An inkjet printing process for depositing palladium (Pd) thin films from a highly loaded ink (>14 wt%) is reported. The viscosity and surface tension of a Pd-organic precursor solution is adjusted using toluene to form a printable and stable ink. A two-step thermolysis process is developed to convert the printed ink to continuous and uniform Pd films with good adhesion to different substrates. Using only one printing pass, a low electrical resistivity of 2.6 μΩ m of the Pd film is obtained. To demonstrate the electrochemical pH sensing application, the surfaces of the printed Pd films are oxidized for ion-to-electron transduction and the underlying layer is left for electron conduction. Then, solid-state reference electrodes are integrated beside the bifunctional Pd electrodes by inkjet printing. These potentiometric sensors have sensitivities of 60.6 ± 0.1 and 57 ± 0.6 mV pH −1 on glass and polyimide substrates, and short response times of 11 and 6 s, respectively. Also, accurate pH values of real water samples are obtained by using the printed sensors with a low-cost multimeter. These results indicate that the facile and cost-effective inkjet printing and integration techniques may be applied in fabricating future electrochemical monitoring systems for environmental parameters and human health conditions.
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IntroductionInkjet printing is an easy-to-use and low-cost approach to simultaneously deposit and pattern thin film materials from solutions. This technology can produce structures with fine patterns, consumes a small amount of materials, does not need complicated equipment, and is compatible with largearea processing lines for flexible and non-planar substrates. [1] Numerous applications, for example, high-resolution electrodes, [2,3] field-effect transistors, [4] solar cells, [5] light-emitting devices, [6] bio/chemical sensors, [7] and bio-printed tissues, [8] were enabled by using inkjet printing technology. In these electron transfer in the high-resistance films results in a poor sensing performance. [23] One method to reduce the resistance is to print the lightly loaded ink using multiple passes, but this is time-consuming. [15] Alternatively, highly loaded Pd inks and their inkjet printing processes can be developed to deposit continuous, homogenous, and conductive Pd films using a single print pass, thus making it a fast film deposition technique.In this work, we developed an ink loaded with >14 wt% Pd for inkjet printing. The inkjet printing process for such ink is optimized for the deposition of continuous, uniform and lowresistivity thin films with good adhesion to the underlying substrates. Utilizing this ink and printing process, we demonstrate the practical and cost-effective fabrication of an integrated pH sensing platform on both rigid and flexible substrates. Bifunctional sensing electrodes are fabricated by oxidizing the printed Pd. The PdO-rich surfaces function as pH sensing layers and the conductive portion beneath the surfaces are electron conduction paths. Solid-state reference elec...