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.