Study of failure modes in two sulphide-based solid electrolyte all-solid-state batteries via in situ SEM

Autor: Neelam Ghanshyam Yadav, Nicolas Folastre, Mickael Bolmont, Arash Jamali, Mathieu Morcrette, Carine Davoisne
Přispěvatelé: Laboratoire réactivité et chimie des solides - UMR CNRS 7314 (LRCS), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Advanced Lithium Energy Storage Systems - ALISTORE-ERI (ALISTORE-ERI), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Rok vydání: 2022
Předmět:
Zdroj: Journal of Materials Chemistry A
Journal of Materials Chemistry A, 2022, 10 (33), pp.17142-17155. ⟨10.1039/d2ta01889f⟩
ISSN: 2050-7496
2050-7488
Popis: International audience; Lithium metal was left unused for a long time in conventional liquid-based batteries, with a fear of catching fire for safety reasons. However, with advancements in solid electrolytes, these were considered the holy grail in the development of Li metal-based all-solid-state batteries (ASSBs) alongside NMC which is considered the next-generation cathode material. Unfortunately, Li metal faces tremendous challenges when brought into contact with many currently considered promising solid electrolytes (SEs). The associated challenges are electrical, electro-(chemical) and mechanical instabilities. Surprisingly, if one studies the literature thoroughly, it seems that batteries based on SEs show much faster dendrite formation than liquid electrolytes. For this particular study, thanks to in situ and operando SEM, we studied these sulfide-based SEs, viz. β-Li3PS4 (LPS) and Li6PS5Cl (LPSCl). We highlight the key differences in failure modes of two sulfide-based SEs, by keeping the anode (Li metal) and cathode (NMC111) constant. For both the SEs, initially, electro-chemo-mechanical stress is induced, due to volume expansion of active materials and plating during cycling. However, in the case of LPS, this leads to electrical failure causing a short circuit, whereas in the case of LPSCl it leads to further mechanical damage-causing delamination of the cathode. Thus, the porous structure of SEs heavily determines the mechanical behaviour of the ASSB, the distribution of the induced electro-chemo-mechanical stress and in turn, the mechanism of ASSB failure. The other striking observations are: (1) cracks travel ahead of the dendrites (2) cracks grow and propagate at a much faster rate in the case of β-LPS than in LPSCl (3) higher surface roughness of LPSCl gives rise to many different morphologies of Li deposition/dendrites (4) the cathode electrolyte interface (CEI) forms and grows at a much faster rate in the case of LPS than in LPSCl. We demonstrate that differences in cycling performance and mode of failure are due to the differences in SEs. We also highlight that the key limitation in implementing Li metal as an anode in ASSBs is the dendrite formation and mechanical instability. These findings again emphasize the importance of coating active materials, the introduction of a buffer layer between the SE/Li metal interface, coating of SE, or the need for using composite/hybrid or bilayer solid electrolytes at least.
Databáze: OpenAIRE