Improved interfacial li-ion transport in composite polymer electrolytes via surface modification of LLZO

Counihan, Michael J.; Lee, Jungkuk; Mirmira, Priyadarshini; Barai, Pallab; Burns, Meghan E.; Amanchukwu, Chibueze V.; Srinivasan, Venkat; Zhang, Yuepeng; Tepavcevic, Sanja

doi:10.20517/energymater.2024.195

Improved interfacial li-ion transport in composite polymer electrolytes via surface modification of LLZO

Journal Article · Tue Jan 21 23:00:00 EST 2025 · Energy Materials

DOI:https://doi.org/10.20517/energymater.2024.195· OSTI ID:2574955

Counihan, Michael J. ^[1]; Lee, Jungkuk ^[1]; Mirmira, Priyadarshini ^[2]; Barai, Pallab ^[1]; Burns, Meghan E. ^[3]; Amanchukwu, Chibueze V. ^[2]; Srinivasan, Venkat ^[1]; Zhang, Yuepeng ^[1]; ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. of Chicago, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)

Composite polymer electrolytes that incorporate ceramic fillers in a polymer matrix offer mechanical strength and flexibility as solid electrolytes for lithium metal batteries. However, fast Li⁺ transport between polymer and Li⁺-conductive filler phases is not a simple achievement due to high barriers for Li⁺ exchange across the interphase. This study demonstrates how modification of Li₇La₃Zr₂O₁₂ (LLZO) nanofiller surfaces with silane chemistries influences Li⁺ transport at local and global electrolyte scales. Anhydrous reactions covalently link amine-functionalized silanes [(3-aminopropyl)triethoxysilane (APTES)] to LLZO nanoparticles, which protects LLZO in air. APTES functionalization lowers the poly (ethylene oxide) (PEO)-LLZO interphase resistance to half that of unmodified LLZO and increases effective Li⁺ transference number, while insulating Al₂O₃ completely blocks ion exchange and lowers transference number and conductivity in PEO-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-LLZO composites. Modeling an inner resistive interphase between LLZO and PEO surrounded by an outer conductive interphase explains non-linear conductivity trends. Solid-state ⁷Li & ⁶Li nuclear magnetic resonance shows Li⁺ only exchanges between PEO-LiTFSI and some LLZO interphase, with no appreciable Li⁺ transport through bulk LLZO. Surface functionalization is a promising path toward lowering the polymer-ceramic interphase resistance. This work demonstrates that local changes in Li⁺ transport affect macroscopic performance, highlighting the intricate relationships between all interfaces in inherently heterogeneous composite polymer electrolytes.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2574955

Journal Information:: Energy Materials, Journal Name: Energy Materials Journal Issue: 3 Vol. 5; ISSN 2770-5900

Publisher:: OAECopyright Statement

Country of Publication:: United States

Language:: English

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