Pressure effects on electrochemical and crack driving forces in aluminium-doped LLZO-based all-solid-state lithium metal batteries

• Published in: Journal of power sources 2024-09, Vol.613, p.234873, Article 234873
• Main Authors: Adjah, John, Orisekeh, Kingsley I., Vandadi, Mobin, Ahmed, Ridwan A., Asare, Joseph, Agyei-Tuffour, Benjamin, Dodoo-Arhin, David, Nyankson, Emmanuel, Rahbar, Nima, Soboyejo, Winston O.
• Format: Article
• Language: English
• Subjects: All-solid-state lithium batteries (ASSLBs); And stresses; Battery degradation; Electrochemical performance; Induced strains; Stacking pressure; Yielding and cracking
• ISSN: 0378-7753
• DOI: 10.1016/j.jpowsour.2024.234873

This study employed a combination of computational models and experimental techniques to investigate the effects of stacking pressure on the mechanical deformation and electrochemical performance of All-Solid-State Li metal batteries (ASSLBs). The effects of the stacking pressure were studied in Al-doped LLZO-based electrolytes at the electrode/electrolyte interface and within the electrodes. Optical microscopy and digital imaging correlation (DIC) techniques were used to study the strain distributions induced in the Al-LLZO-based electrolyte at different stack pressures. The results show that minimal levels of stack pressure result in low strains within the electrolyte, whereas intermediate increasing pressures increase the interfacial contacts and electrochemical performance of the cells. However, higher stacking pressures result in higher induced levels of local stresses and strains, which are sufficient to cause cracking and degradation of the electrochemical performance. The implications of the results are discussed for the pressure-assisted manufacturing of all-solid-state lithium metal batteries. •Pressure applied improves electrode/electrolyte interfacial contacts.•Numerical simulation of pressure-induced interfacial contact and deformation.•SEM images show crack patterns at different stack pressures.•Moderate stack pressures improve electrochemical characteristics without cracking.•High stack pressures induced significant axial/shear strains and cracking in the electrolyte.