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This study reports on the first all‐printed vertically stacked organic electrochemical transistors (OECTs) operating in accumulation mode; the devices, relying on poly([4,4′‐bis(2‐(2‐(2‐methoxyethoxy)ethoxy)ethoxy)‐2,2′‐bithiophen‐5,5′‐diyl]‐alt‐[thieno[3,2‐b]thiophene‐2,5‐diyl]) (pgBTTT) as the active channel material, are fabricated via a combination of screen and inkjet printing technologies. The resulting OECTs (W/L ≈5) demonstrate good switching performance; gm, norm ≈13 mS cm−1, µC* ≈21 F cm−1 V−1 s−1, ON–OFF ratio > 104 and good cycling stability upon continuous operation for 2 h. The inkjet printing process of pgBTTT is established by first solubilizing the polymer in dihydrolevoglucosenone (Cyrene), a non‐toxic, cellulose‐derived, and biodegradable solvent. The resulting ink formulations exhibit good jettability, thereby providing reproducible and stable p‐type accumulation mode all‐printed OECTs with high performance. Besides the environmental and safety benefits of this solvent, this study also demonstrates the assessment of how the solvent affects the performance of spin‐coated OECTs, which justifies the choice of Cyrene as an alternative to commonly used harmful solvents such as chloroform, also from a device perspective. Hence, this approach shows a new possibility of obtaining more sustainable printed electronic devices, which will eventually result in all‐printed OECT‐based logic circuits operating in complementary mode. [ABSTRACT FROM AUTHOR]

Stretchable organic electrochemical transistors (OECTs) are promising for wearable applications within biosensing, bio‐signal recording, and addressing circuitry. Efficient large‐scale fabrication of OECTs can be performed with printing methods but to date there are no reports on high‐performance fully printed stretchable OECTs. Herein, this challenge is addressed by developing fully screen‐printed stretchable OECTs based on an architecture that minimizes electrochemical side reactions and improves long‐term stability. Fabrication of the OECTs is enabled by in‐house development of three stretchable functional screen‐printing inks and related printing processes. The stretchable OECTs show good characteristics in terms of transfer curves, output characteristics, and transient response up to 100% static strain and 500 strain cycles at 25% and 50% strain. The strain insensitivity of the OECTs can be further improved by strain conditioning, resulting in stable performance up to 50% strain. Finally, an electrochromic smart pixel is demonstrated by connecting a stretchable OECT to a stretchable electrochromic display. It is believed that the development of screen‐printed stretchable electrochemical devices, and OECTs in particular, will pave the way for their use in wearable applications and commercial products. [ABSTRACT FROM AUTHOR]

Microfluidic surface chemistry can enable control of capillary‐driven flow without the need for bulky external instrumentation. A novel pondered nonhomogeneous coating defines regions with different wetting properties on the microchannel walls. It changes the curvature of the liquid–air meniscus at various channel cross‐sections and consequently leads to different capillary pressures, which is favorable in the strive toward automatic flow control. This is accomplished by the deposition of hydrophilic coatings on the surface of multilevel 3D‐printed (3DP) microfluidic devices via inkjet printing, thereby retaining the surface hydrophilicity for at least 6 months of storage. To the best of our knowledge, this is the first demonstration of capillary flow control in 3DP microfluidics enabled by inkjet printing. The method is used to create "stop" and "delay" valves to enable preprogrammed capillary flow for sequential release of fluids. To demonstrate further utilization in point‐of‐care sensing applications, screen printed organic electrochemical transistors are integrated within the microfluidic chips to sense, sequentially and independently from external actions, chloride anions in the (1–100) × 10−3m range. The results present a cost‐effective fabrication method of compact, yet comprehensive, all‐printed sensing platforms that allow fast ion detection (<60 s), including the capability of automatic delivery of multiple test solutions. [ABSTRACT FROM AUTHOR]

Wood is an inherently hygroscopic material which tends to absorb moisture from its surrounding. Moisture in wood is a determining factor for the quality of wood being employed in construction, since it causes weakening, deformation, rotting, and ultimately leading to failure of the structures resulting in costs to the economy, the environment, and to the safety of residents. Therefore, monitoring moisture in wood during the construction phase and after construction is vital for the future of smart and sustainable buildings. Employing bio‐based materials for the construction of electronics is one way to mitigate the environmental impact of such electronics. Herein, a bio‐graphene sensor for monitoring the moisture inside and around wooden surfaces is fabricated using laser‐induced graphitization of a lignin‐based ink precursor. The bio‐graphene sensors are used to measure humidity in the range of 10% up to 90% at 25 °C. Using laser induced graphitization, conductor resistivity of 18.6 Ω sq−1 is obtained for spruce wood and 57.1 Ω sq−1 for pine wood. The sensitivity of sensors fabricated on spruce and pine wood is 2.6 and 0.74 MΩ per % RH. Surface morphology and degree of graphitization are investigated using scanning electron microscopy, Raman spectroscopy, and thermogravimetric analysis methods. [ABSTRACT FROM AUTHOR]

Triboelectric nanogenerators (TENGs) are a new class of energy harvesting devices that have the potential to become a dominating technology for producing renewable energy. The versatility of their designs allows TENGs to harvest mechanical energy from sources like wind and water. Currently used renewable energy technologies have a restricted number of materials from which they can be constructed, such as metals, plastics, semiconductors, and rare‐earth metals. These materials are all non‐renewable in themselves as they require mining/drilling and are difficult to recycle at end of life. TENGs on the other hand can be built from a large repertoire of materials, including materials from bio‐based sources. Here, a TENG constructed fully from wood‐derived materials like lignin, cellulose, paper, and cardboard, thus making it 100% green, recyclable, and even biodegradable, is demonstrated. The device can produce a maximum voltage, current, and power of 232 V, 17 mA m–2, and 1.6 W m–2, respectively, which is enough to power electronic systems and charge 6.5 µF capacitors. Finally, the device is used in a smart package application as a self‐powered impact sensor. The work shows the feasibility of producing renewable energy technologies that are sustainable both with respect to their energy sources and their material composition. [ABSTRACT FROM AUTHOR]

Low weight, small footprint, and high performances are essential requisites for the implementation of energy storage devices within consumer electronics. One way to achieve these goals is to increase the thickness of the active material layer. In this work, carbonized and graphitized rayon felt, a cellulose‐derived material, is used as a three‐dimensional current collector scaffold to enable the incorporation of large amount of active energy storage materials and ionic liquid‐based gel electrolyte in the supercapacitor devices. PEDOT:PSS, alone or in combination with active carbon, has been used as the active material. Three‐dimensional supercapacitors with high per unit area capacitance (more than 1.1 F/cm2) have been achieved owing to the loading of large amount of active material in the felt matrix. Areal energy density of more than 101 μWh/cm2 and areal power density of more than 5.9 mW/cm2 have been achieved for 0.8 V operating voltage at a current density of 1 mA/cm2. A nanographite material was found to be beneficial in reducing the internal serial resistance of the supercapacitor to lower than 1.7 Ω. Furthermore, it was shown that even after 2000 times cycling test, the devices could still retain its performance with at least 88% coulombic efficiency for all the devices. All the materials are readily available commercially, environmentally sustainable and the process can potentially be upscaled with industrial process. [ABSTRACT FROM AUTHOR]

This work demonstrates a novel fabrication approach based on the combination of screen and aerosol jet printing to manufacture fully printed organic electrochemical transistors (OECTs) and OECT‐based logic circuits on PET substrates with superior performances. The use of aerosol jet printing allows for a reduction of the channel width to ≈15 µm and the estimated volume by a factor of ≈40, compared to the fully screen printed OECTs. Hence, the OECT devices and OECT‐based logic circuits fabricated with the proposed approach emerge with a high ON/OFF ratio (103–104) and remarkably fast switching response, reaching an ON/OFF ratio of >103 in 4–8 ms, which is further demonstrated by a propagation delay time of just above 1 ms in OECT‐based logic inverter circuits operated at a frequency of 100 Hz. All‐printed monolithically integrated OECT‐based five‐stage ring oscillator circuits further validated the concept with a resulting self‐oscillation frequency of 60 Hz. [ABSTRACT FROM AUTHOR]

Organic electrochemical transistors (OECTs) are finding widespread application in biosensing, thanks to their high sensitivity, broad dynamic range, and low limit of detection. An OECT biosensor requires the immobilization of a biorecognition probe on the gate, or else on the channel, through several, often lengthy, chemical steps. In this work, a fast and straightforward way to functionalize the carbon gate of a fully screen‐printed OECT by means of a polydopamine (PDA) film is presented. By chemical immobilization of an amine‐terminated single‐stranded oligonucleotide, containing the HSP70 promoter CCAAT sequence, on the PDA film, the detection of the complementary DNA strand is demonstrated. Furthermore, the specificity of the developed genosensor is assessed by comparing its response to the fully complementary strand with the one to partially complementary and noncomplementary oligonucleotides. The developed sensor shows a theoretical limit of detection (LOD) of 100 × 10−15m and a dynamic range over four orders of magnitude. [ABSTRACT FROM AUTHOR]

Low‐cost, minimally invasive sensors able to provide real‐time monitoring of wound infection can enable the optimization of healthcare resources in chronic wounds management. Here, a novel printed organic electrochemical transistors (OECT) biosensor for monitoring uric acid (UA), a bacterial infection biomarker in wounds, is demonstrated in artificial wound exudate. The sensor exploits the enzymatic conversion of UA to 5‐hydroxyisourate, catalyzed by Uricase entrapped in a dual‐ionic‐layer hydrogel membrane casted onto the gate. The sensor response is based on the catalytic oxidation of the hydrogen peroxide, generated as part of the Uricase regeneration process, at the Pt modified gate. The proposed dual membrane avoids the occurrence of nonspecific faradic reactions as, for example, the direct oxidation of UA or other electroactive molecules that would introduce a potentially false negative response. The biosensor is robust and its response is reproducible both in phosphate buffer saline and in complex solutions mimicking the wound exudate. The sensor has a high sensitivity in the range encompassing the pathological levels of UA in wounds (<200 μm) exhibiting a limit of detection of 4.5 μm in artificial wound exudate. All these characteristics make this OECT‐based biosensor attractive for wound monitoring interfaced to the patient. [ABSTRACT FROM AUTHOR]

The bioconjugation of polyoxometalates (POMs), which are inorganic metal oxido clusters, to DNA strands to obtain functional labeled DNA primers and their potential use in electrochemical detection have been investigated. Activated monooxoacylated polyoxotungstates [SiW11O39{Sn(CH2)2CO}]8− and [P2W17O61{Sn(CH2)2CO}]6− have been used to link to a 5′-NH2 terminated 21-mer DNA forward primer through amide coupling. The functionalized primer was characterized by using a battery of techniques, including electrophoresis, mass spectrometry, as well as IR and Raman spectroscopy. The functionality of the POM-labeled primers was demonstrated through hybridization with a surface-immobilized probe. Finally, the labeled primers were successfully used in the polymerase chain reaction (PCR) and the PCR products were characterized by using electrophoresis. [ABSTRACT FROM AUTHOR]

A controlled, rapid, and potentiostat-free method has been developed for grafting the diazonium salt (3,5-bis(4-diazophenoxy)benzoic acid tetrafluoroborate (DCOOH)) on gold and carbon substrates, based on a Zn-mediated chemical dediazonation. The highly stable thin layer organic platforms obtained were characterized by cyclic voltammetry, AFM, impedance, XP, and Raman spectroscopies. A dediazonation mechanism based on radical formation is proposed. Finally, DCOOH was proved as a linker to an aminated electroactive probe. [ABSTRACT FROM AUTHOR]

Carbon is a highly adaptable family of materials and is one of the most chemically stable materials known, providing a remarkable platform for the development of tunable molecular interfaces. Herein, we report a two-step process for the electrochemical hydrogenation of glassy carbon followed by either chemical or electrochemical chlorination to provide a highly reactive surface for further functionalization. The carbon surface at each stage of the process is characterized by AFM, SEM, Raman, attenuated total reflectance (ATR) FTIR, X-ray photoelectron spectroscopy (XPS), and electroanalytical techniques. Electrochemical chlorination of hydrogen-terminated surfaces is achieved in just 5 min at room temperature with hydrochloric acid, and chemical chlorination is performed with phosphorus pentachloride at 50 °C over a three-hour period. A more controlled and uniform surface is obtained using the electrochemical approach, as chemical chlorination is observed to damage the glassy carbon surface. A ferrocene-labeled alkylthiol is used as a model system to demonstrate the genericity and potential application of the highly reactive chlorinated surface formed, and the methodology is optimized. This process is then applied to thiolated DNA, and the functionality of the immobilized DNA probe is demonstrated. XPS reveals the covalent bond formed to be a CS bond. The thermal stability of the thiolated molecules anchored on the glassy carbon is evaluated, and is found to be far superior to that on gold surfaces. This is the first report on the electrochemical hydrogenation and electrochemical chlorination of a glassy carbon surface, and this facile process can be applied to the highly stable functionalization of carbon surfaces with a plethora of diverse molecules, finding widespread applications. [ABSTRACT FROM AUTHOR]

Energy harvesting from photosynthetic membranes, proteins, or bacteria through bio‐photovoltaic or bio‐electrochemical approaches has been proposed as a new route to clean energy. A major shortcoming of these and solar cell technologies is the underutilization of solar irradiation wavelengths in the IR region, especially those in the far IR region. Here, a biohybrid energy‐harvesting device is demonstrated that exploits IR radiation, via convection and thermoelectric effects, to improve the resulting energy conversion performance. A composite of nanocellulose and the conducting polymer system poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is used as the anode in biohybrid cells that includes thylakoid membranes (TMs) and redox mediators (RMs) in solution. By irradiating the conducting polymer electrode by an IR light‐emitting diode, a sixfold enhancement in the harvested bio‐photovoltaic power is achieved, without compromising stability of operation. Investigation of the output currents reveals that IR irradiation generates convective heat transfer in the electrolyte bulk, which enhances the redox reactions of RMs at the anode by suppressing diffusion limitations. In addition, a fast‐transient thermoelectric component, originating from the PEDOT:PSS‐nanocellulose‐electrolyte interphase, further increases the bio‐photocurrent. These results pave the way for the development of energy‐harvesting biohybrids that make use of heat, via IR absorption, to enhance energy conversion efficiency. [ABSTRACT FROM AUTHOR]

The photochemical core of every photosynthetic apparatus is the reaction center, a transmembrane enzyme that converts photons into charge‐separated states across the biological membrane with an almost unitary quantum yield. A light‐responsive organic transistor architecture, which converts light into electrical current by exploiting the efficiency of this biological machinery, is presented. Proper surface tailoring enables the integration of the bacterial reaction center as photoactive element in organic transistors, allowing the transduction of its photogenerated voltage into photomodulation of the output current up to two orders of magnitude. This device architecture, termed light‐responsive electrolyte‐gated organic transistor, is the prototype of a new generation of low‐power hybrid bio‐optoelectronic organic devices. [ABSTRACT FROM AUTHOR]

The development of electronics with net zero carbon emissions through more efficient and environmentally friendly materials and processes is still a challenge. Here, alternative chemical synthesis routes of metal conductive nanoparticles, based on biodegradable materials are explored, such as nickel, iron–nickel alloy and iron nanoparticles, to be used, in the long term, as fillers in inks for inject printing. Thus, Ni and FeNi metal nanoparticles of 25–12 nm, forming aggregates of 614–574 nm, respectively, are synthesized in water in the presence of a polyol and a reducing agent and under microwave heating that enables a more uniform and fast heating. Iron nanoparticles of 120 ± 40 nm are synthesized in polyol that limits the aggregation and the oxidation degree. Commercial metal nanoparticles of iron and nickel, are coated with ethylene glycol and used for comparison. The conductivity of nanoparticles when pressed into pellets remains similar for both commercial and synthesized samples. However, when deposited on a strip line and heated, synthesized Ni, FeNi, and Fe nanoparticles show significant conductivity and interesting magnetic properties. It is demonstrated that the nanosize facilitates sintering at reduced temperatures and the capping agents prevent oxidation, resulting in promising conductive fillers for printed electronic applications. [ABSTRACT FROM AUTHOR]