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.
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.
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.
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.
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