Hierarchically core-shell structured nanocellulose/carbon nanotube hybrid aerogels for patternable, self-healing and flexible supercapacitors

Xiaoyu Cheng; Huixiang Wang; Shaowei Wang; Yue Jiao; Chenyu Sang; Shaohua Jiang; Shuijian He; Changtong Mei; Xinwu Xu; Huining Xiao; Jingquan Han

doi:10.1016/j.jcis.2024.01.160

Hierarchically core-shell structured nanocellulose/carbon nanotube hybrid aerogels for patternable, self-healing and flexible supercapacitors

J Colloid Interface Sci. 2024 Apr 15:660:923-933. doi: 10.1016/j.jcis.2024.01.160. Epub 2024 Jan 24.

Authors

Affiliations

¹ Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Joint International Research Lab of Lignocellulosic Functional Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China.
² Department of Biological Sciences, Xinzhou Normal University, Xinzhou, Shanxi 034000, China.
³ Chemical Engineering Department, New Brunswick University, Fredericton, New Brunswick E3B5A3, Canada. Electronic address: hxiao@unb.ca.
⁴ Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Joint International Research Lab of Lignocellulosic Functional Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China. Electronic address: hjq@njfu.edu.cn.

PMID: 38280285
DOI: 10.1016/j.jcis.2024.01.160

Abstract

The flexible and self-healing supercapacitors (SCs) are considered to be promising smart energy storage devices. Nevertheless, the SCs integrated with flexibility, lightweight, pattern editability, self-healing capabilities and desirable electrochemical properties remain a challenge. Herein, an all-in-one self-healing SC fabricated with the free-standing hybrid film (TCMP) composed of the 2,2,6,6-tetramethylpiperidin-1-yloxy-oxidized cellulose nanofibers (TOCNs) carried carbon nanotubes (CNTs), manganese dioxide (MnO₂) and polyaniline (PANI) as the electrode, polyvinyl alcohol/sulfuric acid (PVA/H₂SO₄) gel as the electrolyte and dynamically cross-linked cellulose nanofibers/PVA/sodium tetraborate decahydrate (CNF/PB) hydrogel as the self-healing electrode matrix is developed. The TCMP film electrodes are fabricated through a facile in-situ polymerization of MnO₂ and PANI in TOCNs-dispersed CNTs composite networks, exhibiting lightweight, high electrical conductivity, flexibility, pattern editability and excellent electrochemical properties. Benefited from the hierarchically porous structure and high mechanical properties of TOCNs, excellent electrical conductivity of CNTs and the desirable synergistic effect of pseudocapacitance induced by MnO₂ and PANI, the assembled SC with an interdigital structure demonstrated a high areal capacitance of 1108 mF cm^-2 at 2 mA cm^-2, large areal energy density of 153.7 μWh cm^-2 at 1101.7 μW cm^-2. A satisfactory bending cycle performance (capacitance retention up to 95 % after 200 bending deformations) and self-healing characteristics (∼90 % capacitance retention after 10 cut/repair cycles) are demonstrated for the TCMP-based symmetric SC, delivering a feasible strategy for electrochemical energy storage devices with excellent performance, designable patterns and desirable safe lifespan.

Keywords: Carbon nanotube; Manganese dioxide; Nanocellulose; Polyaniline; Self-healing; Supercapacitor.