Lateral flow biosensors are analytical devices that detect biomaterials with physicochemical signals, such as optical signals. Unlike other biosensors, lateral flow biosensors are based on porous membranes, which use capillary force to transport biomaterials spontaneously. However, lateral flow biosensors are fabricated in batch mode, which means that membranes need to be cut from the rolls, pretreated, and assembled using a step-by-step process. Thus, there is a need for a more efficient manufacturing process. This thesis aims to accelerate the fabrication process by developing a method wherein the whole device is printed directly, including the printable substrates, as well as by developing a clog-free process for depositing expensive reagents. These novel printable porous media were developed using printing inks that contained various pigments and polymer binders. To this end, candidate formulations were screened from nine hundred inks formulations via wicking experiments. The results of these tests showed that the most promising formulations were based on calcium carbonates and latex polymers. This formulation was then used to develop printable porous media that can easily be printed into complex patterns, with changeable wicking speeds within each pattern. In addition, a bio- colorimetric assay of alkaline phosphates conducted on these porous media showed strong color signals that were comparable to the traditional membrane-based lateral flow strips. Clog-free printing processes were investigated by using a piezoelectric inkjet printer to print silica sols and six nanoparticle inks. The results of these tests showed that the vibration of the piezoelectric layer and the deposition of particles on the printhead surfaces induced clogging issues. Over time, the silica sols formed multilayer deposits on the print head surface, which subsequently detached due to the vibration of the piezoelectric layer. Consequently, these large sheets of silica clogged the nozzles during printing. This clogging issue was eliminated by adjusting the pH value of the silica sol inks to 3.1. The hydrophobic cationic polystyrene nanoparticles form a sub-monolayer on the printhead surface, which causes air entrainment and promotes air bubble adhesion into the interior of the print head surface when the piezoelectric layer deforms. Thus, alternate surface chemistries for the print head and ink particle surfaces may be required in order to print hydrophobic ink materials. Overall, this enhanced understanding of these clogging mechanisms helps to explain why printer performance varies when different particles are used. / Thesis / Doctor of Philosophy (PhD) / Many devices in our day-to-day lives incorporate lateral flow biosensors, for example, home pregnancy test kits. These tests allow users to obtain results within 30 minutes by simply applying a few droplets of urine onto a test strip. However, these biosensors are largely manufactured using manual processes: workers cut strips (also called substrates) from sheets, deposit reagents onto the strips, and then assemble the pretreated strips into devices. As such, these processes are time consuming and less productive. To accelerate the manufacturing process, we developed printable porous substrates and a clog-free printing process for depositing expensive reagents onto the substrates. Novel porous media can be flexibly printed into complex patterns using pigment- based inks. Moreover, the use of different pigments within the designed patterns enables these porous media to control wicking velocity. In addition to printable porous substrates, the research in this thesis shows that the manufacturing process can be improved by using piezoelectric inkjet printers. The use of these printers not only allows the expensive reagents to be precisely deposited onto the substrates, but it also offers a more cost-effective method of doing so. Finally, in order to ensure the printing process remained clog-free, we systematically investigated clogging mechanisms by printing with different polymers and nanoparticles.

<div>This thesis includes two parts. The main part is on the topic of conductivity prediction for Inkjet printed silver electrodes. The second part is about the follow-up work of toner usage prediction of laser electro-photographic printers. </div><div><br></div><div>For conductivity prediction of Inkjet printed silver electrodes part, the brief introduction is described below. Recently, electronic devices made with Inkjet printing technique and flexible thin films have attracted great attention due to their potential applications in sensor manufacturing. This imaging system has become a great tool to monitor the quality of Inkjet printed electrodes due to the fact that most thickness or resistance measuring devices can destroy the surface of a printed electrode or even whole electrode. Thus, a non-contact image-based approach to estimate sheet resistance of Inkjet printed electrodes is developed.</div><div><br></div><div>The approach has two stages. Firstly, strip-shaped electrodes are systematically printed with various printing parameters. The sheet resistance measurement data as</div><div>well as images of the electrodes are acquired. Then, based on the real experimental data, the fitting model is constructed and further used in predicting the sheet</div><div>resistance of the Inkjet printed silver electrodes.</div><div><br></div><div>For toner usage prediction part, the introduction is described below. With the widespread use of laser electro-photographic printers in both industry and households fields, estimation of toner usage has great significance to ensuring the full utilization of each cartridge. The follow-up work is focused on testing and improving feasibility, reliability, and adaptability of the Black Box Model (BBM) based two-stage strategy in estimating the toner usage. Comparing with previous methods, the training process for the firrst stage requires less time and disk storage, all while maintaining high accuracy. For the second stage, experiments are performed on various models of printers, with cyan(C), magenta(M), yellow(Y), and black(K) color cartridges.</div>

Os novos processos de impressão têm exigido novas características do papel. Entre os novos processos encontram-se as impressões digitais, em especial, a impressão por jato de tinta. Este tipo de impressão é baseado na ejeção de uma gota de tinta por um orifício em uma cabeça de impressão, que atinge o substrato formando um pixel. A definição das imagens formadas neste tipo de impressão é, portanto, dependente das características da tinta e, principalmente, do substrato. O presente trabalho tem por objetivo caracterizar as propriedades do papel que são importantes para a impressão por jato de tinta, desde o momento em que a tinta atinge a superfície do papel até a sua absorção. As propriedades consideradas neste estudo foram: a rugosidade, a porosidade e as propriedades químicas da superfície. A rugosidade foi avaliada pelos métodos tradicionais da área de papel e celulose (baseados em vazão de ar), por método perfilométrico e, qualitativamente, por imagens obtidas por microscopia eletrônica de varredura (MEV). Para a porosidade foi utilizado um método tradicional, além de porosimetria de intrusão de mercúrio e microtomografia de raios X, e a composição química da superfície foi avaliada por espectroscopia por energia dispersiva (EDS) e espectroscopia Raman. A partir dos resultados obtidos, as propriedades do papel foram qualificadas e as suas influências no espalhamento e absorção de líquidos em geral foram identificadas. Além da caracterização das propriedades superficiais e porosimétricas do papel, as correlações entre as propriedades e os diferentes métodos utilizados na sua determinação foram discutidas. Os métodos de análise tradicional não conseguem caracterizar os papéis em níveis de resolução capazes de fornecer informações sobre a influência das propriedades estudadas na impressão por jato de tinta. Ao mesmo tempo, a caracterização do papel para este tipo de impressão e a compreensão das influências das propriedades do papel no espalhamento e absorção de tinta e líquidos em geral só é possível quando as propriedades são analisadas em conjunto. / The new printing processes have required new features of the paper. Among the new printing processes are the digital printing, in particular, the inkjet printing. This type of printing is based on the ejection of an ink drop through a hole in a print head, which reaches the substrate forming a pixel. The resolution of the images formed in this type of printing is therefore dependent on the characteristics of the ink, and especially of the substrate. The present work aims to characterize the properties of paper that are important to the inkjet printing, from the moment the ink hits the paper surface to its absorption. The properties considered in this study were: roughness, porosity and chemical properties of the surface. The roughness was evaluated by traditional methods in pulp and paper sector (based on air flow), by profilometry and qualitative using images obtained by scanning electron microscopy (SEM). For the porosity, a traditional method was used, and also mercury intrusion porosimetry and X-ray microtomography. The chemical composition of the surface was evaluated by energy dispersive spectroscopy (EDS) and Raman spectroscopy. From the results obtained, the paper properties were described and their influence on the spreading and absorption of liquids in general have been identified. Besides the characterization of the paper surface properties and porosity, the correlations between the properties and the different methods used for measurement were discussed. The traditional analysis methods can not characterize the paper in levels of resolution capable of providing information about the influence of the properties studied in inkjet printing. At the same time, to characterize paper for this printing process and to understand the influences of the paper properties on the spreading and absorption of inks and liquids in general the paper properties have to be analyzed together.

Over the last decade, two dimensional (2D) materials have attracted considerable attention from both the scientific and engineering community due to their unique properties. One important advance of 2D materials is that they can be exfoliated into nanosheets suspended in a liquid phase and that this allows the formulation of 2D nanomaterials inks. Such inks can be deposited as functional components through low-cost inkjet printing techniques. Many 2D materials based inks have been produced over the years. This thesis investigates the use of inkjet printing to deposit 2D materials such as graphene oxide (GO) and black phosphorus (BP).GO, a derivative of graphene, has been widely used to produce graphene-based conductors via inkjet printing owing to its good stability in readily available solvents such as water. In this work, highly conductive reduced graphene oxide (rGO) films with bulk conductivity in excess of 2 × 10^4 Sm-1 have been prepared by inkjet printing a GO aqueous ink, with mean flake size 35.9 micro metre, through a 60 micro metre inkjet printing nozzle followed by a reduction step. Experimental results showed that individual GO flakes up to 200 micro metre diameter can be successfully printed with no instances of nozzle blocking or poor printing performance. The mechanism by which this occurs is believed to be GO sheet folding during drop formation followed by elastic unfolding during drop impact and spreading. In addition, the influence of GO flake size on rGO film conductivity has been investigated. It was found that the rGO film conductivity increased about 60% when the mean flake size of the GO flakes in the ink increases from 0.68 micro metre to 35.9 micro metre. The drying behaviour of printed GO droplets has been studied on eight GO aqueous inks in which the mean flake size of GO was varied over a range from 0.68 to 35.9 micro metre. It was found that the coffee ring effect (inhomogeneous drying of a droplet to leave a ring like deposit) of dried droplets of the GO ink weakened and disappeared when the flake size increasing. It was found that, with a printed deposit around 340 micro metre in diameter, the coffee ring effect (CRE) was suppressed with the mean flake size > 10.3 micro metre. The critical flake size for CRE suppression reduced to 5.97 and 3.68 micro metre when the substrate temperature was 40 and 50 °C, respectively. It was further found that the CRE weakened with decreasing printed drop size, with the critical flake size reducing to 1.58 micro metre with a printed drop diameter of 30 micro metre.The interaction between BP nanometre thickness flakes and humid atmospheres was investigated using an inkjet printed BP sensor. The BP sensor showed was very sensitive to changes in humidity with a response time of a few seconds and the effect is reproducible in minutes. However, long term exposure to humid air with a relative humidity (RH) > 11% leads to a significant chemical change in the BP films, with Fourier transform infra-red spectroscopy (FTIR) indicating partial hydrolysis of the BP to form phosphate and phosphonate ions. Low temperature heat treatment of BP films under dry conditions after exposure to elevated RH leads to a partial recovery of the impedance response and reversion to a chemical state similar to that before exposure to a humid environment. The recovery of BP properties is most complete after exposure to lower humidity environments (RH < 11%), although exact replication of the original impedance response and FTIR spectrum was not possible.

This thesis presents the development of all-inkjet-printed low-voltage organic thin-film transistors. Organic thin-film transistors (OTFTs), taking advantage of low-temperature printability, mechanical flexibility, and multi-functionality, are promising for a wide range of emerging applications such as wearable electronics. Printed OTFTs provide great benefits in fabrication cost reduction, but they need a very high operating voltage and exhibit severe instability during storage and operation in ambient environment. In this study, all-inkjet-printed OTFTs with a low operating voltage of less than 3 V are demonstrated through reducing trap density in the fabricated devices. The transistors use 6,13-bis(triisopropylsilylethynyl)pentacene as the semiconductor, poly(4-vinylphenol) as the dielectric, silver as the electrodes, and CYTOP as the encapsulation. Several aspects of physical and chemical properties of polymer dielectrics are studied to achieve this goal, including cross-linking, wetting, and moisture affinity. Through the careful selection of device architecture and control of the inkjet-printing processes, the semiconductor-dielectric interface trap density of the fabricated OTFTs is significantly reduced. The applicability of this approach to different materials is also investigated and confirmed, including polyvinyl cinnamate as the dielectric, 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene as the semiconductor, and anisole as the solvent for semiconductor inks. Based on the investigation of different materials, the characteristics and parameters of all-inkjet-printed OTFTs are optimised, demonstrating an ultra-steep subthreshold of 60.2 mV/decade approaching the theoretical limit and a low operating voltage of 1 V. In order to explore their feasibility in real-world applications, the stability of all-inkjet-printed OTFTs is investigated and the factors of instability are analysed. Based on these findings, the stability of the fabricated device is improved, such that the threshold voltage shift is less than 0.1 V in ambient environment storage for 3 months and operation for 1 hour. The electrical characteristics of OTFTs in the subthreshold regime are studied for analogue circuit design. Based on the developed low-voltage stable transistors, an ultra-low-power (< 1 nW) high-gain (> 200 V/V) amplifier is presented and utilised to detect electrophysiological signals from the human body.

abstract: Reactive inkjet printing (RIJP) is a direct-write deposition technique that synthesizes and patterns functional materials simultaneously. It is a route to cheap fabrication of highly conductive features on a versatile range of substrates. Silver reactive inks have become a staple of conductive inkjet printing for application in printed and flexible electronics, photovoltaic metallization, and more. However, the high cost of silver makes these less effective for disposable and low-cost applications. This work aimed to develop a particle-free formulation for a nickel reactive ink capable of metallizing highly pure nickel at temperatures under 100 °C to facilitate printing on substrates like paper or plastic. Nickel offers a significantly cheaper alternative to silver at slightly reduced bulk conductivity. To meet these aims, three archetypes of inks were formulated. First were a set of glycerol-based inks temperature ink containing nickel acetate, hydrazine, and ammonia in a mixture of water and glycerol. This ink reduced between 115 – 200 °C to produce slightly oxidized deposits of nickel with carbon content around 10 wt %. The high temperature was addressed in a second series, which replaced glycerol with lower boiling glycols and added sodium hydroxide as a strong base to enhance thermodynamics and kinetics of reduction. These inks reduced between 60 and 100 °C but sodium salts contaminated the final deposits. In a third set of inks, sodium hydroxide was replaced with tetramethylammonium hydroxide (TMAH), a strong organic base, to address contamination. These inks also reduced between 60 and 100 °C. Pipetting or printing onto gold coated substrates produce metallic flakes coated in a clear, thick residue. EDS measured carbon and oxygen content up to 70 wt % of deposits. The residue was hypothesized to be a non-volatile byproduct of TMAH and acetate. Recommendations are provided to address the residue. Ultimately the formulated reactive inks did not meet design targets. However, this thesis sets the framework to design an optimal nickel reactive ink in future work. / Dissertation/Thesis / Masters Thesis Chemical Engineering 2019

<p>Linköpings Universitet och Acreo AB i Norrköping bedriver ett forskningssamarbete rörande organisk elektrokemisk elektronik och det man kallar papperselektronik. Målet på Acreo är att kunna trycka denna typ av elektronik med snabba trycktekniker så som offset- eller flexotryck. Idag görs de flesta demonstratorer och prototyper, baserade på denna typ av elektrokemisk elektronik, med manuella och subtraktiva mönstringsmetoder. Det skulle vara intressant att hitta fler verktyg och automatiserade tekniker som kan underlätta detta arbete. Målet med detta examensarbete har varit att utvärdera vilken potential bläckstråleteknik respektive screentryck har som tillverkningsmetoder för organiska elektrokemiska elektroniksystem samt att jämföra de båda teknikernas för- och nackdelar. Vad gäller bläckstråletekniken, så ingick även i uppgiften att modifiera en bläckstråleskrivare avsedd för kontor/hemmabruk för att möjliggöra tryckning av de två grundläggande materialen inom organisk elektrokemisk elektronik - den konjugerade polymeren PEDOT och en elektrolyt.</p><p>I denna uppsats rapporteras om hur en procedur för produktion av elektrokemisk elektronik har utvecklats. Världens första elektrokemiska transistor som producerats helt med bläckstråleteknik presenteras tillsammans med fullt fungerande implementeringar i logiska kretsar. Karaktärisering av filmer, komponenter och kretsar som producerats med bläckstråle- och screentrycksteknik har legat till grund för den utvärdering och jämförelse som har gjorts av teknikerna. Resultaten ser lovande ut och kan motivera vidare utveckling av bläckstrålesystem för produktion av prototyper och mindre serier. En kombination av de båda nämnda teknikerna är också ett tänkbart alternativ för småskalig tillverkning.</p> / <p>Linköping University and the research institute Acreo AB in Norrköping are in collaboration conducting research on organic electrochemical electronic devices. Acreo is pushing the development of high-speed reel-to-reel printing of this type of electronics. Today, most demonstrators and prototypes are made using manual, subtractive patterning methods. More tools, simplifying this work, are of interest. The purpose of this thesis work was to evaluate the potential of both inkjet and screen printing as manufacturing tools of electrochemical devices and to conduct a comparative study of these two additive patterning technologies. The work on inkjet printing included the modification of a commercially available desktop inkjet printer in order to print the conjugated polymer PEDOT and an electrolyte solution - these are the two basic components of organic electrochemical devices. For screen printing, existing equipment at Acreo AB was employed for device production.</p><p>In this report the successful development of a simple system and procedure for the inkjet printing of organic electrochemical devices is described. The first all-inkjet printed electrochemical transistor (ECT) and fully functional implementations of these ECTs in printed electrochemical logical circuits are presented.</p><p>The characterization of inkjet and screen printed devices has, along with an evaluation of how suitable the two printing procedures are for prototype production, been the foundation of the comparison of the two printing technologies.</p><p>The results are promising and should encourage further effort to develop a more complete and easily controlled inkjet system for this application. At this stage of development, a combination of the two technologies seems like an efficient approach.</p>

Introduced in 1991, solid ink color printing technology is widely used in the office printing, prepress proofing, and wide format color printing markets. Ink droplets are first deposited on a rotating drum and then transferred to paper to reproduce images with high print quality. The objective of this thesis is to develop scientific knowledge of ink droplet deposition, which is needed for precise image buildup on the drum surface. The first problem studied in the thesis is droplet formation from the printhead with varied working voltages and jetting frequencies. Attention is paid to the formation of satellite droplets, the contraction of ligaments and the startup of high frequency jetting. The jetting conditions for obtaining consistent droplet generation with satellites are determined. A theoretical model is developed to predict the lifetime of ligaments. The second problem we studied is the deposition of single droplets on solid surfaces. The surface texture and final shape of deposited droplets are correlated with impact conditions, which include printhead temperature, substrate temperature, distance from printhead to substrate, and the type of substrate surface. An analytical model is developed to evaluate the interaction of oscillation and viscous damping in the droplet during impact. The third problem covered in the thesis is the deposition of multiple ink droplets on the drum surface. Interaction between droplets causes drawback effect, which degrades print quality. We define a parameter to quantify the drawback effect with varied deposition conditions. A simple model is provided to predict conditions for making continuous lines based on the results of two ink droplets deposition. To understand the hydrodynamics in causing drawback effect, a series of experiments using large liquid droplets are carried out. Focus is put on the evolution of spread length and dynamics of contact line. Correlations for maximum and minimum spread lengths are developed, which are used to reveal the cause of drawback effect in the deposition of ink droplets.

A hygroexpansimeter, cockling tester and a novel x-ray microtomography technique were employed to characterize hygroexpansivity as well as macro- and micro-scale cockling of wood-free paper sheets containing varying amounts of aspen high yield pulp (HYP) in order to validate its potential applicability in inkjet printing. Results from the hygroexpansimeter confirm previous findings that substitution levels of 30% and above lead to a slight deterioration of hygroexpansivity; however, contrary to the expected outcome, aspen HYP did not necessarily result in a higher tendency to form cockles. In fact, a comparison of the cockling behaviour between various paper samples and commercial paper substantiates that up to 40% of aspen HYP can replace hardwood bleached Kraft pulp. The preservation of out-of-plane dimensional stability in non-coated samples is most likely due to the increase in bending stiffness of the paper as it became bulkier with more aspen HYP.

A hygroexpansimeter, cockling tester and a novel x-ray microtomography technique were employed to characterize hygroexpansivity as well as macro- and micro-scale cockling of wood-free paper sheets containing varying amounts of aspen high yield pulp (HYP) in order to validate its potential applicability in inkjet printing. Results from the hygroexpansimeter confirm previous findings that substitution levels of 30% and above lead to a slight deterioration of hygroexpansivity; however, contrary to the expected outcome, aspen HYP did not necessarily result in a higher tendency to form cockles. In fact, a comparison of the cockling behaviour between various paper samples and commercial paper substantiates that up to 40% of aspen HYP can replace hardwood bleached Kraft pulp. The preservation of out-of-plane dimensional stability in non-coated samples is most likely due to the increase in bending stiffness of the paper as it became bulkier with more aspen HYP.