Evaluation on the Intrinsic Physicoelectrochemical Attributes and Engineering of Micro-, Nano-, and 2D-Structured Allotropic Carbon-Based Papers for Flexible Electronics

[Image: see text] Flexible electronics have gained more attention for emerging electronic devices such as sensors, biosensors, and batteries with advantageous properties including being thin, lightweight, flexible, and low-cost. The development of various forms of allotropic carbon papers provided a new dry-manufacturing route for the fabrication of flexible and wearable electronics, while the electrochemical performance and the bending stability are largely influenced by the bulk morphology and the micro-/nanostructured domains of the carbon papers. Here, we evaluate systematically the intrinsic physicoelectrochemical properties of allotropic carbon-based conducting papers as flexible electrodes including carbon-nanotubes-paper (CNTs-paper), graphene-paper (GR-paper), and carbon-fiber-paper (CF-paper), followed by functionalization of the allotropic carbon papers for the fabrication of flexible electrodes. The morphology, chemical structure, and defects originating from the allotropic nanostructured carbon materials were characterized by scanning electron microscopy (SEM) and Raman spectroscopy, followed by evaluating the electrochemical performance of the corresponding flexible electrodes by cyclic voltammetry and electrochemical impedance spectroscopy. The electron-transfer rate constants of the CNTs-paper and GR-paper electrodes were ∼14 times higher compared with the CF-paper electrode. The CNTs-paper and GR-paper electrodes composed of nanostructured carbon showed significantly higher bending stabilities of 5.61 and 4.96 times compared with the CF-paper. The carbon-paper flexible electrodes were further functionalized with an inorganic catalyst, Prussian blue (PB), forming the PB-carbon-paper catalytic electrode and an organic conducting polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), forming the PEDOT-carbon-paper capacitive electrode. The intrinsic attribute of different allotropic carbon electrodes affects the deposition of PB and PEDOT, leading to different electrocatalytic and capacitive performances. These findings are insightful for the future development and fabrication of advanced flexible electronics with allotropic carbon papers.