Velocity and size measurement of droplets from an ultrasonic spray coater using photon correlation spectroscopy and turbidimetry.

We have developed a combination of light scattering techniques to study and characterize droplets of an ultrasonic spray coater in flight. For this economically relevant spray coater, there is so far no reliable technique to systematically adjust the experimental parameters. We have combined photon correlation spectroscopy and turbidimetry to determine the size and speed of the droplets depending on parameters of the printing process as shroud gas pressure, flow rate, and atomizing power. Our method will allow us to predetermine these parameters to control the properties of the coated films as, e.g., thickness from tens of nanometers to micrometers.

Links Between Heathland Fungal Biomass Mineralization, Melanization, and Hydrophobicity.

Comprehending the decomposition process is crucial for our understanding of the mechanisms of carbon (C) sequestration in soils. The decomposition of plant biomass has been extensively studied. It revealed that extrinsic biomass properties that restrict its access to decomposers influence decomposition more than intrinsic ones that are only related to its chemical structure. Fungal biomass has been much less investigated, even though it contributes to a large extent to soil organic matter, and is characterized by specific biochemical properties. In this study, we investigated the extent to which decomposition of heathland fungal biomass was affected by its hydrophobicity (extrinsic property) and melanin content (intrinsic property). We hypothesized that, as for plant biomass, hydrophobicity would have a greater impact on decomposition than melanin content. Mineralization was determined as the mineralization of soil organic carbon (SOC) into CO2 by headspace GC/MS after inoculation by a heathland soil microbial community. Results show that decomposition was not affected by hydrophobicity, but was negatively correlated with melanin content. We argue that it may indicate that either melanin content is both an intrinsic and extrinsic property, or that some soil decomposers evolved the ability to use surfactants to access to hydrophobic biomass. In the latter case, biomass hydrophobicity should not be considered as a crucial extrinsic factor. We also explored the ecology of decomposition, melanin content, and hydrophobicity, among heathland soil fungal guilds. Ascomycete black yeasts had the highest melanin content, and hyaline Basidiomycete yeasts the lowest. Hydrophobicity was an all-or-nothing trait, with most isolates being hydrophobic.

Diels-Alder Network Blends as Self-Healing Encapsulants for Liquid Metal-Based Stretchable Electronics.

Two dynamic covalent networks based on the Diels-Alder reaction were blended to exploit the properties of the dissimilar polymer backbones. Furan-functionalized polyether amines based on poly(propylene oxide) (PPO) FD4000 and polydimethylsiloxane (PDMS) FS5000 were mixed in a common solvent and reversibly cross-linked with the same bismaleimide DPBM. The morphology of the phase-separated blends is primarily controlled by the concentration of backbones. Increasing the PDMS content of the blends results in a dilute droplet morphology at 25 wt %, with a growing size and concentration of droplets and the formation of two separate PPO- and PDMS-rich layers at 50 wt %. Further increasing the PDMS content to 75 wt % leads to larger droplets and a thicker layer of the secondary phase. The hydrophobic PDMS phase creates a barrier against water, while the more hydrophilic PPO phase enhances the resistance against oxygen diffusion. Lowering the maleimide-to-furan stoichiometric ratio resulted in a decrease in cross-link density and thus more flexible and stretchable encapsulants. Changes in the stoichiometric ratio also affected the phase morphology due to resulting changes in phase separation and network formation kinetics. Lowering the stoichiometric ratio also resulted in enhanced self-healing properties of 96% at room temperature as a consequence of the increased chain mobility in the blended networks. The self-healing blends were used to encapsulate liquid metal circuits to create stretchable strain sensors with a linear electro-mechanical response without much drift or hysteresis, which could be efficiently recovered by 90% after the damage-healing cycles.

The Influence of UV-Ozone, O2 Plasma, and CF4 Plasma Treatment on the Droplet-Based Deposition of Diamond Nanoparticles.

Surface treatment is critical for homogeneous coating over a large area and high-resolution patterning of nanodiamond (ND) particles. To optimize the interaction between the surface of a substrate and the colloid of ND particles, it is essential to remove hydrocarbon contamination by surface treatment and to increase the surface energy of the substrate, hence improving the diamond film homogeneity upon its deposition. However, the impact of substrate surface treatment on the properties of coatings and patterns is not fully understood. This study explores the impact of UV-ozone, O2 plasma, and CF4 plasma treatments on the wetting properties of the fused silica glass substrate surface. We identify the optimal time interval between the treatment and subsequent ND coating/patterning processes, which were conducted using inkjet printing and ultrasonic spray coating techniques. Our results showed that UV-ozone and O2 plasma resulted in hydrophilic surfaces, while CF4 plasma treatment resulted in hydrophobic surfaces. We demonstrate the use of CF4 plasma treatment before inkjet printing to generate high-resolution patterns with dots as small as 30 µm in diameter. Ultrasonic spray coating showed homogeneous coatings after using UV-ozone and O2 plasma treatment. The findings of this study provide valuable insights into the hydrocarbon airborne contamination on cleaned surfaces over time even in clean-room environments and have a notable impact on the performance of liquid coatings and patterns. We highlight the importance of timing between the surface treatment and printing in achieving high resolution or homogeneity.

Plasmon enhanced fluorescence from meticulously positioned gold nanoparticles, deposited by ultra sonic spray coating on organic light emitting diodes.

Enhancement of the spontaneous emission of fluorophores aided by plasmonic nanoparticles (PNPs) prompts the growth of plasmonic organic light emitting diodes (OLEDs). Together with the spatial dependence of the fluorophore and PNPs on enhanced fluorescence, the surface coverage of the PNPs controls the charge transport in OLEDs. Hence, here, the spatial and surface coverage reliance of plasmonic gold nanoparticles is controlled by a roll-to-roll compatible ultrasonic spray coating technique. A 2-fold enhancement in the multi photon fluorescence is seen by two-photon fluorescence microscopy for a polystyrene sulfonate (PSS) stabilized gold nanoparticle located 10 nm away from the super yellow fluorophore. Fluorescence enhancement combined with ∼2% surface coverage of PNPs, provides a 33%, 20% and ∼40% increase in the electroluminescence, luminous efficacy and external quantum efficiency, respectively.

Stretchable printed device for the simultaneous sensing of temperature and strain validated in a mouse wound healing model.

Temperature and strain are two vital parameters that play a significant role in wound diagnosis and healing. As periodic temperature measurements with a custom thermometer or strain measurements with conventional metallic gauges became less feasible for the modern competent health monitoring, individual temperature and strain measurement modalities incorporated into wearables and patches were developed. The proposed research in the article shows the development of a single sensor solution which can simultaneously measure both the above mentioned parameters. This work integrates a thermoelectric principle based temperature measurement approach into wearables, ensuring flexibility and bendability properties without affecting its thermo-generated voltage. The modified thermoelectric material helped to achieve stretchability of the sensor, thanks to its superior mechano-transduction properties. Moreover, the stretch-induced resistance changes become an additional marker for strain measurements so that both the parameters can be measured with the same sensor. Due to the independent measurement parameters (open circuit voltage and sensor resistance), the sensing model is greatly attractive for measurements without cross-sensitivity. The highly resilient temperature and strain sensor show excellent linearity, repeatability and good sensitivity. Besides, due to the compatibility of the fabrication scheme to low-temperature processing of the flexible materials and to mass volume production, printed fabrication methodologies were adopted to realize the sensor. This promises low-cost production and a disposable nature (single use) of the sensor patch. For the first time, this innovative temperature-strain dual parameter sensor concept has been tested on mice wounds in vivo. The preliminary experiments on mice wounds offer prospects for developing smart, i.e. sensorized, wound dressings for clinical applications.

Biocompatibility Testing of Liquid Metal as an Interconnection Material for Flexible Implant Technology.

Galinstan, a liquid metal at room temperature, is a promising material for use in flexible electronics. Since it has been successfully integrated in devices for external use, e.g., as stretchable electronic skin in tactile sensation, the possibility of using galinstan for flexible implant technology comes to mind. Usage of liquid metals in a flexible implant would reduce the risk of broken conductive pathways in the implants and therefore reduce the possibility of implant failure. However, the biocompatibility of the liquid metal under study, i.e., galinstan, has not been proven in state-of-the-art literature. Therefore, in this paper, a material combination of galinstan and silicone rubber is under investigation regarding the success of sterilization methods and to establish biocompatibility testing for an in vivo application. First cell biocompatibility tests (WST-1 assays) and cell toxicity tests (LDH assays) show promising results regarding biocompatibility. This work paves the way towards the successful integration of stretchable devices using liquid metals embedded in a silicone rubber encapsulant for flexible surface electro-cortical grid arrays and other flexible implants.

Oxygen Gas and UV Barrier Properties of Nano-ZnO-Coated PET and PHBHHx Materials Fabricated by Ultrasonic Spray-Coating Technique.

Ultrasonic spray-coating (USSC)-a wet chemical deposition method to deposit ultrathin (down to 20 nm) coatings-is being applied as a promising alternative deposition method for functional coatings due to an economical, simple, and precise coating process with easy control over its operating parameters. In this research, zinc oxide nanoparticles (ZnO NPs) were ultrasonically spray-coated on commercial-grade polyethylene terephthalate (PET) and poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBHHx) films. The most suitable parameters for the ink composition, the ultrasonic spray-coating process, and the number of coating passes (up to 50×) were selected on the basis of a series of experiments. The oxygen gas barrier properties in terms of the oxygen transmission rate (OTR) of neat PET, and 3×, 5×, 10×, and 50× ZnO NP-coated PET and PHBHHx substrates were investigated. The OTR values for neat PET, and 3×, 5×, and 10× ZnO NP-coated PET substrates were found to be the same; however, a 5% reduction in OTR for 50× ZnO NP-coated PET substrate was observed compared to the neat PET substrate. No reduction in OTR was found for any above number of coating passes on PHBHHx substrates against the neat PHBHHx substrate. However, the ultraviolet (UV) tests of 3×, 5×, and 10× ZnO NP-coated PET and PHBHH× substrates revealed a significant decrease in percentage transmission for 10× coated PET and PHBHHx substrates as compared to their 3× and 5× ZnO NP-coated substrates, respectively. It was revealed from the study that the 50× ZnO NP coating of the PET substrate created a slight difference in OTR as compared to the reference substrate. However, the ultrasonic spray-coating method created a significant UV barrier effect for 3×, 5×, and 10× ZnO NP-coated PET and PHBHHx substrates, which demonstrates that the optimized coating method cannot be used to create a high oxygen barrier but can certainly be applied for UV barrier applications in food packaging. It is concluded that ultrasonic spray deposition of ZnO NPs on PET and PHBHHx materials has shown promising results for UV barrier properties, demonstrating the advantages of using this method compared to other coating methods with regard to cost-effectiveness, precise coating, and better process control.

Monitoring Body Fluids in Textiles: Combining Impedance and Thermal Principles in a Printed, Wearable, and Washable Sensor.

This work explores the feasibility of coupling two different techniques, the impedance and the transient plane source (TPS) principle, to quantify the moisture content and its compositional parameters simultaneously. The sensor is realized directly on textiles with the use of printing and coating technology. Impedance measurements use the fluid's electrical properties, while the TPS measurements are based on the thermal effusivity of the liquid. Impedance and TPS measurements show equal competency in measuring the fluid volume with a lowest measurable quantity of 0.5 µL, enabling ultralow volume passive measurements for sweat analysis. Both sensor principles were tested by monitoring the drying of a wet cloth and the measurements show perfect repeatability and accuracy. Nevertheless, when the biofluid property changes, the TPS sensor does not reflect this information on its readings, whereas, on the other hand, impedance can provide information on compositional changes. However, since the volume of the fluid changes simultaneously, one cannot differentiate between a volume change and a compositional change from impedance measurements alone. Therefore, we show in this work that we can apply impedance to measure the compositional properties; meanwhile, the TPS measurements accurately carry out volume measurements irrespective of the interferences from its compositional variations. To prove this, both of these techniques are applied for the quantification and composition monitoring of sweat, showing the capability to measure moisture content and compositional parameters simultaneously. TPS measurements can also be an indicator of the local temperature of the medium confined by the sensor, and it does not influence the fluid parameters. Compiling both impedance and thermal sensors in a single platform triggers smart wearable prospects of metering the liquid volume and simultaneously analyzing other compositional changes and body temperature. Finally, the repeatability and stability of the sensor readings and the washability of the device are tested. This device could be a potential sensing tool in real-life applications, such as wound monitoring and sweat analysis, and could be a promising addition toward future smart wearable sensors.

Screen Printed Antennas on Fiber-Based Substrates for Sustainable HF RFID Assisted E-Fulfilment Smart Packaging.

Intelligent packaging is an emerging technology, aiming to improve the standard communication function of packaging. Radio frequency identification (RFID) assisted smart packaging is of high interest, but the uptake is limited as the market needs cost-efficient and sustainable applications. The integration of screen printed antennas and RFID chips as smart labels in reusable cardboard packaging could offer a solution. Although paper is an interesting and recyclable material, printing on this substrate is challenging as the ink conductivity is highly influenced by the paper properties. In this study, the best paper/functional silver ink combinations were first selected out of 76 paper substrates based on the paper surface roughness, air permeance, sheet resistance and SEM characterization. Next, a flexible high frequency RFID chip (13.56 MHz) was connected on top of screen printed antennas with a conductive adhesive. Functional RFID labels were integrated in cardboard packaging and its potential application as reusable smart box for third party logistics was tested. In parallel, a web-based software application mimicking its functional abilities in the logistic cycle was developed. This multidisciplinary approach to developing an easy-scalable screen printed antenna and RFID-assisted smart packaging application is a good example for future implementation of hybrid electronics in sustainable smart packaging.

Influence of Polymer Concentration and Nozzle Material on Centrifugal Fiber Spinning.

Centrifugal fiber spinning has recently emerged as a highly promising alternative technique for the production of nonwoven, ultrafine fiber mats. Due to its high production rate, it could provide a more technologically relevant fiber spinning technique than electrospinning. In this contribution, we examine the influence of polymer concentration and nozzle material on the centrifugal spinning process and the fiber morphology. We find that increasing the polymer concentration transforms the process from a beaded-fiber regime to a continuous-fiber regime. Furthermore, we find that not only fiber diameter is strongly concentration-dependent, but also the nozzle material plays a significant role, especially in the continuous-fiber regime. This was evaluated by the use of a polytetrafluoroethylene (PTFE) and an aluminum nozzle. We discuss the influence of polymer concentration on fiber morphology and show that the choice of nozzle material has a significant influence on the fiber diameter.

Layer Morphology and Ink Compatibility of Silver Nanoparticle Inkjet Inks for Near-Infrared Sintering.

The field of printed electronics is rapidly evolving, producing low cost applications with enhanced performances with transparent, stretchable properties and higher reliability. Due to the versatility of printed electronics, industry can consider the implementation of electronics in a way which was never possible before. However, a post-processing step to achieve conductive structures-known as sintering-limits the production ease and speed of printed electronics. This study addresses the issues related to fast sintering without scarifying important properties such as conductivity and surface roughness. A drop-on-demand inkjet printer is employed to deposit silver nanoparticle-based inks. The post-processing time of these inks is reduced by replacing the conventional oven sintering procedure with the state-of-the-art method, named near-infrared sintering. By doing so, the post-processing time shortens from 30-60 min to 6-8 s. Furthermore, the maximum substrate temperature during sintering is reduced from 200 °C to 120 °C. Based on the results of this study, one can conclude that near-infrared sintering is a ready-to-industrialize post-processing method for the production of printed electronics, capable of sintering inks at high speed, low temperature and with low complexity. Furthermore, it becomes clear that ink optimization plays an important role in processing inkjet printable inks, especially after being near-infrared sintered.

Inkjet Printing of PEDOT:PSS Based Conductive Patterns for 3D Forming Applications.

This paper presents the formulation, inkjet printing, and vacuum forming of a conductive and stretchable polymer, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), ink on a stretchable and transparent thermoplastic polyurethane (TPU) substrate. The formulation of the conductive and stretchable ink is achieved by combining PEDOT:PSS with additional solvents, to achieve the right inkjet properties for drop-on-demand (DoD) inkjet printing. A conductive pattern can be printed from the 21 µm orifice on a flexible and stretchable TPU substrate, with a linewidth down to 44 µm. The properties of the printed pattern, in terms of sheet resistance, morphology, transparency, impact of weather conditions, and stretching are investigated and show sheet resistances up to 45 Ohm/sq and transparencies as high as 95%, which is comparable to indium tin oxide (ITO). Moreover, in contrast to ITO, one-time stretching up to 40% can be achieved, increasing the sheet resistance up to 214 Ohm/sq only, showing the great potential of this ink for one-time stretching. Finally, as a proof of this one-time stretching, the printed samples are vacuum formed around a 3D object, still showing sufficient conductivity to be applied as a capacitive touch sensor.

(Bio)polymer/ZnO Nanocomposites for Packaging Applications: A Review of Gas Barrier and Mechanical Properties.

Nanotechnology is playing a pivotal role in improving quality of life due to its versatile applications in many areas of research. In this regard, nanoparticles have gained significant importance. Zinc oxide nanoparticles (ZnO NPs) amongst other nanoparticles are being used in producing nanocomposites. Methods like solvent casting, solution casting, solvent volatilization, twin-screw extrusion, melt compounding and extrusion blow molding have been applied to produce ZnO NPs based (bio)polymer composites. These composites are of great interest in the research area of food packaging materials due to their improved multifunctional characteristics like their mechanical, barrier and antimicrobial properties. This paper gives an overview of the main methods to synthesize ZnO NPs, methods to incorporate ZnO NPs in (bio)polymers, and finally, the gas barrier and mechanical properties of the nanocomposites. As a conclusion, a maximum decline in oxygen, carbon dioxide and water vapor permeability was reported as 66%, 17% and 38% respectively, while tensile strength and young's modulus were observed to increase by 32% and 57% respectively, for different (bio)polymer/ZnO nanocomposites.

Charge-Discharge Characteristics of Textile Energy Storage Devices Having Different PEDOT:PSS Ratios and Conductive Yarns Configuration.

Conductive polymer PEDOT:PSS, sandwiched between two conductive yarns, has been proven to have capacitive behavior in our textile energy storage devices. Full understanding of its underlying mechanism is still intriguing. The effect of the PEDOT to PSS ratio and the configuration of the electrode yarns are the focus of this study. Three commercial PEDOT:PSS yarns, Clevios P-VP-AI-4083, Ossila AI 4083, and Orgacon ICP 1050, as well as stainless steel and silver-coated polybenzoxazole (Ag/PBO) yarns, in various combinations, were used as solid electrolytes and electrodes, respectively. Analyses with NMR, ICP-OES, TGA, and resistivity measurement were employed to characterize the PEDOT:PSS. The device charge-discharge performance was measured by the Arduino microcontroller. Clevios and Ossila were found to have identical characteristics with a similar ratio, that is, 1:5.26, hence a higher resistivity of 1000 Ω.cm, while Orgacon had a lower PEDOT to PSS ratio, that is, 1:4.65, with a lower resistivity of 0.25⁻1 Ω.cm. The thermal stability of PEDOT:PSS up to 250 °C was proven. Devices with PEDOT:PSS having lower conductivity, such as Clevios P-VP-AI-4083 or Ossila AI 4083, showed capacitive behavior. For a better charge-discharge profile, it is also suggested that the PEDOT to electrode resistance should be low. These results led to a conclusion that a larger ratio of PEDOT to PSS, having higher resistivity, is more desirable, but further research is needed.

Fabrication Approaches to Interconnect Based Devices for Stretchable Electronics: A Review.

Stretchable electronics promise to naturalize the way that we are surrounded by and interact with our devices. Sensors that can stretch and bend furthermore have become increasingly relevant as the technology behind them matures rapidly from lab-based workflows to industrially applicable production principles. Regardless of the specific materials used, creating stretchable conductors involves either the implementation of strain reliefs through insightful geometric patterning, the dispersion of stiff conductive filler in an elastomeric matrix, or the employment of intrinsically stretchable conductive materials. These basic principles however have spawned a myriad of materials systems wherein future application engineers need to find their way. This paper reports a literature study on the spectrum of different approaches towards stretchable electronics, discusses standardization of characteristic tests together with their reports and estimates matureness for industry. Patterned copper foils that are embedded in elastomeric sheets, which are closest to conventional electronic circuits processing, make up one end of the spectrum. Furthest from industry are the more recent circuits based on intrinsically stretchable liquid metals. These show extremely promising results, however, as a technology, liquid metal is not mature enough to be adapted. Printing makes up the transition between both ends, and is also well established on an industrial level, but traditionally not linked to creating electronics. Even though a certain level of maturity was found amongst the approaches that are reviewed herein, industrial adaptation for consumer electronics remains unpredictable without a designated break-through commercial application.

Printing Smart Designs of Light Emitting Devices with Maintained Textile Properties.

To maintain typical textile properties, smart designs of light emitting devices are printed directly onto textile substrates. A first approach shows improved designs for alternating current powder electroluminescence (ACPEL) devices. A configuration with the following build-up, starting from the textile substrate, was applied using the screen printing technique: silver (10 µm)/barium titanate (10 µm)/zinc-oxide (10 µm) and poly(3,4-ethylenedioxythiophene)poly(styrenesulfonate) (10 µm). Textile properties such as flexibility, drapability and air permeability are preserved by implementing a pixel-like design of the printed layers. Another route is the application of organic light emitting devices (OLEDs) fabricated out of following layers, also starting from the textile substrate: polyurethane or acrylate (10-20 µm) as smoothing layer/silver (200 nm)/poly(3,4-ethylenedioxythiophene)poly(styrenesulfonate) (35 nm)/super yellow (80 nm)/calcium/aluminum (12/17 nm). Their very thin nm-range layer thickness, preserving the flexibility and drapability of the substrate, and their low working voltage, makes these devices the possible future in light-emitting wearables.

Steering the Properties of MoOx Hole Transporting Layers in OPVs and OLEDs: Interface Morphology vs. Electronic Structure.

The identification, fine-tuning, and process optimization of appropriate hole transporting layers (HTLs) for organic solar cells is indispensable for the production of efficient and sustainable functional devices. In this study, the optimization of a solution-processed molybdenum oxide (MoOx) layer fabricated from a combustion precursor is carried out via the introduction of zirconium and tin additives. The evaluation of the output characteristics of both organic photovoltaic (OPV) and organic light emitting diode (OLED) devices demonstrates the beneficial influence upon the addition of the Zr and Sn ions compared to the generic MoOx precursor. A dopant effect in which the heteroatoms and the molybdenum oxide form a chemical identity with fundamentally different structural properties could not be observed, as the additives do not affect the molybdenum oxide composition or electronic band structure. An improved surface roughness due to a reduced crystallinity was found to be a key parameter leading to the superior performance of the devices employing modified HTLs.