Three-Dimensional Monolithic Organic Battery Electrodes

• Published in: ACS nano Vol. 13; no. 12; pp. 14357 - 14367
• Main Authors: Ryu, Jaegeon, Park, Byeongho, Kang, Jieun, Hong, Dongki, Kim, Sung-Dae, Yoo, Jung-Keun, Yi, Jin Woo, Park, Soojin, Oh, Youngseok
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 24.12.2019
• Subjects: imide-based network; aerogels; lithium-ion batteries; monolithic organic electrodes; single-walled carbon nanotubes
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.9b07807

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–1 (corresponding to the areal capacity of ∼2.8 mA h cm–2). 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.