Solution-Processable Conductive Graphene-Based Materials for Flexible Electronics

This thesis work explores electrical conductors based on few-layer graphene flakes as an enabler for low-cost, mechanically flexible, and high-conductivity conductors in large area flexible and printed electronic devices. The flakes are deposited from aqueous solutions and processed at low temperature. Graphene is selected for its excellent properties in mechanical, optical, electronic, and electrical aspects. However, thin films of pristine few-layer graphene flakes deposited from dispersions normally exhibit inferior electrical conductivity. One cause responsible for this problem is the loose stacking and random orientation of graphene flakes in a graphene deposition. We have solved this problem by implementing a simple post-deposition treatment leading to dramatically densified and planarized thin films. Significantly increased electrical conductivity by ~20 times is obtained. The 1-pyrenebutyric acid tetrabutylammonium salt as an exfoliation enhancer and dispersant in water yields ~110 S/m in conductivity when the graphene based thin films are processed at 90 °C. In order to achieve higher conductivity, a room-temperature method for site-selective copper electroless deposition has been developed. This method is of particular interest for the self-aligned copper deposition to the predefined graphene films. The resultant two-layer graphene/copper structure is characterized by an overall conductivity of ~7.9 × 105 S/m, an increase by ~7000 times from the template graphene films. Several electronic circuits based on the graphene/copper bilayer interconnect have been subsequently fabricated on plastic foils as proof-of-concept demonstrators. Alternatively, highly conductive composites featuring graphene flakes coated with silver nanoparticles with electrical conductivity beyond 106 S/m can be readily obtained at 100 oC. Moreover, a highly conductive reduced-graphene-oxide/copper hybrid hydrogel has been achieved by mixing aqueous graphene oxide solution and copper-containing Fehling's solution. The corresponding aerogel of high porosity exhibits an apparent electrical conductivity of ~430 S/m and delivers a specific capacity of ~453 mAh g−1 at current density of 1 A/g. The experimental results presented in this thesis show that the solution-phase, low-temperature fabrication of highly conductive graphene-based materials holds promises for flexible electronics and energy storage applications.