Atomic-scale origin of the low grain-boundary resistance in perovskite solid electrolyte Li0.375Sr0.4375Ta0.75Zr0.25O3

Tom Lee, Ji Qi, Chaitanya A. Gadre, Huaixun Huyan, Shu-Ting Ko, Yunxing Zuo, Chaojie Du, Jie Li, Toshihiro Aoki, Ruqian Wu (), Jian Luo (), Shyue Ping Ong () and Xiaoqing Pan ()
Additional contact information
Tom Lee: University of California at Irvine
Ji Qi: University of California San Diego
Chaitanya A. Gadre: University of California at Irvine
Huaixun Huyan: University of California at Irvine
Shu-Ting Ko: University of California San Diego
Yunxing Zuo: University of California San Diego
Chaojie Du: University of California at Irvine
Jie Li: University of California at Irvine
Toshihiro Aoki: University of California at Irvine
Ruqian Wu: University of California at Irvine
Jian Luo: University of California San Diego
Shyue Ping Ong: University of California San Diego
Xiaoqing Pan: University of California at Irvine

Nature Communications, 2023, vol. 14, issue 1, 1-14

Abstract: Abstract Oxide solid electrolytes (OSEs) have the potential to achieve improved safety and energy density for lithium-ion batteries, but their high grain-boundary (GB) resistance generally is a bottleneck. In the well-studied perovskite oxide solid electrolyte, Li3xLa2/3-xTiO3 (LLTO), the ionic conductivity of grain boundaries is about three orders of magnitude lower than that of the bulk. In contrast, the related Li0.375Sr0.4375Ta0.75Zr0.25O3 (LSTZ0.75) perovskite exhibits low grain boundary resistance for reasons yet unknown. Here, we use aberration-corrected scanning transmission electron microscopy and spectroscopy, along with an active learning moment tensor potential, to reveal the atomic scale structure and composition of LSTZ0.75 grain boundaries. Vibrational electron energy loss spectroscopy is applied for the first time to reveal atomically resolved vibrations at grain boundaries of LSTZ0.75 and to characterize the otherwise unmeasurable Li distribution therein. We find that Li depletion, which is a major reason for the low grain boundary ionic conductivity of LLTO, is absent for the grain boundaries of LSTZ0.75. Instead, the low grain boundary resistivity of LSTZ0.75 is attributed to the formation of a nanoscale defective cubic perovskite interfacial structure that contained abundant vacancies. Our study provides new insights into the atomic scale mechanisms of low grain boundary resistivity.

Date: 2023
References: View references in EconPapers View complete reference list from CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-023-37115-6 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37115-6

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-023-37115-6

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().