Cryogenic electron microscopy reveals that applied pressure promotes short circuits in Li batteries

Katharine L Harrison; Laura C Merrill; Daniel Martin Long; Steven J Randolph; Subrahmanyam Goriparti; Joseph Christian; Benjamin Warren; Scott A Roberts; Stephen J Harris; Daniel L Perry; Katherine L Jungjohann

doi:10.1016/j.isci.2021.103394

Cryogenic electron microscopy reveals that applied pressure promotes short circuits in Li batteries

iScience. 2021 Nov 1;24(12):103394. doi: 10.1016/j.isci.2021.103394. eCollection 2021 Dec 17.

Affiliations

¹ Nanoscale Sciences, Sandia National Laboratories, Albuquerque, NM 87123, USA.
² Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque, NM 87123, USA.
³ Materials & Structural Analysis Division, Thermo Fisher Scientific, Hillsboro, OR 97124, USA.
⁴ Thermal/Fluid Component Science, Sandia National Laboratories, Albuquerque, NM 87123, USA.
⁵ Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
⁶ Materials Characterization and Performance, Sandia National Laboratories, Albuquerque, NM 87123, USA.

Abstract

Li metal anodes are enticing for batteries due to high theoretical charge storage capacity, but commercialization is plagued by dendritic Li growth and short circuits when cycled at high currents. Applied pressure has been suggested to improve morphology, and therefore performance. We hypothesized that increasing pressure would suppress dendritic growth at high currents. To test this hypothesis, here, we extensively use cryogenic scanning electron microscopy to show that varying the applied pressure from 0.01 to 1 MPa has little impact on Li morphology after one deposition. We show that pressure improves Li density and preserves Li inventory after 50 cycles. However, contrary to our hypothesis, pressure exacerbates dendritic growth through the separator, promoting short circuits. Therefore, we suspect Li inventory is better preserved in cells cycled at high pressure only because the shorts carry a larger portion of the current, with less being carried by electrochemical reactions that slowly consume Li inventory.

Keywords: Electrochemical energy storage; Energy materials; Materials characterization; Materials characterization techniques; Materials chemistry; Materials science.