Enhanced ion transport behaviors in composite polymer electrolyte: the case of a looser chain folding structure

Pei, Dexuan; Ma, Rui; Yang, Gang; Li, Yuhang; Huang, Can; Zi-ying, Liu; Huang, Shuo; Jin, Hongyun; Cao, Guozhong

doi:10.1039/d1ta10669d

Cited by 13 publications

(4 citation statements)

References 48 publications

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“…The lower ionic conductivity of CPEs with 500 nm particles after cyclic compression thus reveals a potential negative impact on the interfacial lithium-ion conduction pathways caused by mechanical cycling. Nuclear magnetic resonance (NMR) methods have shown that smaller particles (30 vs 200 nm) are associated with looser chain folding structure based on characteristic relaxation times of polycaprolactone (PCL) electrolytes with LiTFSI and Al 2 O 3 particles . Alteration of chain folding over many cycles of structural deformation can have an adverse effect on lithium-ion transport through the electrolyte in a way that is more pronounced for composites with smaller particles.…”

Section: Resultsmentioning

confidence: 99%

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Yoon,

Mulay,

Baltazar

et al. 2023

ACS Appl. Energy Mater.

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Composite polymer electrolytes (CPEs) strike an effective balance between ionic conductivity and mechanical flexibility for lithium-ion solid-state batteries. Long-term performance, however, is limited by capacity fading after hundreds of charge and discharge cycles. The causes of performance degradation include multiple contributing factors such as dendrite formation, physicochemical changes in electrolytes, and structural remodeling of porous electrodes. Among the many factors that contribute to performance degradation, the effect of stress specifically on the composite electrolyte is not well understood. This study examines the mechanical changes in a poly(ethylene oxide) electrolyte with bis(trifluoromethane) sulfonimide. Two different sizes of Li6.4La3Zr1.4Ta0.6O12 particles (500 nm and 5 μm) are compared to evaluate the effect of the surface-to-volume ratio of the ion-conducting fillers within the composite. Cyclic compression was applied to mimic stress cycling in the electrolyte, which would be caused by asymmetric volume changes that occur during charging and discharging cycles. The electrolytes exhibited fatigue softening, whereby the compressive modulus gradually decreased with an increase in the number of cycles. When the electrolyte was tested for 500 cycles at 30% compressive strain, the compressive modulus of the electrolyte was reduced to approximately 80% of the modulus before cycling. While the extent of softening was similar regardless of particle size, CPEs with 500 nm particles exhibited a significant reduction in ionic conductivity after cyclic compression (1.4 × 10–7 ± 2.3 × 10–8 vs 1.1 × 10–7 ± 2.0 × 10–8 S/cm, mean ± standard deviation, n = 4), whereas there was no significant change in ionic conductivity for CPEs with 5 μm particles. These observations performed deliberately in the absence of charge–discharge cycles show that repetitive mechanical stresses can play a significant role in altering the performance of CPEs, thereby revealing another possible mechanism for performance degradation in all-solid-state batteries.

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Section: Resultsmentioning

confidence: 99%

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Yoon,

Mulay,

Baltazar

et al. 2023

ACS Appl. Energy Mater.

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“…Generally, the presence of nanoparticles in each phase of the polymer blend can lead to a restriction effect on the molecular chain motions and thus a change in its dynamic transitions. [39][40][41] On the other hand, the dynamics of the chain can be evaluated by changes in the F I G U R E 3 (A) Storage modulus and (B) complex viscosity versus angular frequency and (C) Cole-Cole plot at 190 C for PP8/EC2 and nanocomposite samples prepared by different feeding methods containing 2 phr multiwalled carbon nanotubes damping factor (tan δ; peak area) and the glass transition temperature (T g ) in the DMTA curves. [24,42,43] In this regard, a reduction in the damping factor and also a shift of the T g to higher temperature reveal a slowing down of the molecular chain motions.…”

Section: Selective Localization Of Mwcnts Based On Kinetic Parametersmentioning

confidence: 99%

Effect of multi‐walled carbon nanotube localization on toughening mechanism and electrical properties of compatibilized PP/EOC immiscible blend

2022

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Toughness modification of polypropylene (PP), a widely used polymer in industry, is an important factor in overcoming mechanical limitations and extending its scope of application. In the present work, we utilized a combination of nanoparticle and elastomer techniques to enhance the toughness of PP. Accordingly, the nanocomposite blends, including PP, ethylene octene copolymer (EOC), and multi-walled carbon nanotubes (MWCNTs), were pre-

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“…However, the anionic dynamics generally supersedes the cationic dynamics, resulting in low t Li+ in PEO systems, since the anion mobility is less restricted by the polymer segmental motions . Being a semicrystalline polyester with a glass-transition temperature of −65 °C and a melting temperature around 55 °C, poly(ε-caprolactone) (PCL) was selected as a matrix candidate since it displays in fact notably similar physical properties as PEO. − Especially, the PCL exhibits a strong Li-ion solvating capability, which is expected to promote the Li-ion transport. Zhang et al reported a PCL-based CPE with a high degree of LiTFSI dissociation reaching up to 45 wt % .…”

Section: Introductionmentioning

confidence: 99%

Exploring High Li⁺ Transference Number Solid-State Electrolytes Based on a Poly(ε-caprolactone) Polymer Matrix with Efficient Lithium Salt Dissociation for Applications in Lithium-Metal Batteries

Wang

Pei

Liu

et al. 2023

ACS Appl. Energy Mater.

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Composite polymer electrolytes (CPEs) with high security and mechanical flexibility are needed for all-solid-state lithium-metal batteries (LMBs). However, their practical application is hindered by the increasing demand for high-power and high-areal-energy-density storage solutions. Herein, a high-powered CPE relying on poly(ε-caprolactone) (PCL) as the polymer matrix is developed. The binding energy of Li + -PCL is predicted to be −130.163 kcal•mol −1 via density functional theory calculations, which implies a high dissociation of Li salts in the PCL matrix. The weak interactions between the Li + and the polymer chains enable the CPEs with a high Li + transfer number (t Li+ ) of 0.71. Besides, LiFePO 4 //Li batteries deliver a high capacity retention of 85% for over 600 cycles at 2.0C. This work demonstrates the tremendous potential of PCL-based CPEs in promoting the application of high-power-performance LMBs.

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Enhanced ion transport behaviors in composite polymer electrolyte: the case of a looser chain folding structure

Abstract: All-solid-state batteries based on composite polymer electrolytes (CPEs) have drawn significant attention due to their high energy density, security and flexibility. Usually, the improvement of electrochemical performance of CPEs is...

Cited by 13 publications

References 48 publications

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Effect of multi‐walled carbon nanotube localization on toughening mechanism and electrical properties of compatibilized PP/EOC immiscible blend

Exploring High Li⁺ Transference Number Solid-State Electrolytes Based on a Poly(ε-caprolactone) Polymer Matrix with Efficient Lithium Salt Dissociation for Applications in Lithium-Metal Batteries

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Enhanced ion transport behaviors in composite polymer electrolyte: the case of a looser chain folding structure

Abstract: All-solid-state batteries based on composite polymer electrolytes (CPEs) have drawn significant attention due to their high energy density, security and flexibility. Usually, the improvement of electrochemical performance of CPEs is...

Cited by 13 publications

References 48 publications

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

Effect of multi‐walled carbon nanotube localization on toughening mechanism and electrical properties of compatibilized PP/EOC immiscible blend

Exploring High Li+ Transference Number Solid-State Electrolytes Based on a Poly(ε-caprolactone) Polymer Matrix with Efficient Lithium Salt Dissociation for Applications in Lithium-Metal Batteries

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Product

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Exploring High Li⁺ Transference Number Solid-State Electrolytes Based on a Poly(ε-caprolactone) Polymer Matrix with Efficient Lithium Salt Dissociation for Applications in Lithium-Metal Batteries