Large-scale layer-by-layer inkjet printing of flexible iridium-oxide based pH sensors

Metal oxide based pH sensors are used in various applications, especially when the conventional glass electrode is unsuitable due to its fragility or when the applications require disposable sensors, e.g. for biomedical, clinical or food process monitoring. Generally, such pH sensors are produced by thermal oxidation or electrochemical deposition, neither suited for mass production nor miniaturization. Herein, we report on the fabrication of reliable and sensitive pH sensors based on the nano-assembly of iridium oxide (IrOx) nanoparticles and polydiallyldimethylammonium (PDDA) polymer layers. Such potentiometric sensors were very reproducibly fabricated on a large-scale via a layer-by-layer inkjet printing (LbL IJP) methodology. The obtained results indicated the ability of the LbL IJP technique to easily manipulate the NP coverage by the number of printed bilayers, leading to a swift sensor optimization. Open-circuit potentials were recorded to evaluate the pH sensitivity, response time, and reproducibility of the pH electrodes, which exhibit a rapid, linear and near-Nernstian pH response of about 59 mV/pH. Moreover, an RSD of 0.6% for five different electrodes from the same printing batch showed the excellent reproducibility of the IJP process with a correlation coefficient of 0.99 for all measurements. The insights gained in this study could be the basis for a new approach of developing scalable, patterned and flexible pH sensors with improved performance and a wide range of applications.