<p>Despite their favorable interfacial contact and high ionic conductivity, gel polymer electrolytes&#xa0;(GPEs) remain constrained by insufficient electrochemical and thermal/mechanical stability as well as low lithium-ion transference numbers, restricting their long-term application in lithium metal batteries (LMBs). In this study, a poly(ethylene glycol) diacrylate (PEGDA)-based nanocomposite gel polymer electrolyte (NGPE-BN-x) was developed by thermal in situ polymerization, incorporating a few-layer hydroxylated hexagonal boron nitride nanosheets (h-BNNS-OH) as a two-dimensional (2D) nanofiller. The influence of h-BNNS-OH loading (1, 3, and 5 wt%) on lithium ion transference number (<i>t</i><sub><i>Li</i></sub><sup><i>+</i></sup>), ionic conductivity, electrochemical, thermal and mechanical stability was systematically evaluated relative to the pristine GPE. The optimized NGPE-BN-3 exhibited high ionic conductivity (σ = 8.85 mS cm<sup>− 1</sup>), an expanded electrochemical stability window (ESW) of 5.01&#xa0;V, an enhanced <i>t</i><sub><i>Li</i></sub><sup><i>+</i></sup> of 0.66, and improved mechanical strength (0.64&#xa0;MPa) at room temperature. LFP//Li full cells utilizing NGPE-BN-3 yielded a discharge capacity of 162.2 mAh g<sup>− 1</sup> at 0.1&#xa0;C with good rate capability (0.1-2.0&#xa0;C), and prolonged cycling stability at 1&#xa0;C under ambient conditions. The improved electrochemical performance highlights the effectiveness of h-BNNS-OH as a multifunctional additive for PEGDA-based GPEs toward high-performance LMBs.</p> Graphical Abstract <p>This work presents an in situ polymerized PEGDA-based nanocomposite gel polymer electrolyte incorporating a few-layer hydroxylated h-BN nanosheets. The highly dispersed 2D filler regulates anion mobility through Lewis acid-base interactions, enhancing Li⁺ transport, electrochemical stability (5.01&#xa0;V), and thermal stability. The optimized NGPE-BN-3 achieves 8.85 mS cm<sup>− 1</sup> conductivity and <i>t</i><sub><i>Li</i></sub><i>⁺</i> = 0.66, enabling stable LFP//Li cell performance with improved interfacial integrity after cycling.</p>

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PEGDA-based nanocomposite gel polymer electrolytes with hydroxylated h-BN nanosheets enabling fast ion transport and high-voltage stability for lithium metal batteries

  • Gulsah Yaman Uzunoglu

摘要

Despite their favorable interfacial contact and high ionic conductivity, gel polymer electrolytes (GPEs) remain constrained by insufficient electrochemical and thermal/mechanical stability as well as low lithium-ion transference numbers, restricting their long-term application in lithium metal batteries (LMBs). In this study, a poly(ethylene glycol) diacrylate (PEGDA)-based nanocomposite gel polymer electrolyte (NGPE-BN-x) was developed by thermal in situ polymerization, incorporating a few-layer hydroxylated hexagonal boron nitride nanosheets (h-BNNS-OH) as a two-dimensional (2D) nanofiller. The influence of h-BNNS-OH loading (1, 3, and 5 wt%) on lithium ion transference number (tLi+), ionic conductivity, electrochemical, thermal and mechanical stability was systematically evaluated relative to the pristine GPE. The optimized NGPE-BN-3 exhibited high ionic conductivity (σ = 8.85 mS cm− 1), an expanded electrochemical stability window (ESW) of 5.01 V, an enhanced tLi+ of 0.66, and improved mechanical strength (0.64 MPa) at room temperature. LFP//Li full cells utilizing NGPE-BN-3 yielded a discharge capacity of 162.2 mAh g− 1 at 0.1 C with good rate capability (0.1-2.0 C), and prolonged cycling stability at 1 C under ambient conditions. The improved electrochemical performance highlights the effectiveness of h-BNNS-OH as a multifunctional additive for PEGDA-based GPEs toward high-performance LMBs.

Graphical Abstract

This work presents an in situ polymerized PEGDA-based nanocomposite gel polymer electrolyte incorporating a few-layer hydroxylated h-BN nanosheets. The highly dispersed 2D filler regulates anion mobility through Lewis acid-base interactions, enhancing Li⁺ transport, electrochemical stability (5.01 V), and thermal stability. The optimized NGPE-BN-3 achieves 8.85 mS cm− 1 conductivity and tLi = 0.66, enabling stable LFP//Li cell performance with improved interfacial integrity after cycling.