Issue 3, 2024

Inherent limitations of the hydrogen-bonding UPy motif as self-healing functionality for polymer electrolytes

Abstract

The development of advanced materials displaying reversible functionalities, such as self-healing is particularly desirable for energy storage devices, since the cycle life of many rechargeable batteries is limited due to the irreversible mechanical damages over the cycling processes. Hydrogen-bonding self-healing polymers functionalized with ureido pyrimidinone (UPy) has received great interest for energy storage applications, particularly for polymer electrolytes. Herein, we design a star-branched poly(ε-caprolactone-co-trimethylene carbonate) end-capped with UPy groups for both reinforced mechanical and desired self-healing properties in the polymer electrolytes. Despite the versatile implementation and strong bonding association, the benefits of hydrogen-bonding UPy functionalities are diminished after the dissolution of LiTFSI salt in the self-healing polymer matrix. Experimental analysis and molecular dynamics simulations were performed to gain insight into the dynamics of the self-healing polymer electrolyte system. FTIR shows a dramatic decrease in the intensities of the hydrogen-bonded C[double bond, length as m-dash]O signals belonging to UPy motifs after adding LiTFSI salt, indicative of a significant reduction in the total number of hydrogen-bonding and more loosened cross-linked polymer network. This is also noticed as a simultaneous deterioration of the mechanical properties. Molecular dynamics simulations reveal that the complex interplay of C[double bond, length as m-dash]O--Li+ coordination bonds and hydrogen bonding between TFSI anions and UPy motifs are responsible for the mechanical deterioration of the self-healing polymer electrolytes.

Graphical abstract: Inherent limitations of the hydrogen-bonding UPy motif as self-healing functionality for polymer electrolytes

Supplementary files

Article information

Article type
Paper
Submitted
18 jan 2024
Accepted
14 mar 2024
First published
22 mar 2024
This article is Open Access
Creative Commons BY license

RSC Appl. Polym., 2024,2, 374-383

Inherent limitations of the hydrogen-bonding UPy motif as self-healing functionality for polymer electrolytes

C. Thu Mai, H. Gudla, G. Hernández, K. Edström and J. Mindemark, RSC Appl. Polym., 2024, 2, 374 DOI: 10.1039/D4LP00017J

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