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Title: Elucidating Polymer Binder Entanglement in Freestanding Sulfide Solid-State Electrolyte Membranes

Journal Article · · ACS Energy Letters
 [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [3]; ORCiD logo [4];  [4]; ORCiD logo [5];  [4]; ORCiD logo [2]
  1. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Florida A & M University, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (United States)
  2. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  3. Freed-Hardeman Univ., Henderson, TN (United States)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  5. Florida A & M University, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (United States)

This study advances the development of flexible, sheet-type sulfide solid-state electrolytes (SSEs) for use in all-solid-state batteries, emphasizing the important and previously insufficiently investigated role of polymer binder entanglement. Here, the molecular weight of polymer binders is pivotal in crafting robust, freestanding SSE films. Our research uncovers a dual impact: higher molecular weight binders bolster the structural integrity of SSE films but elevate grain boundary resistance and diminish critical current density, whereas lower molecular weight poly(isobutylene) films, despite their more uniform distribution, lack the essential strain hardening or strength for sustained active material contact. Crucially, full cells employing higher molecular weight binders demonstrate improved discharge capacity retention, contrasting sharply with the notable capacity degradation in lower molecular weight cells. Our findings not only deepen the comprehension of binder influences in solid-state batteries but also chart a course for refining all-solid-state battery technologies, a key stride for the future of energy storage solutions.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2376351
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 6 Vol. 9; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (24)

Physio‐Electrochemically Durable Dry‐Processed Solid‐State Electrolyte Films for All‐Solid‐State Batteries journal April 2023
Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries journal February 2018
Slurry‐Fabricable Li + ‐Conductive Polymeric Binders for Practical All‐Solid‐State Lithium‐Ion Batteries Enabled by Solvate Ionic Liquids journal February 2019
Identifying the Origins of Microstructural Defects Such as Cracking within Ni‐Rich NMC811 Cathode Particles for Lithium‐Ion Batteries journal November 2020
Impact of Solvent Treatment of the Superionic Argyrodite Li 6 PS 5 Cl on Solid‐State Battery Performance journal January 2021
Improving the cycling performance of LiNi0.8Co0.1Mn0.1O2 by surface coating with Li2TiO3 journal September 2016
Toward practical all-solid-state lithium-ion batteries with high energy density and safety: Comparative study for electrodes fabricated by dry- and slurry-mixing processes journal January 2018
Liquid-involved synthesis and processing of sulfide-based solid electrolytes, electrodes, and all-solid-state batteries journal December 2019
Design-of-experiments-guided optimization of slurry-cast cathodes for solid-state batteries journal June 2021
High Ionic Conductivity of Liquid-Phase-Synthesized Li 3 PS 4 Solid Electrolyte, Comparable to That Obtained via Ball Milling journal February 2021
Thin and Flexible Solid Electrolyte Membranes with Ultrahigh Thermal Stability Derived from Solution-Processable Li Argyrodites for All-Solid-State Li-Ion Batteries journal February 2020
Fabrication of High-Quality Thin Solid-State Electrolyte Films Assisted by Machine Learning journal April 2021
Solvent-Free Approach for Interweaving Freestanding and Ultrathin Inorganic Solid Electrolyte Membranes journal December 2021
Intrinsic Origins of Crack Generation in Ni-rich LiNi0.8Co0.1Mn0.1O2 Layered Oxide Cathode Material journal January 2017
Chemical stability of sulfide solid-state electrolytes: stability toward humid air and compatibility with solvents and binders journal January 2022
Degradation of high-voltage cathodes for advanced lithium-ion batteries – differential capacity study on differently balanced cells journal December 2018
Determining phase transitions of layered oxides via electrochemical and crystallographic analysis journal January 2020
Polymer Physics book June 2003
Adverse Effects of Trace Non-polar Binder on Ion Transport in Free-standing Sulfide Solid Electrolyte Separators journal August 2023
Slurry-Based Processing of Solid Electrolytes: A Comparative Binder Study journal January 2018
Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries journal January 2017
Introduction to Polymers book June 2011
Navigating the complexities of solvent and binder selection for solution processing of sulfide solid-state electrolytes journal August 2023
Polymer/Solvent Interaction Parameters journal March 1966