Three-Dimensional Monolithic Organic Battery Electrodes.

Ryu, Jaegeon; Park, Byeongho; Kang, Jieun; Hong, Dongki; Kim, Sung-Dae; Yoo, Jung-Keun; Yi, Jin Woo; Park, Soojin et al. · ACS Nano · 2019

basic_science · Level V

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Abstract

Design of freestanding electrodes incorporated with redox-active organic materials has been limited by the poor intrinsic electrical conductivity and lack of methodology driving the feasible integration of conductive substrate and the organic molecules. Single-walled carbon nanotube (SWCNT) aerogels, which possess continuous network structure and high surface area, offer a three-dimensional electrically conducting scaffold. Here, we fabricate monolithic organic electrodes by coating a nanometer-scale imide-based network (IBN) that possesses abundant redox-active sites on the 3D SWCNT scaffold. The substantially integrated 3D monolithic organic electrodes sustain high electrical conductance through a 3D electronic pathway in their compressed form (∼21 μm). A thin and controllable layer (<8 nm) of IBN organic materials has a strong adhesion onto the ultra-lightweight and conductive substrate and facilitates multielectron redox reactions to deliver a specific capacity of up to 1550 mA h g<sup>-1</sup> (corresponding to the areal capacity of ∼2.8 mA h cm<sup>-2</sup>). The redox-active IBN in synergy with the 3D SWCNT scaffold can enable superior electrochemical performances compared to the previously reported organic-based electrode architectures and inorganic-based electrodes.