For wearable electronic devices to be fully integrated into garments, without restricting or impeding movement, requires flexible and stretchable inks and coatings, which must have consistent performance and recover from mechanical strain. Combining Carbon Black (CB) and ammonia plasma functionalized Graphite Nanoplatelets (GNPs) in a Thermoplastic Polyurethane (TPU) resin created a conductive ink that could stretch to substrate failure (>300% nominal strain) and cyclic strains of up to 100% while maintaining an electrical network. This highly stretchable, conductive screen-printable ink was developed using relatively low-cost carbon materials and scalable processes making it a candidate for future wearable developments. The electromechanical performance of the carbon ink for wearable technology is compared to a screen-printable silver as a control. After initial plastic deformation and the alignment of the nano carbons in the matrix, the electrical performance was consistent under cycling to 100% nominal strain. Although the GNP flakes are pulled further apart a consistent, but less conductive path remains through the CB/TPU matrix. In contrast to the nano carbon ink, a more conductive ink made using silver flakes lost conductivity at 166% nominal strain falling short of the substrate failure strain. This was attributed to the failure of direct contact between the silver flakes.
Printing inks typically consist of a functional component dispersed within a low-viscosity resin/solvent system where interparticle interactions would be expected to play a significant role in dispersion, especially for the high-aspect-ratio nanocarbons such as the graphite nanoplatelets (GNPs). Rheology has been suggested as a method for assessing the dispersion of carbon nanomaterials in a fluid. The effects of phase volume of ammonia plasma-functionalized GNPs on a near-Newtonian low-viscosity thermoplastic polyurethane (TPU) resin system have been studied using shear and quiescent oscillatory rheology. At low concentrations, the GNPs were well dispersed with a similar shear profile and viscoelastic behavior to the unfilled TPU resin, as viscous behavior prevailed indicating the absence of any long-range order within the fluid. Particle interactions increased rapidly as the phase volume tended toward maximum packing fraction, producing rapid increases in the relative viscosity, increased low shear rate shear thinning, and the elastic response becoming increasingly frequency independent. The nanoscale dimensions and high-aspect-ratio GNPs occupied a large volume within the flow, while small interparticle distances caused rapid increases in the particle-particle interactions to form flocculates that pack less effectively. Established rheological models were fitted to the experimental data to model the effect of high-aspect-ratio nanocarbon on the viscosity of a low-viscosity system. Using the intrinsic viscosity and the maximum packing fraction as fitting parameters, the Krieger-Dougherty (K-D) model provided the best fit with values. There was good agreement between the estimates of aspect ratio from the SEM images and the predictions of the aspect ratio from the rheological models. The fitting of the K-D model to measured viscosities at various phase volumes could be an effective method in characterizing the shape and dispersion of high-aspect-ratio nanocarbons.
Carbon-based pastes and inks are used extensively in a wide range of printed electronics because of their widespread availability, electrical conductivity and low cost. Overcoming the inherent tendency of the nano-carbon to agglomerate to form a stable dispersion is necessary if these inks are to be taken from the lab scale to industrial production. Plasma functionalization of graphite nanoplatelets (GNP) adds functional groups to their surface to improve their interaction with the polymer resin. This offers an attractive method to overcome these problems when creating next generation inks. Both dynamic and oscillatory rheology were used to evaluate the stability of inks made with different loadings of functionalized and unfunctionalized GNP in a thin resin, typical of a production ink. The rheology and the printability tests showed the same level of dispersion and electrical performance had been achieved with both functionalized and unfunctionalized GNPs. The unfunctionalized GNPs agglomerate to form larger, lower aspect particles, reducing interparticle interactions and particle–medium interactions. Over a 12-week period, the viscosity, shear thinning behavior and viscoelastic properties of the unfunctionalized GNP inks fell, with decreases in viscosity at 1.17 s−1 of 24, 30, 39% for the ϕ = 0.071, 0.098, 0.127 GNP suspensions, respectively. However, the rheological properties of the functionalized GNP suspensions remained stable as the GNPs interacted better with the polymer in the resin to create a steric barrier which prevented the GNPs from approaching close enough for van der Waals forces to be effective.
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