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Fully exploiting the properties of 2D crystals requires a mass productionmethod able to produce heterostructures of arbitrary complexity on anysubstrate, including plastic. Solution processing of graphene allows simple andlow-cost techniques such as inkjet printing to be used for device fabrication.However, available inkjet printable formulations are still far from ideal asthey are either based on toxic solvents, have low concentration, or requiretime-consuming and expensive formulation processing. In addition, none of thoseformulations are suitable for thin-film heterostructure fabrication due to there-mixing of different 2D crystals, giving rise to uncontrolled interfaces,which results in poor device performance and lack of reproducibility. In thiswork we show a general formulation engineering approach to achieve highlyconcentrated, and inkjet printable water-based 2D crystal formulations, whichalso provides optimal film formation for multi-stack fabrication. We showexamples of all-inkjet printed heterostructures, such as large area arrays ofphotosensors on plastic and paper and programmable logic memory devices, fullyexploiting the design flexibility of inkjet printing. Finally, dose-escalationcytotoxicity assays in vitro also confirm the inks biocompatible character,revealing the possibility of extending use of such 2D crystal formulations todrug delivery and biomedical applications.

Water-based and Biocompatible 2D Crystal Inks: from Ink Formulation to All- Inkjet Printed Heterostructures