The origin of chemical inhomogeneity in garnet electrolytes and its impact on the electrochemical performance. Issue 28 (13th July 2020)

• Record Type: Journal Article
• Authors: Brugge, Rowena H.; Pesci, Federico M.; Cavallaro, Andrea; Sole, Christopher; Isaacs, Mark A.; Kerherve, Gwilherm; Weatherup, Robert S.; Aguadero, Ainara
• Is Part Of: Journal of materials chemistry. Volume 8:Issue 28(2020)
• Page Start: 14265
• Page End: 14276
• Publication Date: 2020-07-13
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d0ta04974c
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : The intrinsically defective nature of garnet-type electrolytes is revealed, probing the chemistry of the surface, grains and grain boundaries. Abstract : The interface between solid electrolytes and lithium metal electrodes determines the performance of an all-solid-state battery in terms of the ability to demand high power densities and prevent the formation of lithium dendrites. This interface depends strongly on the nature of the solid electrolyte surface in contact with the metallic anode. In the garnet electrolyte/Li system, most papers have focused on the role of current inhomogeneities induced by void formation in the Li metal electrode and the presence of insulating reaction layers following air exposure. However, extended defects in the solid electrolyte induced by chemical and/or structural inhomogeneities can also lead to uneven current distribution, impacting the performance of these systems. In this work, we use complementary surface analysis techniques with varying analysis depths to probe chemical distribution within grains and grain boundaries at the surface and in the bulk of garnet-type electrolytes to explain their electrochemical performance. We show that morphology, post-treatments and storage conditions can greatly affect the surface chemical distribution of grains and grain boundaries. These properties are important to understand since they will dictate the ionic and electronic transport near the interfacial zone between metal and electrolyte which is key to determining chemo-mechanical stability.