Self-Assembling Graphene Layers for Electrochemical Sensors Printed in a Single Screen-Printing Process

This article reports findings on screen-printed electrodes employed in microfluidic diagnostic devices. The research described includes developing a series of graphene- and other carbon form-based printing pastes compared to their rheological parameters, such as viscosity in static and shear-thinning conditions, yield stress, and shear rate required for thinning. In addition, the morphology, electrical conductivity, and electrochemical properties of the electrodes, printed with the examined pastes, were investigated. Correlation analysis was performed between all measured parameters for six electrode materials, yielding highly significant (p-value between 0.002 and 0.017) correlations between electron transfer resistance (Ret), redox peak separation, and static viscosity and thinning shear-rate threshold. The observed more electrochemically accessible surface was explained according to the fluid mechanics of heterophase suspensions. Under changing shear stress, the agglomeration enhanced by the graphene nanoplatelets’ interparticle affinity led to phase separation. Less viscous pastes were thinned to a lesser degree, allowing non-permanent clusters to de-agglomerate. Thus, the breaking of temporary agglomerates yielded an unblocked electrode surface. Since the mechanism of phase ordering through agglomeration and de-agglomeration is affected by the pastes’ rheology and stress during the printing process and requires no further treatment, it can be appropriately labeled as a self-assembling electrode material.