Low temperature sintering of fully inorganic all-solid-state batteries – Impact of interfaces on full cell performance

Ihrig, Martin; Finsterbusch, Martin; Tsai, Chih‐Long; Laptev, Alexander M.; Tu, Chia Hao; Bram, Martin; Sohn, Yoo Jung; Ye, Ruijie; Sevinc, Serkan; Lin, Shih‐kang; Fattakhova‐Rohlfing, Dina; Guillon, Olivier

doi:10.1016/j.jpowsour.2020.228905

Cited by 60 publications

(94 citation statements)

References 55 publications

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“…3 for lithium aluminum titanium phosphate (LATP) electrolyte, it is possible to densify ceramics at much reduced temperatures compared to free sintering. They might for instance bring solutions to the current challenge of co-sintering mixed cathode for solid-state batteries [16,17].…”

Section: Accepted Articlementioning

confidence: 99%

“…They might, for instance, bring solutions to the current challenge of co-sintering mixed cathode for solid-state batteries. 16,17 Still, stringent efforts are required to transfer the accumulated laboratory-scale experience to industrial mass production, but by choosing interesting business cases, new sintering technologies can make their way toward commercialization. Looking back at the development of field-assisted sintering technology/spark plasma sintering over the last years, both diversified product range and automatization have enabled to make use of such innovation.…”

Section: On the Importance Of Materials Integration And Processingmentioning

confidence: 99%

“…As shown in Figure 3 for lithium‐aluminum‐titanium‐phosphate (LATP) electrolyte, it is possible to densify ceramics at much reduced temperatures compared with free sintering. They might, for instance, bring solutions to the current challenge of co‐sintering mixed cathode for solid‐state batteries 16,17 . Still, stringent efforts are required to transfer the accumulated laboratory‐scale experience to industrial mass production, but by choosing interesting business cases, new sintering technologies can make their way toward commercialization.…”

Section: On the Importance Of Materials Integration And Processingmentioning

confidence: 99%

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Ceramic materials for energy conversion and storage: A perspective

Guillon

2021

Int J Ceramic Engine & Sci

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Advanced ceramic materials with tailored properties are at the core of established and emerging energy technologies. Applications encompass high-temperature power generation, energy harvesting and electrochemical conversion and storage. New opportunities for materials design, the importance of processing and material integration and the need for long-term testing under realistic conditions are highlighted in the present perspective.

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Section: Accepted Articlementioning

confidence: 99%

Section: On the Importance Of Materials Integration And Processingmentioning

confidence: 99%

Section: On the Importance Of Materials Integration And Processingmentioning

confidence: 99%

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Ceramic materials for energy conversion and storage: A perspective

Guillon

2021

Int J Ceramic Engine & Sci

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“…In the field of All Solid-State Li-ion Batteries (ASSLiB), mainly Spark Plasma Sintering (SPS) has been used to shape and sinter entire multi-material systems based on NASICONtype Li + ionic conductors such as Li 1+x Al x Ti 2-x (PO 4 ) 3 (LATP) or Li 1+x Al x Ge 2-x (PO 4 ) 3 (LAGP) [29][30][31] or, more recently, on garnet-based electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) with LiCoO 2 (LCO) as positive electrode material. 32,33 SPS does not require any charge transfer reaction because the sample is heated by an external source. However, SPS requires a more complex and expensive equipment than FS, as well as a special graphite die which can lead to reduction of some components (the active materials (eg, LCO) and the electrolyte (eg, LATP) in such multi-material systems.…”

Section: Introductionmentioning

confidence: 99%

“…In the field of All Solid‐State Li‐ion Batteries (ASSLiB), mainly Spark Plasma Sintering (SPS) has been used to shape and sinter entire multi‐material systems based on NASICON‐type Li + ionic conductors such as Li 1+x Al x Ti 2‐x (PO 4 ) 3 (LATP) or Li 1+x Al x Ge 2‐x (PO 4 ) 3 (LAGP) 29‐31 or, more recently, on garnet‐based electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) with LiCoO 2 (LCO) as positive electrode material 32,33 . SPS does not require any charge transfer reaction because the sample is heated by an external source.…”

Section: Introductionmentioning

confidence: 99%

Flash sintering of cationic conductive ceramics: A way to build multilayer systems

et al. 2021

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Flash Sintering (FS), that allows densifying ceramics at low furnace temperature in a few seconds, requires a reversible electrochemical reaction to enable the current flow through the electrode / material interface. For Li + pure ionic conductors such as Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP), the best material to ensure this fast charge transfer reaction is a mixed Li + /e − conductor, eg, LiCoO 2 (LCO). This paper demonstrates the feasibility of FS on LCO between two Pt electrodes and on multi-layers systems using LCO or LATP+LCO composite as electrodes. It is shown that a composite electrode both allows the flash event to occur and prevents the delamination possibly observed with pure LCO by lowering interfacial stresses.

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The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

Scheld

Kim

Schwab

et al. 2023

Adv Funct Materials

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Solid‐state batteries (SSBs) with a Li7La3Zr2O12 (LLZO) garnet electrolyte are attracting much attention as robust and safe alternative to conventional lithium‐ion batteries. Technical challenges in the practical implementation of garnet SSBs are related to the need for high‐temperature sintering, which often leads to undesirable chemical reactions with the cathode material. While these reactions are well understood for composite cathodes, very little is known about similar processes between cathode and separator during battery fabrication. This work focuses on understanding the processes between the composite LiCoO2‐LLZO cathode and the LLZO separator and how they affect the battery performance. The extensive diffusion of Co‐ions within LLZO, which leads to the often‐observed LLZO darkening, is shown to have a significant impact on ionic conductivity, electronic conductivity, and dendrite stability of the separator. Experimental data coupled with large‐scale molecular dynamics simulations uncover the diffusion mechanism for Co‐ions and identify secondary phases that form during these interactions. In addition to extensive Co‐ion diffusion within the grains, a non‐uniform segregation of Co‐ions at grain boundaries is found leading to the formation of three distinct Co‐containing phases. This work offers a general approach to studying the fundamental ion diffusion processes that occur during the fabrication of oxide SSBs.

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Low temperature sintering of fully inorganic all-solid-state batteries – Impact of interfaces on full cell performance

Cited by 60 publications

References 55 publications

Ceramic materials for energy conversion and storage: A perspective

Ceramic materials for energy conversion and storage: A perspective

Flash sintering of cationic conductive ceramics: A way to build multilayer systems

The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

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