Zhou, Zekun; Tao, Zengren; Zhang, Linyun; Zheng, Xueying; Xiao, Xieyi; Liu, Zhen; Li, Xin; Liu, Guangfeng; Zhao, Pengfei; Zhang, Peng

ACS APPLIED MATERIALS & INTERFACES

2022, , 1944-8244

Zhou, Zekun; Tao, Zengren; Zhang, Linyun; Zheng, Xueying; Xiao, Xieyi; Liu, Zhen; Li, Xin; Liu, Guangfeng; Zhao, Pengfei; Zhang, Peng

A scalable manufacturing protocol is developed to prepare polymer-based solvent-free all-solid flexible energy storage devices based on a two-roll mill and adapted rubber mixing technology. The as-prepared solid polymer electrolytes (SPEs) consisting of commercial poly(methyl methacrylate)-grafted natural rubber (MG30) and lithium bis(trifluoromethanesulfonyl)imide achieve a superior ionic conductivity of 2.7 x 10-3 S cm(-1) at 30 ?. The superior ionic conductivity is attributed to the formation of an ionic cluster network in the composite as proved by small-angle X-ray scattering and infrared spectroscopy measurements. Moreover, the as-prepared SPEs show good mechanical stability over a broad temperature range, that is , a storage modulus above 1 x 104 Pa from 30 to 120 ? as indicated by the rheology data. Furthermore, the SPEs were assembled with the carbon black-filled MG30 (i.e., MG30C) electrode into a flexible supercapacitor cell, which had a wide voltage window of 3.5 V, good energy density of 28.4 mu W hmiddotcm-2 at 160 ? and good temperature tolerance up to 160 ?. This scaling-up manufacture strategy shows tremendous potential to the advancing of SPEs in applications of flexible energy storage device.