Water-based and biocompatible 2D crystal inks for all-inkjet-printed heterostructures

Fully exploiting the properties of 2D crystals requires a mass production method able to produce heterostructures of arbitrary complexity on any substrate, including plastic. Solution processing of graphene allows simple and low-cost techniques such as inkjet printing to be used for device fabrication. However, available inkjet printable formulations are still far from ideal as they are either based on toxic solvents, have low concentration, or require time-consuming and expensive formulation processing. In addition, none of those formulations are suitable for thin-film heterostructure fabrication due to the re-mixing of different 2D crystals, giving rise to uncontrolled interfaces, which results in poor device performance and lack of reproducibility. In this work we show a general formulation engineering approach to achieve highly concentrated, and inkjet printable water-based 2D crystal formulations, which also provides optimal film formation for multi-stack fabrication. We show examples of all-inkjet printed heterostructures, such as large area arrays of photosensors on plastic and paper and programmable logic memory devices, fully exploiting the design flexibility of inkjet printing. Finally, dose-escalation cytotoxicity assays in vitro also confirm the inks biocompatible character, revealing the possibility of extending use of such 2D crystal formulations to drug delivery and biomedical applications.