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Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a benchmark hole-transporting (p-type) polymer that finds applications in diverse electronic devices. Most of its success is due to its facile synthesis in water, exceptional processability from aqueous solutions, and outstanding electrical performance in ambient. Applications in fields like (opto-)electronics, bioelectronics, and energy harvesting/storage devices often necessitate the complementary use of both p-type and n-type (electron-transporting) materials. However, the availability of n-type materials amenable to water-based polymerization and processing remains limited. Herein, we present a novel synthesis method enabling direct polymerization in water, yielding a highly conductive, water-processable n-type conjugated polymer, namely, poly[(2,2 '-(2,5-dihydroxy-1,4-phenylene)diacetic acid)-stat-3,7-dihydrobenzo[1,2-b:4,5-b ']difuran-2,6-dione] (PDADF), with remarkable electrical conductivity as high as 66 S cm(-1), ranking among the highest for n-type polymers processed using green solvents. The new n-type polymer PDADF also exhibits outstanding stability, maintaining 90% of its initial conductivity after 146 days of storage in air. Our synthetic approach, along with the novel polymer it yields, promises significant advancements for the sustainable development of organic electronic materials and devices., Funding Agencies|Knut and Alice Wallenberg Foundation [2021.0058, 2021.0230, 2022.0034, 2023.0464]; Wallenberg Initiative Materials Science for Sustainability WISE); Swedish Research Council [2020-03243, 2020-04538, 2022-04053]; Olle Engkvists Stiftelse [204-0256]; European Commission through the HORATES [GA-955837]; SUNREY [GA-101084422]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University; National Research Foundation (NRF) of Korea [2009-00971]; [2019R1A6A1A11044070]

Heat is an inexhaustible source of energy, and it can be exploited by thermoelectronics to produce electrical power or electrical responses. The search for a low-cost thermoelectric material that could achieve high efficiencies and can also be straightforwardly scalable has turned significant attention to the halide perovskite family. Here, we report the thermal voltage response of bismuth-based perovskite derivates and suggest a path to increase the electrical conductivity by applying chalcogenide doping. The films were produced by drop-casting or spin coating, and sulfur was introduced in the precursor solution using bismuth triethylxanthate. The physical-chemical analysis confirms the substitution. The sulfur introduction caused resistivity reduction by 2 orders of magnitude, and the thermal voltage exceeded 40 mV K-1 near 300 K in doped and undoped bismuth-based perovskite derivates. X-ray diffraction, Raman spectroscopy, and grazing-incidence wide-angle X-ray scattering were employed to confirm the structure. X-ray photoelectron spectroscopy, elemental analysis, scanning electron microscopy, and energy-dispersive X-ray spectroscopy were employed to study the composition and morphology of the produced thin films. UV-visible absorbance, photoluminescence, inverse photoemission, and ultraviolet photoelectron spectroscopies have been used to investigate the energy band gap., Funding Agencies|H2020 Marie Sklodowska-Curie Actions [56338]; European Union [IESR3193231]; Royal Society International Exchanges Award; Fondo di Ateneo Quota Competitiva [2023-ATEQC-0078]; Innovate UK; National Recovery and Resilience Plan (NRRP) Mission 4 Component 2 Investment Line 1.5 [UF140372, URF/R/201013]

The surge in the number of distributed microelectronics and sensors requires versatile, scalable, and affordable power sources. Heat-harvesting organic thermoelectric generators (TEGs) are regarded as potential key components of the future energy landscape. Recent advances in the performance of organic thermoelectric materials have made practical applications of organic TEGs more feasible than ever before, yet the challenges of designing and fabricating organic TEGs suitable for real scenarios are scarcely addressed. Specifically, small sensors and wearables demand for micro-thermoelectric generators (mu TEGs) with high power density architectures and small form factors, while typical demonstrations of organic TEGs are characterized by < 10 thermocouples (TCs) per cm(2). This work presents a rolled, organic mu TEG architecture combining large-area, solution-based deposition techniques, such as inkjet and spray-coating, and an ultrathin parylene substrate to achieve a thermocouple density of 1842 TCs cm(-2). Such demonstrative mu TEG reaches a thermoelectric conversion performance of 0.15 mu W cm(-2) at Delta T = 50 K. Such power output is well in line with finite element method simulations, which highlight the benefit of the architecture and show that remarkable power densities, in the mW cm(-2) range at Delta T = 10 K, are realistically achievable with geometrical improvements and already ongoing advancements in organic thermoelectric inks., Funding Agencies|H2020 Marie Sklstrok;odowska-Curie Actions [955837 - HORATES]

Organic semiconductors are increasingly being decorated with hydrophilic solubilising chains to create materials that can function as mixed ionic-electronic conductors, which are promising candidates for interfacing biological systems with organic electronics. While numerous organic semiconductors, including p- and n-type materials, small molecules and polymers, have been successfully tailored to encompass mixed conduction properties, common to all these systems is that they have been semicrystalline materials. Here, we explore how side chain engineering in the nano-crystalline indacenodithiophene-co-benzothiadiazole (IDTBT) polymer can be used to instil ionic transport properties and how this in turn influences the electronic transport properties. This allows us to ultimately assess the mixed ionic-electronic transport properties of these new IDTBT polymers using the organic electrochemical transistor as the testing platform. Using a complementary experimental and computational approach, we find that polar IDTBT derivatives can be infiltrated by water and solvated ions, they can be electrochemically doped efficiently in aqueous electrolyte with fast doping kinetics, and upon aqueous swelling there is no deterioration of the close interchain contacts that are vital for efficient charge transport in the IDTBT system. Despite these promising attributes, mixed ionic-electronic charge transport properties are surprisingly poor in all the polar IDTBT derivatives. Albeit a "negative" result, this finding clearly contradicts established side chain engineering rules for mixed ionic-electronic conductors, which motivated our continued investigation of this system. We eventually find this anomalous behaviour to be caused by increasing energetic disorder in the polymers with increasing polar side chain content. We have investigated computationally how the polar side chain motifs contribute to this detrimental energetic inhomogeneity and ultimately use the learnings to propose, Funding Agencies|European Commission [964677, 2.5020.11]; European Commission Horizon 2020 Future and Emerging Technologies (FET) [1117545]; Walloon Region; National Science Foundation [DMR-1751308]; NSF [DE-AC02-06CH11357]; DOE Office of Science by Argonne National Laboratory

Heat is an inexhaustible source of energy, and it can be exploited by thermoelectronics to produce electrical power or electrical responses. The search for a low-cost thermoelectric material that could achieve high efficiencies and can also be straightforwardly scalable has turned significant attention to the halide perovskite family. Here, we report the thermal voltage response of bismuth-based perovskite derivates and suggest a path to increase the electrical conductivity by applying chalcogenide doping. The films were produced by drop-casting or spin coating, and sulfur was introduced in the precursor solution using bismuth triethylxanthate. The physical-chemical analysis confirms the substitution. The sulfur introduction caused resistivity reduction by 2 orders of magnitude, and the thermal voltage exceeded 40 mV K-1 near 300 K in doped and undoped bismuth-based perovskite derivates. X-ray diffraction, Raman spectroscopy, and grazing-incidence wide-angle X-ray scattering were employed to confirm the structure. X-ray photoelectron spectroscopy, elemental analysis, scanning electron microscopy, and energy-dispersive X-ray spectroscopy were employed to study the composition and morphology of the produced thin films. UV-visible absorbance, photoluminescence, inverse photoemission, and ultraviolet photoelectron spectroscopies have been used to investigate the energy band gap.