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DOE OSTI · 3010971

Improving Ionic Conformality Across Polymer Electrolyte|Electrode Interfaces

Min, Jungki [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)] (ORCID:0000000345726895)·Pietra, Nicholas F. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Connor, Callum [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)]·Liang, Zhaohui [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)]·Jackson, Erin C. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Tao, Lei [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Xia, Dawei [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Feng, Xu [Univ. of Delaware, Newark, DE (United States)]·Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405)·Bak, Seong‐Min [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Yonsei Univ., Seoul (Korea, Republic of)]·Moore, Robert B. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Madsen, Louis A. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)]·Lin, Feng [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)] (ORCID:0000000237293148)
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Abstract

Maintaining uniform ionic transport at electrode|electrolyte interfaces, i.e., ionic conformality, remains challenging in polymer electrolyte (PE)-based solid-state batteries. Morphological conformality does not necessarily imply ionic conformality. In PEs, which typically consist of a mechanically supporting component and distinct ionically conductive components, the rearrangement or depletion of mobile ion-conductive domains at interfaces can disrupt ionic transport pathways. Such localized ionic depletion contributes to interfacial instability and capacity degradation in high-voltage lithium-metal batteries. Herein, an electrolyte design approach aimed at minimizing interfacial heterogeneities is demonstrated through compositional adjustments, characterized by spatially resolved structural and chemical X-ray techniques and NMR diffusometry to elucidate ion transport dynamics. This approach improves ionic conformality at electrode interfaces, enhancing cycling stability in Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) coin and pouch cells cycled at high voltages. These results contribute to understanding interfacial behaviors in multiphase PEs and inform strategies for improving stability across solid-state battery interfaces.

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36 MATERIALS SCIENCEelectrolyte additiveinterfacemolecular ionic compositesolid-state lithium batteriessynchrotron X-ray analyses

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Min, Jungki [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)] (ORCID:0000000345726895), Pietra, Nicholas F. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Connor, Callum [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)], Liang, Zhaohui [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)], Jackson, Erin C. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Tao, Lei [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Xia, Dawei [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Feng, Xu [Univ. of Delaware, Newark, DE (United States)], Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405), Bak, Seong‐Min [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Yonsei Univ., Seoul (Korea, Republic of)], Moore, Robert B. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Madsen, Louis A. [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)], Lin, Feng [Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Brown Univ., Providence, RI (United States)] (ORCID:0000000237293148). 2025-12-21. Improving Ionic Conformality Across Polymer Electrolyte|Electrode Interfaces. https://doi.org/10.1002/adma.202515865

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36 MATERIALS SCIENCE subjectelectrolyte additive subjectinterface subjectmolecular ionic composite subject

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