Please use this identifier to cite or link to this item: http://dr.iiserpune.ac.in:8080/xmlui/handle/123456789/7703
Title: A soft co-crystalline solid electrolyte for lithium-ion batteries
Authors: PRAKASH, PRABHAT
Fall, Birane
Aguirre, Jordan
Sonnenberg, Laura A.
Chinnam, Parameswara Rao
Chereddy, Sumanth
Dikin, Dmitriy A.
VENKATNATHAN, ARUN
Wunder, Stephanie L.
Zdilla, Michael J.
Dept. of Chemistry
Keywords: Atomistic models
Batteries
2023-APR-WEEK1
TOC-APR-2023
2023
Issue Date: May-2023
Publisher: Springer Nature
Citation: Nature Materials, 22, 627–635.
Abstract: Alternative solid electrolytes are the next key step in advancing lithium batteries with better thermal and chemical stability. A soft solid electrolyte, (Adpn)2LiPF6 (Adpn, adiponitrile), is synthesized and characterized that exhibits high thermal and electrochemical stability and good ionic conductivity, overcoming several limitations of conventional organic and ceramic materials. The surface of the electrolyte possesses a liquid nano-layer of Adpn that links grains for a facile ionic conduction without high pressure/temperature treatments. Further, the material can quickly self-heal if fractured and provides liquid-like conduction paths via the grain boundaries. A substantially high ion conductivity (~10−4 S cm–1) and lithium-ion transference number (0.54) are obtained due to weak interactions between ‘hard’ (charge dense) Li+ ions and the ‘soft’ (electronically polarizable) –C≡N group of Adpn. Molecular simulations predict that Li+ ions migrate at the co-crystal grain boundaries with a (preferentially) lower activation energy Ea and within the interstitial regions between the co-crystals with higher Ea values, where the bulk conductivity is a smaller but extant contribution. These co-crystals establish a special concept of crystal design to increase the thermal stability of LiPF6 by separating ions in the Adpn solvent matrix, and also exhibit a unique mechanism of ion conduction via low-resistance grain boundaries, which contrasts with ceramics or gel electrolytes.
URI: https://doi.org/10.1038/s41563-023-01508-1
http://dr.iiserpune.ac.in:8080/xmlui/handle/123456789/7703
ISSN: 1476-4660
1476-1122
Appears in Collections:JOURNAL ARTICLES

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