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Electrocatalysis enables the industrial transition to sustainable production of chemicals using abundant precursors and electricity from renewable sources. De‐centralized production of hydrogen peroxide (H2O2) from water and oxygen of air is highly desirable for daily life and industry. We report an effective electrochemical refinery (e‐refinery) for H2O2 by means of electrocatalysis‐controlled comproportionation reaction (2H2O+O2→2H2O2), feeding pure water and oxygen only. Mesoporous nickel (II) oxide (NiO) was used as electrocatalyst for oxygen evolution reaction (OER), producing oxygen at the anode. Conducting polymer poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) drove the oxygen reduction reaction (ORR), forming H2O2 on the cathode. The reactions were evaluated in both half‐cell and device configurations. The performance of the H2O2 e‐refinery, assembled on anion‐exchange solid electrolyte and fed with pure water, was limited by the unbalanced ionic transport. Optimization of the operation conditions allowed a conversion efficiency of 80%. [ABSTRACT FROM AUTHOR]

Lignin, obtained as a waste product in huge quantities from the large‐scale cellulose processing industries, holds a great potential to be used as sustainable electrode material for large‐scale electroactive energy storage systems. The fixed number of redox‐active phenolic groups present within the lignin structure limits the electrochemical performance and the total energy storage capacity of the lignin‐based electrodes. Herein, the way to enhance the charge storage capacity of lignin by incorporating additional small catechol molecules into the lignin structure is demonstrated. The catechol derivatives are covalently attached to the lignin via aromatic electrophilic substitution reaction. The increased phenolic groups in all functionalized lignin derivatives notably increase the values of capacitance compared to pristine lignin. Further, solvent fractionation of lignin followed by functionalization using catechol boosts three times the charge capacity of lignin electrode. [ABSTRACT FROM AUTHOR]

The quest for eco‐friendly materials with anticipated positive impact for sustainability is crucial to achieve the UN sustainable development goals. Classical strategies of composite materials can be applied on novel nanomaterials and green materials. Besides the actual technology and applications also processing and manufacturing methods should be further advanced to make entire technology concepts sustainable. Here, they show an efficient way to combine two low‐cost materials, cellulose and zinc oxide (ZnO), to achieve novel functional and "green" materials via paper‐making processes. While cellulose is the most abundant and cost‐effective organic material extractable from nature. ZnO is cheap and known of its photocatalytic, antibacterial, and UV absorption properties. ZnO nanowires are grown directly onto cellulose fibers in water solutions and then dewatered in a process mimicking existing steps of large‐scale papermaking technology. The ZnO NW paper exhibits excellent photo‐conducting properties under simulated sunlight with good ON/OFF switching and long‐term stability (90 minutes). It also acts as an efficient photocatalyst for hydrogen peroxide (H2O2) generation (5.7 × 10−9 m s−1) with an envision the possibility of using it in buildings to enable large surfaces to spontaneously produce H2O2 at its outer surface. Such technology promise for fast degradation of microorganisms to suppress the spreading of diseases. [ABSTRACT FROM AUTHOR]

Practical interest in oxygen reduction reaction (ORR) has traditionally been due to its application at fuel cells' cathode following its complete 4e route to the water. In search of new electrode materials, it was discovered that conducting polymers (CPs) also are capable of driving ORR, though predominantly halting the process at 2e reduction leading to hydrogen peroxide generation. As alternative ways to produce this "green oxidant" are attracting increasing attention, a detailed study of the ORR mechanism at CP electrodes gains importance. Here, we summarize our recent theoretical work on the topic, which underscores the fundamental difference between CP and electrocatalytic metal ORR electrodes. Our insights also bring to us the attention of outer‐sphere electron transfer, not unknown but somewhat ignored in the field. We also put the action of CP electrodes in a more general context of chemical ORR and redox mediation responsible for the electrocatalytic ORR mechanism. [ABSTRACT FROM AUTHOR]

Zn‐ion batteries are one of the hot candidates for low‐cost and sustainable secondary batteries. The hydrogen evolution and dendritic growth upon zinc deposition are today's challenges for that technology. One of the new strategies to cope with these issues is to use "water‐in‐salt" electrolyte (WISE), that is, super concentrated aqueous electrolytes, to broaden its electrochemical stability window (ESW), suppressing hydrogen evolution reaction (HER), and perturbing the dendritic growth. Herein, this work proposes to use "water‐in‐polymer salt" electrolyte (WIPSE) concept to mitigate the challenges with Zn ion batteries and bring this technology toward one of the cheapest, greenest, and most sustainable electrodes: Lignin‐carbon (L‐C) electrode. Potassium polyacrylate (PAAK) as WISE bears out as better electrolyte for L‐C electrodes in terms of self‐discharge, cyclic stability, and specific capacity compared to conventional electrolyte based on chemically cousin molecule potassium acetate. Zinc bis(trifluoromethanesulfonyl) imide (Zn(TFSI)2) added into WIPSE shows deposition and dissolution of Zn in Zn//Zn symmetric cell suggesting that Zn2+ are moving into the polyanionic network. Furthermore, the added bis (trifluor omethanesul fonyl) imide (TFSI−) metal salts trigger a ≈40% enhancement of the capacity of L‐C electrode. These results show a new promising direction toward the development of cost‐effective and sustainable Zn‐lignin batteries. [ABSTRACT FROM AUTHOR]

Lignin, a byproduct from the pulp industry, is one of the redox active biopolymers being investigated as a component in the electrodes for sustainable energy storage applications. Due to its insulating nature, it needs to be combined with a conductor such as carbon or conducting polymer for efficient charge storage. Herein, the lignin/carbon composite electrodes manufactured via mechanical milling (ball milling) are reported. The composite formation, correlation between performance and morphology is studied by comparison with manual mixing and jet milling. Superior charge storage capacity with ≈70% of the total contribution from the Faradaic process involving the redox functionality of lignin is observed in a mechanically milled composite. In comparison, manual mix shows only ≈30% from the lignin storage participation while the rest is due to the electric double layer at the carbon–electrolyte interface. The significant participation of lignin in the ball milled composite is attributed to the homogeneous, intimate mixing of the carbon and the lignin leading the electronic carrier transported in the carbon phase to reach most of the redox group of lignin. A maximum capacity of 49 mAh g−1 is obtained at charge/discharge rate of 0.25 A g−1 for the sample milled for 60 min. [ABSTRACT FROM AUTHOR]

The next generation of green ion selective membranes is foreseen to be based on cellulosic nanomaterials with controllable properties. The introduction of ionic groups into the cellulose structure via chemical modification is one strategy to obtain desired functionalities. In this work, bleached softwood fibers are oxidatively sulfonated and thereafter homogenized to liberate the cellulose nanofibrils (CNFs) from the fiber walls. The liberated CNFs are subsequently used to prepare and characterize novel cellulose membranes. It is found that the degree of sulfonation collectively affects several important properties of the membranes via the density of fixed charged groups on the surfaces of the CNFs, in particular the membrane morphology, water uptake and swelling, and correspondingly the ionic transport. Both ionic conductivity and cation transport increase with the increased level of sulfonation of the starting material. Thus, it is shown that the chemical modification of the CNFs can be used as a tool for precise and rational design of green ion selective membranes that can replace expensive conventional fluorinated ionomer membranes. [ABSTRACT FROM AUTHOR]

Ionic thermoelectric supercapacitors (ITESCs) have recently been developed for converting low‐grade waste heat into electricity. Until now, most reports of ITESCs have been focused on the development of electrolytes, which then have been combined with a specific electrode material. Here, it is demonstrated that the electrode is not only critical for electrical energy storage but also greatly affects the effective thermopower (Seff) of an ITESC. It is shown that the same ion gel can generate a positive thermopower in an ITESC when using gold nanowire (AuNW) electrodes, while generating a negative thermopower when using poly(3,4‐ethylendioxythiophene):polystyrene sulfonate (PEDOT:PSS) electrodes. The achieved negative sign of the Seff could be attributed to the Donnan exclusive effect from the polyanions in the PEDOT:PSS electrodes. After examining the thermovoltage, capacitance and charge retention performance of the two ITESCs, it is concluded that PEDOT:PSS is superior to AuNWs as electrodes. Moreover, a new strategy of constructing an ionic thermopile of multiple p‐ and n‐type legs is achieved by series‐connecting these legs with same electrolyte but different electrodes. Using interfacial effect at ionic gels/PEDOT:PSS electrode interface, an enhanced thermoelectric effect in ITESCs is obtained, which constitutes one more step towards efficient, low‐cost, flexible, and printable ionic thermoelectric modules for energy harvesting. [ABSTRACT FROM AUTHOR]

Producing thick films of conducting polymers by a low‐cost manufacturing technique would enable new applications. However, removing huge solvent volume from diluted suspension or dispersion (1–3 wt%) in which conducting polymers are typically obtained is a true manufacturing challenge. In this work, a procedure is proposed to quickly remove water from the conducting polymer poly(3,4‐ethylenedioxythiophene:poly(4‐styrene sulfonate) (PEDOT:PSS) suspension. The PEDOT:PSS suspension is first flocculated with 1 m H2SO4 transforming PEDOT nanoparticles (≈50–500 nm) into soft microparticles. A filtration process inspired by pulp dewatering in a paper machine on a wire mesh with apertures dimension between 60 µm and 0.5 mm leads to thick free‐standing films (≈0.5 mm). Wire mesh clogging that hinders dewatering (known as dead‐end filtration) is overcome by adding to the flocculated PEDOT:PSS dispersion carbon fibers that aggregate and form efficient water channels. Moreover, this enables fast formation of thick layers under simple atmospheric pressure filtration, thus making the process truly scalable. Thick freestanding PEDOT films thus obtained are used as electrocatalysts for efficient reduction of oxygen to hydrogen peroxide, a promising green chemical and fuel. The inhomogeneity of the films does not affect their electrochemical function. [ABSTRACT FROM AUTHOR]

Organic‐based energy harvesting devices can contribute to a sustainable solution for the transition to renewable energy sources. The concept of ionic thermoelectrics (iTE) has been recently proposed and motivated by the high values of thermo‐voltage in electrolytes. So far, most research has focused on developing new electrolytes with high Seebeck coefficient. Despite the major role of the electrode materials in supercapacitors and batteries, the effect of various electrodes on energy harvesting in iTE devices has not been widely studied. In this work, the conducting polymer poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is investigated as the functional electrodes in iTE supercapacitors. Through investigating the thermo‐voltage of iTEs of the same electrolyte with varying composition of PEDOT electrodes, it is identified that the different PSS content greatly affects the overall thermo‐induced voltage coefficient, Seff (i.e., effective thermopower). The permselective polyanion in the electrode causes cation concentration differences at the electrode/electrolyte interface and contributes to an interfacial potential drop that is temperature dependent. As a result, the overall thermo‐voltage of the device possesses both an interfacial and a bulk contribution. The findings extend the fundamental understanding of iTE effect with functional electrodes, which could lead a new direction to enhance the heat‐to‐electricity conversion. [ABSTRACT FROM AUTHOR]

Biomimicry at the hardware level is expected to overcome at least some of the challenges, including high power consumption, large footprint, two‐dimensionality, and limited functionality, which arise as the field of artificial intelligence matures. One of the main attributes that allow biological systems to thrive is the successful interpretation of and response to environmental signals. Taking inspiration from these systems, the first demonstration of using multiple environmental inputs to trigger the formation and control the growth of an evolvable synaptic transistor is reported here. The resulting transistor exhibits long‐term changes in the channel conductance at a fixed gate voltage. Biomimetic logic circuits are investigated based on this evolvable transistor that implement temperature and pressure inputs to achieve higher order processes like self‐regulation of synaptic strength and coincidence detection. [ABSTRACT FROM AUTHOR]

The oxygen reduction reaction (ORR) limits the efficiency of oxygen‐associated energy conversion in fuel cells and air‐metal batteries. Today, expensive noble metal catalysts are often utilized to enhance the ORR and the resulting conversion efficiency in those devices. Hence, there is an intensive research to find efficient electrodes, exhibiting a favorable electronic structure, for ORR based on abundant materials that can be manufactured using low cost processes. In that context, metal‐free carbon‐based nanostructures and conducting polymers have been actively investigated. The negatively doped poly(benzimidazobenzophenanthroline) (BBL) as an efficient and stable oxygen cathode material is reported here. Compared to the benchmark p‐doped conducting polymer poly(3,4‐ethylendioxythiophene) (PEDOT), the BBL provides electrocatalysis that fully reduces dioxygen into water, via a (2 + 2)‐electron transfer pathway with hydrogen peroxide (H2O2) as an intermediate; while PEDOT limits the ORR to H2O2. It is demonstrated that n‐doped BBL is a promising air electrode material for low‐cost and ecofriendly model fuel cells, without the need of any co‐catalysts, and its performance is found to be superior to p‐doped PEDOT air electrodes. [ABSTRACT FROM AUTHOR]

The selective ion transport characteristics of a conducting polymer electrode, based on poly(3,4‐ethylenedioxythiophene) (PEDOT), is evaluated with respect to its electrocatalytic performance, specifically targeting redox switching of quinone couples. Employing model organic redox quinones, here, the novel phenomenon of ion‐selective electrocatalysis (ISEC) is conceptualized. The effect of ISEC is studied and evaluated using two forms of PEDOT electrodes, which differ in their ion‐exchange characteristics, by comparing the redox transformations of catechol and tiron. It is rationalized that the choice of the specific redox couple and the ion selectivity characteristics of the conducting polymer electrode impacts the activation losses in aqueous organic redox‐flow batteries. By carefully selecting and designing the conducting polymer electrodes, high conversion efficiency on acid‐resistant electrodes is obtained. As far as it is known, this is the first redox flow battery to include conducting polymer electrodes operating in both the posolyte and negolyte configurations, thus the first "all‐organic" RFBs. [ABSTRACT FROM AUTHOR]

Seawater desalination and wastewater purification technologies are the main strategies against the global fresh water shortage. Among these technologies, solar‐driven evaporation is effective in extracting fresh water by efficiently exploiting solar energy. However, building a sustainable and low‐cost solar steam generator with high conversion efficiency is still a challenge. Here, pure organic aerogels comprising a cellulose scaffold decorated with an organic conducting polymer absorbing in the infrared are employed to establish a high performance solar steam generator. The low density of the aerogel ensures minimal material requirements, while simultaneously satisfying efficient water transport. To localize the absorbed solar energy and make the system floatable, a porous floating and thermal‐insulating foam is placed between the water and the aerogel. Thanks to the high absorbance of the aerogel and the thermal‐localization performance of the foam, the system exhibits a high water evaporation rate of 1.61 kg m−2 h−1 at 1 kW m−2 under 1 sun irradiation, which is higher than most reported solar steam generation devices. [ABSTRACT FROM AUTHOR]

In recent years, there has been an upsurge in the study of novel and alternative energy storage devices beyond lithium‐based systems due to the exponential increase in price of lithium. Sodium (Na) metal‐based batteries can be a possible alternative to lithium‐based batteries due to the similar electrochemical voltage of Na and Li together with the thousand times higher natural abundance of Na compared to Li. Though two different kinds of Na–O2 batteries have been studied specifically based on electrolytes until now, very recently, a hybrid Na–air cell has shown distinctive advantage over nonaqueous cell systems. Hybrid Na–air batteries provide a fundamental advantage due to the formation of highly soluble discharge product (sodium hydroxide) which leads to low overpotentials for charge and discharge processes, high electrical energy efficiency, and good cyclic stability. Herein, the current status and challenges associated with hybrid Na–air batteries are reported. Also, a brief description of nonaqueous Na–O2 batteries and its close competition with hybrid Na–air batteries are provided. [ABSTRACT FROM AUTHOR]

Abstract: The spectra of conducting polymers obtained using ultraviolet photoelectron spectroscopy (UPS) exhibit a typical broadening of the tail σUPS ≈ 1 eV, which by an order of magnitude exceeds a commonly accepted value of the broadening of the tail of the density of states σDOS ≈ 0.1 eV obtained using transport measurements. In this work, an origin of this anomalous broadening of the tail of the UPS spectra in a doped conducting polymer, PEDOT (poly(3,4‐ethylenedioxythiophene)), is discussed. Based on the semiempirical approach and using a realistic morphological model, the density of valence states in PEDOT doped with molecular counterions is computed. It is shown that due to a disordered character of the material with randomly distributed counterions, the localized charge carriers in PEDOT crystallites experience spatially varying electrostatic potential. This leads to spatially varying local vacuum levels and binding energies. Taking this variation into account the UPS spectrum is obtained with the broadening of the tail comparable to the experimentally observed one. The results imply that the observed broadening of the tail of the UPS spectra in PEDOT provides information about a disordered spatially varying potential in the material rather than the broadening of the DOS itself. [ABSTRACT FROM AUTHOR]

Abstract: A free‐standing high‐output power density polymeric thermoelectric (TE) device is realized based on a highly conductive (≈2500 S cm−1) structure‐ordered poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate film (denoted as FS‐PEDOT:PSS) with a Seebeck coefficient of 20.6 µV K−1, an in‐plane thermal conductivity of 0.64 W m−1 K−1, and a peak power factor of 107 µW K−2 m−1 at room temperature. Under a small temperature gradient of 29 K, the TE device demonstrates a maximum output power density of 99 ± 18.7 µW cm−2, which is the highest value achieved in pristine PEDOT:PSS based TE devices. In addition, a fivefold output power is demonstrated by series connecting five devices into a flexible thermoelectric module. The simplicity of assembling the films into flexible thermoelectric modules, the low out‐of‐plane thermal conductivity of 0.27 W m−1 K−1, and free‐standing feature indicates the potential to integrate the FS‐PEDOT:PSS TE modules with textiles to power wearable electronics by harvesting human body's heat. In addition to the high power factor, the high thermal stability of the FS‐PEDOT:PSS films up to 250 °C is confirmed by in situ temperature‐dependent X‐ray diffraction and grazing incident wide angle X‐ray scattering, which makes the FS‐PEDOT:PSS films promising candidates for thermoelectric applications. [ABSTRACT FROM AUTHOR]

ABSTRACT Owing to changes in their chemistry and structure, polymers can be fabricated to demonstrate vastly different electrical conductivities over many orders of magnitude. At the high end of conductivity is the class of conducting polymers, which are ideal candidates for many applications in low-cost electronics. Here, we report the influence of the nature of the doping anion at high doping levels within the semi-metallic conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) on its electronic transport properties. Hall effect measurements on a variety of PEDOT samples show that the choice of doping anion can lead to an order of magnitude enhancement in the charge carrier mobility > 3 cm2/Vs at conductivities approaching 3000 S/cm under ambient conditions. Grazing Incidence Wide Angle X-ray Scattering, Density Functional Theory calculations, and Molecular Dynamics simulations indicate that the chosen doping anion modifies the way PEDOT chains stack together. This link between structure and specific anion doping at high doping levels has ramifications for the fabrication of conducting polymer-based devices. © 2017 The Authors. Journal of Polymer Science Part B: Polymer Physics Published by Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018, 56, 97-104 [ABSTRACT FROM AUTHOR]

The evolution of the society is characterized by an increasing flow of information from things to the internet. Sensors have become the cornerstone of the internet-of-everything as they track various parameters in the society and send them to the cloud for analysis, forecast, or learning. With the many parameters to sense, sensors are becoming complex and difficult to manufacture. To reduce the complexity of manufacturing, one can instead create advanced functional materials that react to multiple stimuli. To this end, conducting polymer aerogels are promising materials as they combine elasticity and sensitivity to pressure and temperature. However, the challenge is to read independently pressure and temperature output signals without cross-talk. Here, a strategy to fully decouple temperature and pressure reading in a dual-parameter sensor based on thermoelectric polymer aerogels is demonstrated. It is found that aerogels made of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) can display properties of semiconductors lying at the transition between insulator and semimetal upon exposure to high boiling point polar solvents, such as dimethylsulfoxide (DMSO). Importantly, because of the temperature-independent charge transport observed for DMSO-treated PEDOT-based aerogel, a decoupled pressure and temperature sensing can be achieved without cross-talk in the dual-parameter sensor devices. [ABSTRACT FROM AUTHOR]

Poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is the most studied and explored mixed ion-electron conducting polymer system. PEDOT:PSS is commonly included as an electroactive conductor in various organic devices, e.g., supercapacitors, displays, transistors, and energy-converters. In spite of its long-term use as a material for storage and transport of charges, the fundamentals of its bulk capacitance remain poorly understood. Generally, charge storage in supercapacitors is due to formation of electrical double layers or redox reactions, and it is widely accepted that PEDOT:PSS belongs to the latter category. Herein, experimental evidence and theoretical modeling results are reported that significantly depart from this commonly accepted picture. By applying a two-phase, 2D modeling approach it is demonstrated that the major contribution to the capacitance of the two-phase PEDOT:PSS originates from electrical double layers formed along the interfaces between nanoscaled PEDOT-rich and PSS-rich interconnected grains that comprises two phases of the bulk of PEDOT:PSS. This new insight paves a way for designing materials and devices, based on mixed ion-electron conductors, with improved performance. [ABSTRACT FROM AUTHOR]

ABSTRACT Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate) (PEDOT:PSS) has been reported as a successful functional material in a broad variety of applications. One of the most important advantages of PEDOT:PSS is its water-solubility, which enables simple and environmental friendly manufacturing processes. Unfortunately, this also implies that pristine PEDOT:PSS films are unsuitable for applications in aqueous environments. To reach stability in polar solvents, (3-glycidyloxypropyl)trimethoxysilane (GOPS) is typically used to cross-link PEDOT:PSS. Although this strategy is widely used, its mechanism and effect on PEDOT:PSS performance have not been articulated yet. Here, we present a broad study that provides a better understanding of the effect of GOPS on the electrical and electronic properties of PEDOT:PSS. We show that the GOPS reacts with the sulfonic acid group of the excess PSS, causing a change in the PEDOT:PSS film morphology, while the oxidation level of PEDOT remains unaffected. This is at the origin of the observed conductivity changes. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2017, 55, 814-820 [ABSTRACT FROM AUTHOR]

Thermoelectric materials enable conversion of heat to electrical energy. The performance of electronic thermoelectric materials is typically evaluated using a figure of merit ZT = σα2T/λ, where σ is the conductivity, α is the so‐called Seebeck coefficient, and λ is the thermal conductivity. However, it has been unclear how to best evaluate the performance of ionic thermoelectric materials, like ionic solids and electrolytes. These systems cannot be directly used in a traditional thermoelectric generator, because they are based on ions that cannot pass the interface between the thermoelectric material and external metal electrodes. Instead, energy can be harvested from the ionic thermoelectric effect by charging a supercapacitor. In this study, the authors investigate the ionic thermoelectric properties at varied relative humidity for the polyelectrolyte polystyrene sulfonate sodium and correlate these properties with the charging efficiency when used in an ionic thermoelectric supercapacitor (ITESC). In analogy with electronic thermoelectric generators, the results show that the charging efficiency of the ITESC can be quantitatively related to the figure of merit ZTi = σiαi2T/λ. This means that the performance of ionic thermoelectric materials can also be compared and predicted based on the ZT, which will be highly valuable in the design of high‐performance ITESCs. [ABSTRACT FROM AUTHOR]

The thermoelectric (TE) phenomena are intensively explored by the scientific community due to the rather inefficient way energy resources are used with a large fraction of energy wasted in the form of heat. Among various materials, mixed ion-electron conductors (MIEC) are recently being explored as potential thermoelectrics, primarily due to their low thermal conductivity. The combination of electronic and ionic charge carriers in those inorganic or organic materials leads to complex evolution of the thermovoltage ( Voc) with time, temperature, and/or humidity. One of the most promising organic thermoelectric materials, poly(3,4-ethyelenedioxythiophene)-polystyrene sulfonate (PEDOT-PSS), is an MIEC. A previous study reveals that at high humidity, PEDOT-PSS undergoes an ionic Seebeck effect due to mobile protons. Yet, this phenomenon is not well understood. In this work, the time dependence of the Voc is studied and its behavior from the contribution of both charge carriers (holes and protons) is explained. The presence of a complex reorganization of the charge carriers promoting an internal electrochemical reaction within the polymer film is identified. Interestingly, it is demonstrated that the time dependence behavior of Voc is a way to distinguish between three classes of polymeric materials: electronic conductor, ionic conductor, and mixed ionic-electronic conductor. [ABSTRACT FROM AUTHOR]

In electronics, the field-effect transistor (FET) is a crucial cornerstone and successful integration of this semiconductor device into circuit applications requires stable and ideal electrical characteristics over a wide range of temperatures and environments. Solution processing, using printing or coating techniques, has been explored to manufacture organic field-effect transistors (OFET) on flexible carriers, enabling radically novel electronics applications. Ideal electrical characteristics, in organic materials, are typically only found in single crystals. Tiresome growth and manipulation of these hamper practical production of flexible OFETs circuits. To date, neither devices nor any circuits, based on solution-processed OFETs, has exhibited an ideal set of characteristics similar or better than today's FET technology based on amorphous silicon. Here, bar-assisted meniscus shearing of dibenzo-tetrathiafulvalene to coat-process self-organized crystalline organic semiconducting domains with high reproducibility is reported. Including these coatings as the channel in OFETs, electric field and temperature-independent charge carrier mobility and no bias stress effects are observed. Furthermore, record-high gain in OFET inverters and exceptional operational stability in both air and water are measured. [ABSTRACT FROM AUTHOR]

The semiconductor-electrode interface impacts the function and the performance of (opto)electronic devices. For printed organic electronics the electrode surface is not atomically clean leading to weakly interacting interfaces. As a result, solution-processed organic ultrathin films on electrodes typically form islands due to dewetting. It has therefore been utterly difficult to achieve homogenous ultrathin conjugated polymer films. This has made the investigation of the correct energetics of the conjugated polymer-electrode interface impossible. Also, this has hampered the development of devices including ultrathin conjugated polymer layers. Here, Langmuir-Shäfer-manufactured homogenous mono- and multilayers of semiconducting polymers on metal electrodes are reported and the energy level bending using photoelectron spectroscopy is tracked. The amorphous films display an abrupt energy level bending that does not extend beyond the first monolayer. These findings provide new insights of the energetics of the polymer-electrode interface and opens up for new high-performing devices based on ultrathin semiconducting polymers. [ABSTRACT FROM AUTHOR]

Conducting polymers display an ionic thermoelectric effect in addition to the known electronic thermoelectric effect. Their Seebeck coefficient is as large as ≈200 μV K−1. This finding discloses a new possible approach to improve the thermoelectric properties of conducting polymers by combining various types of charge carriers of the same sign. [ABSTRACT FROM AUTHOR]

Systematic investigation of the contact resistance in electrolyte-gated organic field-effect transistors (OFETs) demonstrates a dependence of source charge injection versus gate electrode work function. This analysis reveals contact-limitations at the source metal-semiconductor interface and shows that the contact resistance increases as low work function metals are used as the gate electrode. These findings are attributed to the establishment of a built-in potential that is high enough to prevent the Fermi-level pinning at the metal-organic interface. This results in an unfavorable energetic alignment of the source electrode with the valence band of the organic semiconductor. Since the operating voltage in the electrolyte-gated devices is on the same order as the variation of the work functions, it is possible to tune the contact resistance over more than one order of magnitude by varying the gate metal. [ABSTRACT FROM AUTHOR]