High performance all-carbon composite transparent electrodes containing uniform carbon nanotube networks

•Highly efficient and bending durable all-carbon composite transparent electrodes (TEs) are designed.•The performance was strongly dependent on morphology of CNT networks on graphene.•The mechanism relies on the defect reductions in graphene by uniform CNT coating.•The CNT/graphene composite was the most effective TEs against mechanical bending.

Indium tin oxide-free, flexible transparent electrodes (TEs) are crucial for the future commercialization of flexible and wearable electronics. While carbon-based TEs containing carbon nanotube (CNT) networks show promise, they usually exhibit poor dispersion properties, limiting their performance and practicality. In this study, we report a highly efficient and bending durable all-carbon composite TE (ac-TE) that employs uniform CNT networks on a monolayer graphene/polyethylene terephthalate (PET) substrate via a simple air spray deposition method. The air-sprayed CNT/graphene assembly was free-standing on solution, making a polymer-free transfer of carbon composites to target substrates possible. The excellent performance of the ac-TEs was attributed to the uniformly networked CNTs on the polycrystalline graphene with a well-controlled density, effectively bridging the line defects and filling the tears/voids or folds necessarily existing in the as-processed graphene. The sheet resistance of the ac-TEs was increased only 6% from its original value at a bending radius of 2.7 mm, while that of the pristine graphene/PET assembly increased 237%. Mechanical bending of the ac-TEs worsened the electrical performance by only ∼1.7% after 2000 bending cycles at a bending radius of 2.5 mm. Degradation of the performance by the bending was the result of line defects formation in the graphene, demonstrating the potential of the uniform CNT networks to achieve more efficient and flexible carbon-based TEs. Furthermore, the chemically-doped ac-TEs showed commercially suitable electronic and optical properties with much enhanced thermal stability, closer to practical TEs in flexible devices.