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Title: Making Plasticized Polymer Electrolytes Stable Against Sodium Metal for High‐Energy Solid‐State Sodium Batteries

Journal Article · · Angewandte Chemie (International Edition)

Abstract Solid polymer electrolytes based on plastic crystals are promising for solid‐state sodium metal (Na 0 ) batteries, yet their practicality has been hindered by the notorious Na 0 ‐electrolyte interface instability issue, the underlying cause of which remains poorly understood. Here, by leveraging a model plasticized polymer electrolyte based on conventional succinonitrile plastic crystals, we uncover its failure origin in Na 0 batteries is associated with the formation of a thick and non‐uniform solid electrolyte interphase (SEI) and whiskery Na 0 nucleation/growth. Furthermore, we design a new additive‐embedded plasticized polymer electrolyte to manipulate the Na 0 deposition and SEI formulation. For the first time, we demonstrate that introducing fluoroethylene carbonate (FEC) additive into the succinonitrile‐plasticized polymer electrolyte can effectively protect Na 0 against interfacial corrosion by facilitating the growth of dome‐like Na 0 with thin, amorphous, and fluorine‐rich SEIs, thus enabling significantly improved performances of Na//Na symmetric cells (1,800 h at 0.5 mA cm −2 ) and Na//Na 3 V 2 (PO 4 ) 3 full cells (93.0 % capacity retention after 1,200 cycles at 1 C rate in coin cells and 93.1 % capacity retention after 250 cycles at C/3 in pouch cells at room temperature). Our work provides valuable insights into the interfacial failure of plasticized polymer electrolytes and offers a promising solution to resolving the interfacial instability issue.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0021204
OSTI ID:
2318762
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 14 Vol. 63; ISSN 1433-7851
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

References (33)

Elastomeric electrolytes for high-energy solid-state lithium batteries journal January 2022
An asymmetric bilayer polymer-ceramic solid electrolyte for high-performance sodium metal batteries journal November 2022
Combining theories and experiments to understand the sodium nucleation behavior towards safe sodium metal batteries journal January 2020
Mesoporous Single‐Crystal Lithium Titanate Enabling Fast‐Charging Li‐Ion Batteries journal March 2022
Stable Metal Anode enabled by Porous Lithium Foam with Superior Ion Accessibility journal June 2018
All-solid-state sodium batteries enabled by flexible composite electrolytes and plastic-crystal interphase journal March 2020
In-situ construction of multifunctional interlayer enabled dendrite-free garnet-based solid-state batteries journal June 2023
A New Class of Ionically Conducting Fluorinated Ether Electrolytes with High Electrochemical Stability journal April 2020
The plastic-crystalline phase of succinonitrile as a universal matrix for solid-state ionic conductors journal June 2004
Molecular Engineering of Highly Fluorinated Carbon Dots: Tailoring Li+ Dynamics and Interfacial Fluorination for Stable Solid Lithium Batteries journal November 2023
A Plastic-Crystal Electrolyte Interphase for All-Solid-State Sodium Batteries journal April 2017
A cost and resource analysis of sodium-ion batteries journal March 2018
Polymer electrolytes for sodium-ion batteries journal April 2021
In-Situ Polymerized Solid-State Polymer Electrolytes for High-Safety Sodium Metal Batteries: Progress and Perspectives journal October 2023
Probing the Na metal solid electrolyte interphase via cryo-transmission electron microscopy journal May 2021
Quasi-Solid-State Dual-Ion Sodium Metal Batteries for Low-Cost Energy Storage journal April 2020
The influence of FEC on the solvation structure and reduction reaction of LiPF6/EC electrolytes and its implication for solid electrolyte interphase formation journal October 2019
Opportunities for moderate-range electric vehicles using sustainable sodium-ion batteries journal March 2023
NASICON-Structured LiZr2(PO4)3 Surface Modification Improves Ionic Conductivity and Structural Stability of LiCoO2 for a Stable 4.6 V Cathode journal April 2022
Progress in nitrile-based polymer electrolytes for high performance lithium batteries journal January 2016
Transition from Vogel-Fulcher-Tammann to Arrhenius Ion-Conducting Behavior in Poly(Ethyl Acrylate)-Based Solid Polymer Electrolytes via Succinonitrile Plasticizer Addition journal September 2023
Atomic structure of sensitive battery materials and interfaces revealed by cryo–electron microscopy journal October 2017
Anion‐tethered Single Lithium‐ion Conducting Polyelectrolytes through UV‐induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes journal August 2023
Role of succinonitrile in improving ionic conductivity of sodium-ion conductive polymer electrolyte conference January 2018
Nonflammable Nitrile Deep Eutectic Electrolyte Enables High-Voltage Lithium Metal Batteries journal February 2020
Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries journal January 2023
Fundamentals, status and promise of sodium-based batteries journal June 2021
A compatible anode/succinonitrile-based electrolyte interface in all-solid-state Na–CO 2 batteries journal January 2019
Characterization of the structure and chemistry of the solid–electrolyte interface by cryo-EM leads to high-performance solid-state Li-metal batteries journal June 2022
Sodium Metal Anodes: Emerging Solutions to Dendrite Growth journal April 2019
Recent Progress in the Emerging Modification Strategies for Layered Oxide Cathodes toward Practicable Sodium Ion Batteries (Adv. Energy Mater. 27/2023) journal July 2023
A rational configuration for ultralong lifespan all-solid-state organic sodium-metal batteries journal January 2022
Leveraging cryogenic electron microscopy for advancing battery design journal January 2022