsh synthesis conditions and suffer from poor electrode contact at rt; 6 sulfide-based compounds, such as thiophosphates (cubic Na 3 PS 4 , 21 Na 11 Sn 2 PS 12 13 ), and P-replacing derivatives Na 3 SbS 4 , 22 although being softer and more easily processable, provide limited electrochemical stability.…”

“…Finally, their production can skip several conditioning steps needed for the fabrication of conventional cells, thus reducing costs, as already shown for Li-based counterparts. , The challenge for Na-ASSBs has been mainly the development of room-temperature (rt) fast ion conductors that withstand elevated current densities. In the past years, both Li- and Na-based solid ionic conductors have been developed that rival, and in some cases beat, the ionic conductivity of current liquid electrolytes. − Other drawbacks plaguing SSBs that need to be urgently tackled are the narrow electrochemical voltage window, limited chemomechanical stability, , poor compatibility with electrodes, , and a thorough determination of the stack pressure. , Focusing on Na-ion conductors, several classes of chemical compounds acting as SEs have been investigated, e.g., β-Al 2 O 3 and NASICON, that despite their good chemical stability require harsh synthesis conditions and suffer from poor electrode contact at rt; sulfide-based compounds, such as thiophosphates (cubic Na 3 PS 4 , Na 11 Sn 2 PS 12 ), and P-replacing derivatives Na 3 SbS 4 , although being softer and more easily processable, provide limited electrochemical stability. , Furthermore, an emerging class of antiperovskites, with general formula Na 3 OX (X = Cl, Br, I, BH 4 ) is less prone to oxidation, but their compatibility with metal anode and their conductivity are still a matter of discussion.…”

From Lithium‐Metal toward Anode‐Free Solid‐State Batteries: Current Developments, Issues, and Challenges

“…Although the cost reduction by the transition from LMSSB to AFSSB cannot yet be fully quantified reliably, it is clear that there is enormous potential for savings. To reliably estimate these crucial characteristics, future cost and production models [41,51] should also take the anode-free configuration…”

Solid‐State Post Li Metal Ion Batteries: A Sustainable Forthcoming Reality?

“…The difficulties to transition from lab‐scale to large‐scale solid‐state cells, together with the advantages, issues and challenges of solid‐state design are addressed in several specific reviews. [ 20,109–111 ] At present the focus is mainly on Li‐ and Na‐based battery technologies, but most concepts generally might apply to any all‐solid batteries, despite the small number of reports on solid electrolytes for many post‐Li chemistries, which are in some case relatively new (e.g., the Ca‐plating/stripping was first demonstrated in 2016 [ 72 ] ).…”