Dual-Ligand Red Perovskite Ink for Electrohydrodynamic Printing Color Conversion Arrays over 2540 dpi in Near-Eye Micro-LED Display.

The lack of stability of red perovskite nanocrystals (PeNCs) remains the main problem that restricts their patterning application. In this work, the dual-ligand passivation strategy was introduced to stabilize PeNCs and inhibit their halogen ion migration during high-voltage electrohydrodynamic (EHD) inkjet printing. The as-printed red arrays exhibit the highest emisson intensity and least blue shift compared with samples with other passivation strategies under a high electric field during EHD inkjet printing. Combining with blue and green PeNC inks, single-color and tricolor color conversion layer arrays were successfully printed, with minimum pixel size of 5 µm and the highest spatial resolution of 2540 dpi. The color coordinate of CsPbBrI2 NCs arrays are located close to the red point, with a color gumat of 97.28% of Rec. 2020 standard. All of these show great potential in the application of color conversion layers in a near-eye micro-LED display.

Nanostructure Tuning of Gold Nanoparticles Films via Click Sintering.

Colloidal metal nanoparticles dispersions are commonly used to create functional printed electronic devices and they typically require time-, energy- and equipment-consuming post-treatments to improve their electrical and mechanical properties. Traditional methods, e.g. thermal, UV/IR, and microwave treatments, limit the substrate options and may require expensive equipment, not available in all the laboratories. Moreover, these processes also cause the collapse of the film (nano)pores and interstices, limiting or impeding its nanostructuration. Finding a simple approach to obtain complex nanostructured materials with minimal post-treatments remains a challenge. In this study, a new sintering method for gold nanoparticle inks that called as "click sintering" has been reported. The method uses a catalytic reaction to enhance and tune the nanostructuration of the film while sintering the metallic nanoparticles, without requiring any cumbersome post-treatment. This results in a conductive and electroactive nanoporous thin film, whose properties can be tuned by the conditions of the reaction, i.e., concentration of the reagent and time. Therefore, this study presents a novel and innovative one-step approach to simultaneously sinter gold nanoparticles films and create functional nanostructures, directly and easily, introducing a new concept of real-time treatment with possible applications in the fields of flexible electronics, biosensing, energy, and catalysis.

Fully Printed Multilayer Ceramic Capacitors Based on High-k Perovskite Nanosheets.

Printing technology enables the integration of chemically exfoliated perovskite nanosheets into high-performance microcapacitors. Theoretically, the capacitance value can be further enhanced by designing and constructing multilayer structures without increasing the device size. Yet, issues such as interlayer penetration in multilayer heterojunctions constructed using inkjet printing technology further limit the realization of this potential. Herein, a series of multilayer configurations, including Ag/(Ca2NaNb4O13/Ag)n and graphene/(Ca2NaNb4O13/graphene)n (n = 1-3), are successfully inkjet-printed onto diverse rigid and flexible substrates through optimized ink formulations, inkjet printing parameters, thermal treatment conditions, and rational multilayer structural design using high-k perovskite nanosheets, graphene nanosheets and silver. The dielectric performance is optimized by fine-tuning the number of dielectric layers and modifying the electrode/dielectric interface. As a result, the graphene/(Ca2NaNb4O13/graphene)3 multilayer ceramic capacitors exhibit a remarkable capacitance density of 346 ± 12 nF cm-2 and a high dielectric constant of 193 ± 18. Additionally, these devices demonstrate moderate insulation properties, flexibility, thermal stability, and chemical sensitivity. This work shed light on the potential of multilayer structural design in additive manufacturing of high-performance 2D material-based ceramic capacitors.

Systematic Investigation of Novel, Controlled Low-Temperature Sintering Processes for Inkjet Printed Silver Nanoparticle Ink.

Functional inks enable manufacturing of flexible electronic devices by means of printing technology. Silver nanoparticle (Ag NP) ink is widely used for printing conductive components. A sintering process is required to obtain sufficient conductivity. Thermal sintering is the most commonly used method, but the heat must be carefully applied to avoid damaging low-temperature substrates such as polymer films. In this work, two alternative sintering methods, damp heat sintering and water sintering are systematically investigated for inkjet-printed Ag tracks on polymer substrates. Both methods allow sintering polyvinyl pyrrolidone (PVP) capped Ag NPs at 85°C. In this way, the resistance is significantly reduced to only 1.7 times that of the samples on polyimide sintered in an oven at 250°C. The microstructure of sintered Ag NPs is analyzed. Taking the states of the capping layer under different conditions into account, the explanation of the sintering mechanism of Ag NPs at low temperatures is presented. Overall, both damp heat sintering and water sintering are viable options for achieving high conductivity of printed Ag tracks. They can broaden the range of substrates available for flexible electronic device fabrication while mitigating substrate damage risks. The choice between them depends on the specific application and the substrate used.

Engineering Proteins for PEDOT Dispersions: A New Horizon for Highly Mixed Ionic-Electronic Biocompatible Conducting Materials.

Poly (3,4-ethylenedioxythiophene) (PEDOT) doped with polystyrene sulfonate (PSS) is the most used conducting polymer from energy to biomedical applications. Despite its exceptional properties, there is a need for developing new materials that can improve some of its inherent limitations, e.g., biocompatibility. In this context, doping PEDOT is propose with a robust recombinant protein with tunable properties, the consensus tetratricopeptide repeated protein (CTPR). The doping consists of an oxidative polymerization, where the PEDOT chains are stabilized by the negative charges of the CTPR protein. CTPR proteins are evaluated with three different lengths (3, 10, and 20 identical CTPR units) and optimized varied synthetic conditions. These findings revealed higher doping rate and oxidized state of the PEDOT chains when doped with the smallest scaffold (CTPR3). These PEDOT:CTPR hybrids possess ionic and electronic conductivity. Notably, PEDOT:CTPR3 displayed an electronic conductivity of 0.016 S cm-1, higher than any other reported protein-doped PEDOT. This result places PEDOT:CTPR3 at the level of PEDOT-biopolymer hybrids, and brings it closer in performance to PEDOT:PSS gold standard. Furthermore, PEDOT:CTPR3 dispersion is successfully optimized for inkjet printing, preserving its electroactivity properties after printing. This approach opens the door to the use of these novel hybrids for bioelectronics.

Structural Effects of 3D Inkjet-Printed Ni(O)-YSZ Pillared Electrodes on Performances of Solid Oxide Electrochemical Reactors.

Increasing densities of reaction sites for gaseous reactants in solid oxide electrochemical reactors (SOERs), is a key strategy for achieving enhanced performance in either fuel cell or electrolysis modes. Fabrication of 3D structured components in SOERs can enhance those densities of reaction sites, which is achieved by 3D inkjet printing with high reproducibility, having developed inks with appropriate properties. First, the effects of pillar geometries on SOER performances are predicted through numerical simulations, enabling subsequent 3D printing to focus on the more effective geometries. Herein, the study reports the results of experimental validation of those predictions by evaluating the electrochemical performances of cells with various heights of 3D inkjet-printed Ni(O)- yttria stabilized zirconia (YSZ) pillars and YSZ pillars. Those measurements prove that increasing pillar heights generally increases SOER peak power densities in fuel cell mode and increased current densities at the thermoneutral potential (1.285 V) in steam electrolysis mode, as predicted by simulations. With increasing pillar heights, more limitations in performance enhancement are found with YSZ electrolyte pillars than with Ni-YSZ pillars, again as predicted by simulations. The subsequent microstructural analysis of Ni-YSZ pillars proves the suitability of the Ni(O)-YSZ composite particle ink formulation and the reliability of 3D printing.

Inkjet printing of heavy-metal-free quantum dots-based devices: a review.

Inkjet printing (IJP) has become a versatile, cost-effective technology for fabricating organic and hybrid electronic devices. Heavy-metal-based quantum dots (HM QDs) play a significant role in these inkjet-printed devices due to their excellent optoelectrical properties. Despite their utility, the intrinsic toxicity of HM QDs limits their applications in commercial products. To address this limitation, developing alternative HM-free quantum dots (HMF QDs) that have equivalent optoelectronic properties to HM QD is a promising approach to reduce toxicity and environmental impact. This article comprehensively reviews HMF QD-based devices fabricated using IJP methods. The discussion includes the basics of IJP technology, the formulation of printable HMF QD inks, and solutions to the coffee ring effect. Additionally, this review briefly explores the performance of typical state-of-the-art HMF QDs and cutting-edge characterization techniques for QD inks and printed QD films. The performance of printed devices based on HMF QDs is discussed and compared with those fabricated by other techniques. In the conclusion, the persisting challenges are identified, and perspectives on potential avenues for further progress in this rapidly developing research field are provided.

Disaccharide-assisted inkjet freezing for improved cell viability.

Non-permeable disaccharides are widely used as cryoprotectant agents due to their low cytotoxicity, but their protective effect is insufficient when the disaccharides are present only extracellularly. On the other hand, cryoprotectant agent (CPA)-free cryopreservation has been recently achieved by instantaneously inkjet-freezing cells as tiny droplets. However, CPA-free cryopreservation requires skilled handling operations due to instability of the vitreous water without the CPA. In this study, the effectiveness of separately adding two types of disaccharides in inkjet freezing of 3T3 cells was evaluated and the following results were obtained. First, trehalose showed the highest effect at 0.57 M, twice the plasma osmolarity, with a maximum cell viability of over 90 % when freezing 70 pL droplets. However, higher concentrations of trehalose decreased cell viability due to damage caused by dehydration. Similarly, sucrose gave cell viability close to 90 % at 0.57 M with 70 pL droplets, and higher concentrations decreased cell viability. Next, the relationship between minimum trehalose concentrations to prevent intracellular and extracellular ice crystal formation and droplet size was analyzed. The results indicated that trehalose of less than 0.57 M was able to inhibit intracellular ice crystal formation even in the largest droplet used in this study, 450 pL, while trehalose of nearly 0.57 M was required to inhibit extracellular ice crystal formation in the smallest droplet, 70 pL. In other words, the suppression of extracellular ice crystals by the addition of CPA was shown to be crucial in improving the viability of inkjet superflash freezing.

A moisture-enabled fully printable power source inspired by electric eels.

Great efforts have been made to build integrated devices to enable future wearable electronics; however, safe, disposable, and cost-effective power sources still remain a challenge. In this paper, an all-solid-state power source was developed by using graphene materials and can be printed directly on an insulating substrate such as paper. The design of the power source was inspired by electric eels to produce programmable voltage and current by converting the chemical potential energy of the ion gradient to electric energy in the presence of moisture. An ultrahigh voltage of 192 V with 175 cells in series printed on a strip of paper was realized under ambient conditions. For the planar cell, the mathematical fractal design concept was adapted as printed patterns, improving the output power density to 2.5 mW cm-3, comparable to that of lithium thin-film batteries. A foldable three-dimensional (3D) cell was also achieved by employing an origami strategy, demonstrating a versatile design to provide green electric energy. Unlike typical batteries, this power source printed on flexible paper substrate does not require liquid electrolytes, hazardous components, or complicated fabrication processes and is highly customizable to meet the demands of wearable electronics and Internet of Things applications.

Effect of polymethyl methacrylate on in situ patterning of perovskite quantum dots by inkjet printing.

The preparation of perovskite quantum dots (PQDs) using an in situ inkjet printing method is beneficial for improving the problems of aggregation and photoluminescence (PL) quenching during long-term storage. However, the stability of PQDs prepared using this method is still not ideal, and the morphology of in situ-printed patterns needs to be optimized. To address these problems, this study introduced polymethyl methacrylate (PMMA) into the process of in situ inkjet printing of PQDs and explored the effect of PMMA on the in situ patterning effect of PQDs. The results showed that using a mixed precursor solution containing a small amount of PMMA as the printing ink can slow down the shrinkage process of ink droplets and improve the uniformity of film formation. As the printing substrate, PMMA provided a suitable high-viscosity environment for the in situ growth of PQDs. This could effectively suppress the coffee ring effect. In addition, the interaction between the C=O=C group in PMMA and metal ion Pb2+ in the CsPbBr3 precursor molecules was favourable to enhancing the density of PQDs. The prepared PMMA-coated CsPbBr3 quantum dots (QDs) pattern had high stability and could maintain at 90.08% PL intensity after 1 week of exposure to air.

Solid polymer electrolyte-based atomic switches: from materials to mechanisms and applications.

As miniaturization of semiconductor memory devices is reaching its physical and technological limits, there is a demand for memory technologies that operate on new principles. Atomic switches are nanoionic devices that show repeatable resistive switching between high-resistance and low-resistance states under bias voltage applications, based on the transport of metal ions and redox reactions in solids. Their essential structure consists of an ion conductor sandwiched between electrochemically active and inert electrodes. This review focuses on the resistive switching mechanism of atomic switches that utilize a solid polymer electrolyte (SPE) as the ion conductor. Owing to the superior properties of polymer materials such as mechanical flexibility, compatibility with various substrates, and low fabrication costs, SPE-based atomic switches are a promising candidate for the next-generation of volatile and nonvolatile memories. Herein, we describe their operating mechanisms and key factors for controlling the device performance with different polymer matrices. In particular, the effects of moisture absorption in the polymer matrix on the resistive switching behavior are addressed in detail. As potential applications, atomic switches with inkjet-printed SPE and quantum conductance behavior are described. SPE-based atomic switches also have great potential in use for neuromorphic devices. The development of these devices will be enhanced using nanoarchitectonics concepts, which integrate functional materials and devices.

This article reviews a series of works starting with the author's 2011 paper on solid polymer electrolyte-based atomic switches, and describes the current status and future prospects for this technology.

Inkjet Printing Magnetostrictive Materials for Structural Health Monitoring of Carbon Fibre-Reinforced Polymer Composite.

Inkjet printing of magnetic materials has increased in recent years, as it has the potential to improve research in smart, functional materials. Magnetostriction is an inherent property of magnetic materials which allows strain or magnetic fields to be detected. This makes it very attractive for sensors in the area of structural health monitoring by detecting internal strains in carbon fibre-reinforced polymer (CFRP) composite. Inkjet printing offers design flexibility for these sensors to influence the magnetic response to the strain. This allows the sensor to be tailored to suit the location of defects in the CFRP. This research has looked into the viability of printable soft magnetic materials for structural health monitoring (SHM) of CFRP. Magnetite and nickel ink dispersions were selected to print using the JetLab 4 drop-on-demand technique. The printability of both inks was tested by selecting substrate, viscosity and solvent evaporation. Clogging was found to be an issue for both ink dispersions. Sonicating and adjusting the jetting parameters helped in distributing the nanoparticles. We found that magnetite nanoparticles were ideal as a sensor as there is more than double increase in saturation magnetisation by 49 Am2/kg and more than quadruple reduction of coercive field of 5.34 kA/m than nickel. The coil design was found to be the most sensitive to the field as a function of strain, where the gradient was around 80% higher than other sensor designs. Additive layering of 10, 20 and 30 layers of a magnetite square patch was investigated, and it was found that the 20-layered magnetite print had an improved field response to strain while maintaining excellent print resolution. SHM of CFRP was performed by inducing a strain via bending and it was found that the magnetite coil detected a change in field as the strain was applied.

The Role of Interdigitated Electrodes in Printed and Flexible Electronics.

Flexible electronics, also referred to as printable electronics, represent an interesting technology for implementing electronic circuits via depositing electronic devices onto flexible substrates, boosting their possible applications. Among all flexible electronics, interdigitated electrodes (IDEs) are currently being used for different sensor applications since they offer significant benefits beyond their functionality as capacitors, like the generation of high output voltage, fewer fabrication steps, convenience of application of sensitive coatings, material imaging capability and a potential of spectroscopy measurements via electrical excitation frequency variation. This review examines the role of IDEs in printed and flexible electronics since they are progressively being incorporated into a myriad of applications, envisaging that the growth pattern will continue in the next generations of flexible circuits to come.

Rheological Properties and Inkjet Printability of a Green Silver-Based Conductive Ink for Wearable Flexible Textile Antennas.

The development of e-textiles necessitates the creation of highly conductive inks that are compatible with precise inkjet printing, which remains a key challenge. This work presents an innovative, syringe-based method to optimize a novel bio-sourced silver ink for inkjet printing on textiles. We investigate the relationships between inks' composition, rheological properties, and printing behavior, ultimately assessing the electrical performance of the fabricated circuits. Using Na-alginate and polyethylene glycol (PEG) as the suspension matrix, we demonstrate their viscosity depends on the component ratios. Rheological control of the silver nanoparticle-laden ink has become paramount for uniform printing on textiles. A specific formulation (3 wt.% AgNPs, 20 wt.% Na-alginate, 40 wt.% PEG, and 40 wt.% solvent) exhibits the optimal rheology, enabling the printing of 0.1 mm thick conductive lines with a low resistivity (8 × 10-3 Ω/cm). Our findings pave the way for designing eco-friendly ink formulations that are suitable for inkjet printing flexible antennas and other electronic circuits onto textiles, opening up exciting possibilities for the next generation of E-textiles.

Inkjet-Printed Multiwalled Carbon Nanotube Dispersion as Wireless Passive Strain Sensor.

In this study, a multiwalled carbon nanotube (MWCNT) dispersion is used as an ink for a single-nozzle inkjet printing system to produce a planar coil that can be used to determine strain wirelessly. The MWCNT dispersion is non-covalently functionalized by dispersing the CNTs in an anionic surfactant, namely sodium dodecyl sulfate (SDS). The fabrication parameters, such as sonication energy and centrifugation time, are optimized to obtain an aqueous suspension suitable for an inkjet printer. Planar coils with different design parameters are printed on a flexible polyethylene terephthalate (PET) polymer substrate. The design parameters include a different number of windings, inner diameter, outer diameter, and deposited layers. The electrical impedance spectroscopy (EIS) analysis is employed to characterize the printed planar coils, and an equivalent electrical circuit model is derived based on the results. Additionally, the radio frequency identification technique is utilized to wirelessly investigate the read-out mechanism of the printed planar MWCNT coils. The complex impedance of the inductively coupled sensor undergoes a shift under strain, allowing for the monitoring of changes in resonance frequency and bandwidth (i.e., amplitude). The proposed wireless strain sensor exhibits a remarkable gauge factor of 22.5, which is nearly 15 times higher than that of the wireless strain sensors based on conventional metallic strain gauges. The high gauge factor of the proposed sensor suggests its high potential in a wide range of applications, such as structural health monitoring, wearable devices, and soft robotics.

Embedded Sensors with 3D Printing Technology: Review.

Embedded sensors (ESs) are used in smart materials to enable continuous and permanent measurements of their structural integrity, while sensing technology involves developing sensors, sensory systems, or smart materials that monitor a wide range of properties of materials. Incorporating 3D-printed sensors into hosting structures has grown in popularity because of improved assembly processes, reduced system complexity, and lower fabrication costs. 3D-printed sensors can be embedded into structures and attached to surfaces through two methods: attaching to surfaces or embedding in 3D-printed sensors. We discussed various additive manufacturing techniques for fabricating sensors in this review. We also discussed the many strategies for manufacturing sensors using additive manufacturing, as well as how sensors are integrated into the manufacturing process. The review also explained the fundamental mechanisms used in sensors and their applications. The study demonstrated that embedded 3D printing sensors facilitate the development of additive sensor materials for smart goods and the Internet of Things.

Two-Layer Inkjet-Printed Microwave Split-Ring Resonators for Detecting Analyte Binding to the Gold Surface.

This work focuses on demonstrating the working principle of inkjet-printed Au nanoparticle (NP) two-layer Gigahertz (2.6 GHz) microwave split-ring resonators (SRRs) as a novel platform for the detection of analytes on flexible substrates. In contrast to the standard fabrication of split-ring resonator biosensors using printed circuit board technology, which results in a seven-layer system, the resonators in this work were fabricated using a two-layer system. A ground plane is embedded in the SRR measurement setup. In this method, a microwave electromagnetic wave is coupled into the Au SRR via an inkjet-printed Cu-NP stripline that is photonically sintered. This coupling mechanism facilitates the detection of analytes by inducing resonance shifts in the SRR. In this study, the functionality of the printed sensors was demonstrated using two different Au functionalization processes, firstly, with HS-PEG7500-COOH, and, secondly, with protein G with an N-terminal cysteine residue. The sensing capabilities of the printed structures are shown by the attachment of biomolecules to the SRR and the measurement of the resulting resonance shift. The experiments show a clear shift of the resonance frequency in the range of 20-30 MHz for both approaches. These results demonstrate the functionality of the simplified printed two-layer microwave split-ring resonator for use as a biosensor.

Inkjet Printing of High-Color-Purity Blue Organic Light-Emitting Diodes with Host-Free Inks.

Inkjet printing technology offers a unique approach to producing direct-patterned pixels without fine metal masks for active matrix displays. Organic light-emitting diodes (OLEDs) consisting of thermally activated delayed fluorescence (TADF) emitters facilitate efficient light emission without heavy metals, such as platinum and iridium. Multi-resonance TADF molecules, characterized by their small full width at half maxima (FWHM), are highly suitable for the requirements of wide color-gamut displays. Herein, host-free TADF inks with a low concentration of 1 mg/mL were developed and inkjet-printed onto a seeding layer, concurrently serving as the hole-transporting layer. Attributed to the proof-of-concept of host-free inks printed on a mixed seeding layer, a maximum external quantum efficiency of 13.1% (improved by a factor of 21.8) was achieved in the inkjet-printed OLED, with a remarkably narrow FWHM of only 32 nm. Highly efficient energy transfer was facilitated by the effective dispersion of the sensitizer around the terminal emitters.

Nonpolar Solvent Modulated Inkjet Printing of Nanoparticle Self-Assembly Morphologies.

Patterning of luminescent nanomaterials is critical in the fields of display and information encryption, and inkjet printing technology have shown remarkable significance with the advantage of fast, large-scalable and integrative. However, inkjet printing nanoparticle deposits with high-resolution and well controlled morphology from nonpolar solvent droplets is still challenging. Herein, a facile approach of nonpolar solvent modulated inkjet printing of nanoparticles self-assembly patterns driven by the shrinkage of the droplet and inner solutal convection is proposed. Through regulating the solvent composition and nanoparticle concentration, multicolor light-emissive upconversion nanoparticle self-assembly microarrays with tunable morphologies are achieved, showing the integration of designable microscale morphologies and photoluminescences for multimodal anti-counterfeit. Furthermore, inkjet printing of nanoparticles self-assembled continuous lines with adjustable morphologies by controlling the coalescence and drying of the ink droplets is achieved. The high resolution of inkjet printing microarrays and continuous lines' width < 5 and 10 µm is realized, respectively. This nonpolar solvent-modulated inkjet printing of nanoparticle deposits approach facilitates the patterning and integration of different nanomaterials, and is expected to provide a versatile platform for fabricating advanced devices applied in photonics integration, micro-LED, and near-field display.

An Electroactive and Self-Assembling Bio-Ink, based on Protein-Stabilized Nanoclusters and Graphene, for the Manufacture of Fully Inkjet-Printed Paper-Based Analytical Devices.

Hundreds of new electrochemical sensors are reported in literature every year. However, only a few of them makes it to the market. Manufacturability, or rather the lack of it, is the parameter that dictates if new sensing technologies will remain forever in the laboratory in which they are conceived. Inkjet printing is a low-cost and versatile technique that can facilitate the transfer of nanomaterial-based sensors to the market. Herein, an electroactive and self-assembling inkjet-printable ink based on protein-nanomaterial composites and exfoliated graphene is reported. The consensus tetratricopeptide proteins (CTPRs), used to formulate this ink, are engineered to template and coordinate electroactive metallic nanoclusters (NCs), and to self-assemble upon drying, forming stable films. The authors demonstrate that, by incorporating graphene in the ink formulation, it is possible to dramatically improve the electrocatalytic properties of the ink, obtaining an efficient hybrid material for hydrogen peroxide (H2 O2 ) detection. Using this bio-ink, the authors manufactured disposable and environmentally sustainable electrochemical paper-based analytical devices (ePADs) to detect H2 O2 , outperforming commercial screen-printed platforms. Furthermore, it is demonstrated that oxidoreductase enzymes can be included in the formulation, to fully inkjet-print enzymatic amperometric biosensors ready to use.