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A common way of determining the majority charge carriers of pristine and doped semiconducting polymers is to measure the sign of the Seebeck coefficient. However, a polarity change of the Seebeck coefficient has recently been observed to occur in highly doped polymers. Here, it is shown that the Seebeck coefficient inversion is the result of the density of states filling and opening of a hard Coulomb gap around the Fermi energy at high doping levels. Electrochemical n‐doping is used to induce high carrier density (>1 charge/monomer) in the model system poly(benzimidazobenzophenanthroline) (BBL). By combining conductivity and Seebeck coefficient measurements with in situ electron paramagnetic resonance, UV–vis–NIR, Raman spectroelectrochemistry, density functional theory calculations, and kinetic Monte Carlo simulations, the formation of multiply charged species and the opening of a hard Coulomb gap in the density of states, which is responsible for the Seebeck coefficient inversion and drop in electrical conductivity, are uncovered. The findings provide a simple picture that clarifies the roles of energetic disorder and Coulomb interactions in highly doped polymers and have implications for the molecular design of next‐generation conjugated polymers. [ABSTRACT FROM AUTHOR]

Organic electrochemical transistors (OECTs) have the potential to revolutionize the field of organic bioelectronics. To date, most of the reported OECTs include p‐type (semi‐)conducting polymers as the channel material, while n‐type OECTs are yet at an early stage of development, with the best performing electron‐transporting materials still suffering from low transconductance, low electron mobility, and slow response time. Here, the high electrical conductivity of multi‐walled carbon nanotubes (MWCNTs) and the large volumetric capacitance of the ladder‐type π‐conjugated redox polymer poly(benzimidazobenzophenanthroline) (BBL) are leveraged to develop n‐type OECTs with record‐high performance. It is demonstrated that the use of MWCNTs enhances the electron mobility by more than one order of magnitude, yielding fast transistor transient response (down to 15 ms) and high μC* (electron mobility × volumetric capacitance) of about 1 F cm−1 V−1 s−1. This enables the development of complementary inverters with a voltage gain of >16 and a large worst‐case noise margin at a supply voltage of <0.6 V, while consuming less than 1 µW of power. [ABSTRACT FROM AUTHOR]

Conducting polymers, such as the p-doped poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have enabled the development of an array of opto- and bio-electronics devices. However, to make these technologies truly pervasive, stable and easily processable, n-doped conducting polymers are also needed. Despite major efforts, no n-type equivalents to the benchmark PEDOT:PSS exist to date. Here, we report on the development of poly(benzimidazobenzophenanthroline):poly(ethyleneimine) (BBL:PEI) as an ethanol-based n-type conductive ink. BBL:PEI thin films yield an n-type electrical conductivity reaching 8 S cm−1, along with excellent thermal, ambient, and solvent stability. This printable n-type mixed ion-electron conductor has several technological implications for realizing high-performance organic electronic devices, as demonstrated for organic thermoelectric generators with record high power output and n-type organic electrochemical transistors with a unique depletion mode of operation. BBL:PEI inks hold promise for the development of next-generation bioelectronics and wearable devices, in particular targeting novel functionality, efficiency, and power performance. The development of n-type conductive polymer inks is critical for the development of next-generation opto-electronic devices that rely on efficient hole and electron transport. Here, the authors report an alcohol-based, high performance and stable n-type conductive ink for printed electronics. [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]