A flexible free-standing defect-rich MoS2/graphene/carbon nanotube hybrid paper as a binder-free anode for high-performance lithium ion batteries

Abstract

The rapid development of flexible energy storage devices has motivated people to seek reliable electrodes with both high mechanical flexibility and excellent electrochemical performance. Herein, we demonstrate a facile and scalable process to fabricate a flexible free-standing defect-rich MoS₂/graphene/carbon nanotube (dr-MGC) hybrid paper, which can be directly used as a flexible binder-free anode for lithium ion batteries. Benefiting from the excellent dispersibility of defect-rich MoS₂ nanosheets (dr-MoS₂ NSs) and graphene oxide/carbon nanotube (GO/CNT) hybrids in aqueous solution, a unique three-dimensional (3D) nanoporous architecture with ultrathin dr-MoS₂ NSs homogeneously embedded in graphene/CNT frameworks is nicely constructed by a simple vacuum filtration and thermal reduction process. As a consequence, the flexible free-standing dr-MGC21 hybrid paper exhibits a high reversible capacity of 1137.2 mA h g⁻¹ at a current density of 0.1 A g⁻¹ with excellent cyclic stability and rate capability. The superior electrochemical performance of the dr-MGC hybrid paper is ascribed to the 3D nanoporous architecture as well as the synergistic effect between the dr-MoS₂ NSs and conductive graphene/CNT network. Moreover, the idea of utilizing graphene/CNT hybrids as flexible conductive frameworks provides a novel pathway for the large-scale fabrication of various flexible binder-free electrodes for high-performance flexible energy storage devices.