Highly disordered amorphous Li-battery electrolytes
Yuntong Zhu (Massachusetts Institute of Technology)
Zachary D. Hood (Massachusetts Institute of Technology)
Haemin Paik (Massachusetts Institute of Technology)
Pedro B. Groszewicz (TU Delft - Applied Sciences, University of Cambridge)
Steffen P. Emge (University of Cambridge)
Farheen N. Sayed (University of Cambridge)
Chengjun Sun (Argonne National Laboratory)
Moran Balaish (Massachusetts Institute of Technology, Technische Universität München)
David Ehre (Weizmann Institute of Science)
Jennifer L.M. Rupp (Massachusetts Institute of Technology, Weizmann Institute of Science, Technische Universität München)
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Abstract
“Medium-entropy” highly disordered amorphous Li garnets, with ≥4 unique local bonding units (LBUs), hold promise for use as solid-state electrolytes in hybrid or all-solid-state batteries owing to their grain-boundary-free nature and low-temperature synthesis requirement. Through this work, we resolved the local structure of amorphous Li garnet and understood their implication for Li dynamics. These medium-entropy amorphous structures possess unique characteristics with edge- and face-sharing LBUs, not conforming to the classic Zachariasen glass formation rules, and can be synthesized in a wide but processing-friendly temperature range (<680°C). Within these amorphous structures, Li and Zr are identified as the network formers and La as network modifier, with maxima in Li dynamics observed for smaller Li–O and Zr–O coordination; this structure understanding serves as a baseline for identifying additional network formers to further modulate Li transport. Our insight provides fundamental guidelines for the structure and phase design for amorphous Li garnets and paves the way for their integration in next-generation batteries.