Graphene and related two-dimensional materials provide an ideal platform for next generation disruptive technologies and applications. Exploiting these solution-processed two-dimensional materials in printing can accelerate this development by allowing additive patterning on both rigid and conformable substrates for flexible device design and large-scale, high-speed, cost-effective manufacturing. In this review, we summarise the current progress on ink formulation of two-dimensional materials and the printable applications enabled by them. We also present our perspectives on their research and technological future prospects.

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Recent advances in inkjet printing of two-dimensional (2D) crystals show great promise for next-generation printed electronics development. Printing nonuniformity, however, results in poor reproducibility in device performance and remains a major impediment to their large-scale manufacturing. At the heart of this challenge lies the coffee-ring effect (CRE), ring-shaped nonuniform deposits formed during postdeposition drying. We present an experimental study of the drying mechanism of a binary solvent ink formulation. We show that Marangoni-enhanced spreading in this formulation inhibits contact line pinning and deforms the droplet shape to naturally suppress the capillary flows that give rise to the CRE. This general formulation supports uniform deposition of 2D crystals and their derivatives, enabling scalable and even wafer-scale device fabrication, moving them closer to industrial-level additive manufacturing.

Fabricating a protein microarray involves the deposition of nanoliter droplets of solutions on a solid surface. Instead of uniform spots, one often observes ring-like structures that add to the difficulty in quantification. We show that the accumulation of proteins at the air/water interface of the nanodroplet is the reason. Transformation to a uniform spot can be achieved via the addition of competitive surfactants or the control of surface reaction kinetics.

Early diagnosis in exhaled breath is a key technology for next-generation personal healthcare monitoring. Current chemiresistive sensors, primarily based on metal oxide (MOx) thin films, have limited applicability in such portable systems due to their high power consumption, long recovery time, poor device-to-device consistency, and baseline drifts. To address these challenges for ammonia ($${{\rm{NH}}}_{3}$$ NH 3 ) detection in exhaled breath, a critical biomarker for a variety of kidney and liver problems, we present a formulation of a graphene–MOx functional ink-based sensing platform. We integrate our sensing layer directly onto miniaturized CMOS microhotplates (μHP) via inkjet printing, potentially enabling scalability and device-to-device performance repeatability. Using stage-by-stage temporal analysis, and a temperature-pulsed modulation (TM) strategy, we achieve ultrahigh responsivity (1500% at 10 ppm pure $${{\rm{NH}}}_{3}$$ NH 3 ), fast response and recovery time (28 and 43 s), ultralow power consumption (~6 mW), negligible baseline drift (<0.67%), excellent cross-device and cross-cycle consistency (<0.5% and <0.41% variation in responsivity) and long-term stability (<1% variation) in our graphene–zinc oxide (ZnO) formulation, outperforming conventional MOx chemiresistive sensors. We further mitigate the effect of humidity through our measurement protocols, while interference from acetone is compensated through the parallel deployment of an additional inkjet printed graphene–tungsten oxide ($${{\rm{WO}}}_{3}$$ WO 3 ) device as part of the sensor array. Our dual graphene–MOx formulations and their integration with ultralow power CMOS through inkjet printing represent a significant step towards reliable and portable multi-analyte breath diagnostics.

Solution-processable thin-film dielectrics represent an important material family for large-area, fully-printed electronics. Yet, in recent years, it has seen only limited development, and has mostly remained confined to pure polymers. Although it is possible to achieve excellent printability, these polymers have low (≈2-5) dielectric constants (ε r). There have been recent attempts to use solution-processed 2D hexagonal boron nitride (h-BN) as an alternative. However, the deposited h-BN flakes create porous thin-films, compromising their mechanical integrity, substrate adhesion, and susceptibility to moisture. These challenges are addressed by developing a "one-pot" formulation of polyurethane (PU)-based inks with h-BN nano-fillers. The approach enables coating of pinhole-free, flexible PU+h-BN dielectric thin-films. The h-BN dispersion concentration is optimized with respect to exfoliation yield, optical transparency, and thin-film uniformity. A maximum ε r ≈ 7.57 is achieved, a twofold increase over pure PU, with only 0.7 vol% h-BN in the dielectric thinfilm. A high optical transparency of ≈78.0% (≈0.65% variation) is measured across a 25 cm 2 area for a 10 μm thick dielectric. The dielectric property of the composite is also consistent, with a measured areal capacitance variation of <8% across 64 printed capacitors. The formulation represents an optically transparent, flexible thin-film, with enhanced dielectric constant for printed electronics.

Printing has drawn a lot of attention as a means of low per-unit cost and high throughput patterning of graphene inks for scaled-up thin-form factor device manufacturing. However, traditional printing processes require a flat surface and are incapable of achieving patterning onto 3D objects. Here, a conformal printing method is presented to achieve functional graphene-based patterns onto arbitrarily shaped surfaces. Using experimental design, a water-insoluble graphene ink with optimum conductivity is formulated. Then single-and multilayered electrically functional structures are printed onto a sacrificial layer using conventional screen printing. The print is then floated on water, allowing the dissolution of the sacrificial layer, while retaining the functional patterns. The single-and multilayer patterns can then be directly transferred onto arbitrarily shaped 3D objects without requiring any postdeposition processing. Using this technique, conformal printing of single-and multilayer functional devices that include joule heaters, resistive deformation sensors, and proximity sensors on hard, flexible, and soft substrates, such as glass, latex, thermoplastics, textiles, and even candies and marshmallows, is demonstrated. This simple strategy promises to add new device and sensing functionalities to previously inert 3D surfaces.

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