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PreprintCC BY-NCChemRxiv

Understanding and quantifying interfacial ion exchange in hybrid electrolytes

  • Deyang Yu1,2,3,4
  • Bryan D. McCloskey3,4,5,6
  • Rui Qiao7,2
  • Louis A. Madsen1,2
7 affiliations
  1. 1Department of Chemistry and Macromolecules Innovation Institute
  2. 2Virginia Polytechnic Institute and State University
  3. 3Energy Storage and Distributed Resources Division
  4. 4Lawrence Berkeley National Laboratory
  5. 5Department of Chemical & Biomolecular Engineering
  6. 6University of California, Berkeley
  7. 7Department of Mechanical Engineering
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Abstract

In pursuit of practical solid-state lithium batteries with low cost and scalable manufacturing, hybrid electrolytes that combine Li + -conducting inorganic electrolyte particles with liquid or polymer electrolytes have emerged as a promising strategy. 1-2 In these systems, Li + needs to transport through the interface between the percolating organic electrolyte matrix and the dispersed inorganic particles. However, interfacial Li + transport dynamics remain poorly understood largely due to lack of reliable experimental measurements. 3-4 Here, we introduce two straightforward nuclear magnetic resonance techniques − spin saturation transfer and selective inversion-recovery − to directly and unambiguously quantify Li + exchange in hybrid electrolytes. This enables us to build a new theoretical framework based on the exchange kinetics to analyze Li + transport in organic-inorganic hybrid electrolytes. By studying several representative hybrid electrolytes, we demonstrate that the ratio of inorganic particle radius and ionic Kapitza length predicts whether the incorporation of Li + -conducting particles into organic electrolytes will lead to hybrid electrolytes with improved conductivity. This study thus provides quantitative measurements and physical scaling principles to systematically design hybrid electrolytes for solid-state batteries.

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Cite

BibTeXRIS
BibTeX
@misc{yu2026understanding,
  title = {{Understanding and quantifying interfacial ion exchange in hybrid electrolytes}},
  author = {Deyang Yu and Bryan D. McCloskey and Rui Qiao and Louis A. Madsen},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008832/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008832/v1},
  note = {CC BY-NC},
}
RIS
TY  - UNPB
TI  - Understanding and quantifying interfacial ion exchange in hybrid electrolytes
AU  - Deyang Yu
AU  - Bryan D. McCloskey
AU  - Rui Qiao
AU  - Louis A. Madsen
PY  - 2026
DA  - 2026/09/15
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008832/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008832/v1
AB  - In pursuit of practical solid-state lithium batteries with low cost and scalable manufacturing, hybrid electrolytes that combine Li + -conducting inorganic electrolyte particles with liquid or polymer electrolytes have emerged as a promising strategy. 1-2 In these systems, Li + needs to transport through the interface between the percolating organic electrolyte matrix and the dispersed inorganic particles. However, interfacial Li + transport dynamics remain poorly understood largely due to lack of reliable experimental measurements. 3-4 Here, we introduce two straightforward nuclear magnetic resonance techniques − spin saturation transfer and selective inversion-recovery − to directly and unambiguously quantify Li + exchange in hybrid electrolytes. This enables us to build a new theoretical framework based on the exchange kinetics to analyze Li + transport in organic-inorganic hybrid electrolytes. By studying several representative hybrid electrolytes, we demonstrate that the ratio of inorganic particle radius and ionic Kapitza length predicts whether the incorporation of Li + -conducting particles into organic electrolytes will lead to hybrid electrolytes with improved conductivity. This study thus provides quantitative measurements and physical scaling principles to systematically design hybrid electrolytes for solid-state batteries.
ER  -