The influence of interfacial interactions on the conductivity and phase behaviour of organic ionic plastic crystal/polymer nanoparticle composite electrolytes

TY - JOUR

T1 - The influence of interfacial interactions on the conductivity and phase behaviour of organic ionic plastic crystal/polymer nanoparticle composite electrolytes

AU - Nti, Frederick

AU - Porcarelli, Luca

AU - Greene, George W.

AU - Zhu, Haijin

AU - Makhlooghiazad, Faezeh

AU - Mecerreyes, David

AU - Howlett, Patrick C.

AU - Forsyth, Maria

AU - Wang, Xiaoen

N1 - Publisher Copyright: This journal is © The Royal Society of Chemistry.

PY - 2020/3/14

Y1 - 2020/3/14

N2 - Organic ionic plastic crystals (OIPCs) have been recognised as promising solid-state electrolyte materials for next-generation energy storage devices. Recently, the addition of polymer nanofillers to OIPCs has led to the design of OIPC-based solid-state electrolytes with enhanced mechanical stability and ion conductivity. However, the mechanisms of ion conductivity enhancement and the influence of different polymer surface chemistries on the ion dynamics are not yet well understood, which has hindered the further development of high-performance OIPC-based electrolytes. In this work, we selected two different polymer nanoparticles, poly(vinylidene fluoride) (PVDF) and polystyrene (PS), and investigated the effects of the polymer surfaces on the thermal behaviour and ion transport properties of the OIPC, N-ethyl N-methyl pyrrolidinium bis(fluorosulfonyl)imide ([C2mpyr][FSI]). We found significantly different thermal behaviours, as well as ion transport properties in the OIPC/nanoparticle composites. Specifically, compared with pure [C2mpyr][FSI], the addition of PVDF nanoparticles effectively enhanced the ion conductivity of the OIPC composite, with the optimum achieved near the percolation threshold of PVDF nanoparticles. In contrast, the addition of PS nanoparticles to the OIPC led to a slight enhancement at low concentrations and then a significant decrease in conductivity at higher concentrations. DSC, FTIR and EIS confirm that the interaction between the PVDF nanoparticles and the OIPC induces the formation of less ordered OIPC layers on the PVDF surfaces, leading to the conductivity enhancement. Finally, different structure models based on the results of this work are proposed, which provide principle guidelines for the design of future OIPC-based highly conductive electrolyte materials.

AB - Organic ionic plastic crystals (OIPCs) have been recognised as promising solid-state electrolyte materials for next-generation energy storage devices. Recently, the addition of polymer nanofillers to OIPCs has led to the design of OIPC-based solid-state electrolytes with enhanced mechanical stability and ion conductivity. However, the mechanisms of ion conductivity enhancement and the influence of different polymer surface chemistries on the ion dynamics are not yet well understood, which has hindered the further development of high-performance OIPC-based electrolytes. In this work, we selected two different polymer nanoparticles, poly(vinylidene fluoride) (PVDF) and polystyrene (PS), and investigated the effects of the polymer surfaces on the thermal behaviour and ion transport properties of the OIPC, N-ethyl N-methyl pyrrolidinium bis(fluorosulfonyl)imide ([C2mpyr][FSI]). We found significantly different thermal behaviours, as well as ion transport properties in the OIPC/nanoparticle composites. Specifically, compared with pure [C2mpyr][FSI], the addition of PVDF nanoparticles effectively enhanced the ion conductivity of the OIPC composite, with the optimum achieved near the percolation threshold of PVDF nanoparticles. In contrast, the addition of PS nanoparticles to the OIPC led to a slight enhancement at low concentrations and then a significant decrease in conductivity at higher concentrations. DSC, FTIR and EIS confirm that the interaction between the PVDF nanoparticles and the OIPC induces the formation of less ordered OIPC layers on the PVDF surfaces, leading to the conductivity enhancement. Finally, different structure models based on the results of this work are proposed, which provide principle guidelines for the design of future OIPC-based highly conductive electrolyte materials.

UR - http://www.scopus.com/inward/record.url?scp=85081582679&partnerID=8YFLogxK

U2 - 10.1039/c9ta12827a

DO - 10.1039/c9ta12827a

M3 - 文章

AN - SCOPUS:85081582679

SN - 2050-7488

VL - 8

SP - 5350

EP - 5362

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 10

ER -