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Role of Scaffold Architecture and Excess Surface Polymer Layers in a 3D-Interconnected Ceramic/Polymer Composite Electrolyte

Journal Article · · Advanced Energy Materials
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  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
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3D-interconnected ceramic/polymer composite electrolytes offer promise to combine the benefits of both ceramic and polymer electrolytes. However, an in-depth understanding of the role of the ceramic scaffold's architecture, and the associated polymer/ceramic interfaces on the electrochemical properties of such composite electrolytes is still incomplete. Here, these factors are systematically evaluated using an interconnected composite electrolyte with a tunable and well-defined architecture. The ionic conductivity of the ceramic scaffold is strongly dependent on its porosity and tortuosity, as demonstrated experimentally and via theoretical modeling. The connectivity of the ceramic framework avoids the high interfacial impedance at the polymer/ceramic electrolyte interface within the composite. However, this work discovers that the interfacial impedance between the bulk composite and excess surface polymer layers of the composite membrane dominates the overall impedance, resulting in a 1–2 order drop of ionic conductivity compared to the ceramic scaffold. Despite the high impedance interfaces, an improved Li+ transference number is found compared to the neat polymer (0.29 vs 0.05), attributed to the ceramic phase's contributions toward ion transport. Further, this leads to flatter overpotentials in lithium symmetric cell cycling. These results are expected to guide future research directions toward scalable manufacturing of composite electrolytes with optimized architecture and interfaces.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1960700
Alternate ID(s):
OSTI ID: 1974286
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 19 Vol. 13; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
ceramic electrolytes
composite electrolytes
interconnected ceramics
lithium
polymer electrolytes
polymer/ceramic interfaces
solid-state batteries