Lignin, a central renewable carbon resource in the biosphere, has recently emerged as a promising redox-active material for organic batteries. Currently, the main challenge lies in finding a form of lignin that combines water-based processability with good cyclic stability, as the two industrially common forms, kraft lignin and lignosulfonate, each offers only one of these advantages. In this work, we demonstrate that lignin nanoparticles (LNPs) act as redox-active centers that are insoluble but exhibit colloidal stability in aqueous media, allowing for straightforward processing into electrodes for zinc-ion batteries. Electrodes based on conductive composites of LNPs with poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) were shown electrochemically to achieve specific capacities reaching 42.5 mAh/g at a current density of 1 A/g. A zinc-ion battery prototype using this composite demonstrated a specific energy of 54 Wh/kg, outperforming previous lignin-based energy storage devices. This zinc-lignin battery exhibited excellent Coulombic efficiency of around 100%, with a specific capacity of 82.5 mAh/g at 0.05 A/g and a capacity retention of approximately 61% after 2000 charge/discharge cycles. Our results highlight the potential of LNPs in advancing eco-friendly, cost-effective, and high-performance lignin-based energy storage devices.

Lignin has been extensively researched as a cathode active material in secondary batteries. In the present work, the energy storage potential of lignin naturally present in papers made of softwood chemi-thermomechanical pulp (CTMP) is explored. More specifically, effects from softwood CTMP fines on the electrochemical characteristics have been studied. Compared to pulp fibers, fines are higher in lignin content and have higher specific surface area. It was expected that this would be positive for the electrode performance; however, the result points to the opposite. The fines do not significantly contribute to a higher lignin specific capacity, and they deteriorate the cycling stability. Higher fines content was found to result in a higher oxidative activity as well as more abundant competing reactions. These competing reactions are believed to be linked to the cycle stability. Therefore, we hypothesize that the electrochemical stability of lignin can be better understood by studying differences between fines and fiber lignin. As the theoretical specific capacity of this material is about 20 times larger than obtained here, identification of the reasons for this capacity discrepancy is needed to realize the full potential of lignin-based paper batteries.

The redox-diffusion (RD) battery concept introduces an environmentally friendly solution for stretchable batteries in autonomous wearable electronics. By utilising plant-based redox-active biomolecules and cellulose fibers for the electrode scaffold, separator membrane, and current collector, along with a biodegradable elastomer encapsulation, the battery design overcomes the reliance on unsustainable transition metal-based active materials and non-biodegradable elastomers used in existing stretchable batteries. Importantly, it addresses the drawback of limited attainable battery capacity, where increasing the active material loading often leads to thicker and stiffer electrodes with poor mechanical properties. The concept decouples the active material loading from the mechanical structure of the electrode, enabling high mass loadings, while retaining a skin-like young's modulus and stretchability. A stretchable ion-selective membrane facilitates the RD process, allowing two separate redox couples, while preventing crossovers. This results in a high-capacity battery cell that is both electrochemically and mechanically stable, engineered from sustainable plant-based materials. Notably, the battery components are biodegradable at the end of their life, addressing concerns of e-waste and resource depletion. A stretchable battery design that uses sustainable plant-based materials and enables high electrochemical and mechanical performance and is biodegradable at the end-of-life.

Printed electronic paper identifies its interest in flexible organic electronics and sustainable and clean energy applications because of its straightforward production method, cost-effectiveness, and positive environmental impact. However, current limitations include restricted material thickness and the use of supporting substrate for printing. Here, 2D and 3D electronic patterned paper are fabricated from direct ink writing (DIW) nanocellulose and PEDOT:PSS-based materials using syringe deposition and 3D printing. The conductor patterns are integrated in the bulk of the paper, while non-conductive sections are used as support to form free-standing paper. The strong interface between the patterns of electronic patterned paper gives mechanical stability for practical handling. The conductive paper-based electrode has 202 S cm(-1) and is capable of handling electric current up to 0.7 A, which can be used for high-power devices. Printed supercapacitor papers show high specific energy of 4.05 Wh kg(-1), specific power of 4615 W kg(-1) at 0.06 A g(-1), and capacitance retention above 95% after 2000 cycles. The new design structure of electronic patterned papers presents a solution for additive manufacturing of paper-based composites for supercapacitors, wearable electronics, or sensors for smart packaging.

The nature of mass transport in plants has recently inspired the development of low-cost and sustainable wood-based electronics. Herein, we report a wood electrochemical transistor (WECT) where all three electrodes are fully made of conductive wood (CW). The CW is prepared using a two-step strategy of wood delignification followed by wood amalgamation with a mixed electron-ion conducting polymer, poly(3,4-ethylenedioxythiophene)–polystyrene sulfonate (PEDOT:PSS). The modified wood has an electrical conductivity of up to 69 Sm−1 induced by the formation of PEDOT:PSS microstructures inside the wood 3D scaffold. CW is then used to fabricate the WECT, which is capable of modulating an electrical current in a porous and thick transistor channel (1 mm) with an on/off ratio of 50. The device shows a good response to gate voltage modulation and exhibits dynamic switching properties similar to those of an organic electrochemical transistor. This wood-based device and the proposed working principle demonstrate the possibility to incorporate active electronic functionality into the wood, suggesting different types of bio-based electronic devices.

To address the rising need of sustainable solutions in electronic devices, the development of electronically conductive composites based on lightweight but mechanically strong wood structures is highly desirable. Here, a facile approach for the fabrication of highly conductive wood/polypyrrole composites through top-down modification of native lignin followed by polymerization of pyrrole in wood cell wall. By sodium sulfite treatment under neutral condition, sulfonated wood veneers with increased porosity but well-preserved cell wall structure containing native lignin and lignosulfonates are obtained. The wood structure has a content of sulfonic groups up to 343 mu mol g(-1) owing to in situ sulfonated lignin which facilitates subsequent oxidative polymerization of pyrrole, achieving a weight gain of polypyrrole as high as 35 wt%. The lignosulfonates in the wood structure act as dopant and stabilizer for the synthesized polypyrrole. The composite reaches a high conductivity of 186 S m(-1) and a specific pseudocapacitance of 1.71 F cm(-2) at the current density of 8.0 mA cm(-2). These results indicate that tailoring the wood/polymer interface in the cell wall and activating the redox activity of native lignin by sulfonation are important strategies for the fabrication of porous and lightweight wood/conductive polymer composites with potential for sustainable energy applications.

The need for achieving sustainable technologies has encouraged research on renewable and biodegradable materials for novel products that are clean, green, and environmentally friendly. Nanocellulose (NC) has many attractive properties such as high mechanical strength and flexibility, large specific surface area, in addition to possessing good wet stability and resistance to tough chemical environments. NC has also been shown to easily integrate with other materials to form composites. By combining it with conductive and electroactive materials, many of the advantageous properties of NC can be transferred to the resulting composites. Conductive polymers, in particular poly(3,4-ethylenedioxythiophene:poly(styrene sulfonate) (PEDOT:PSS), have been successfully combined with cellulose derivatives where suspensions of NC particles and colloids of PEDOT:PSS are made to interact at a molecular level. Alternatively, different polymerization techniques have been used to coat the cellulose fibrils. When processed in liquid form, the resulting mixture can be used as a conductive ink. This review outlines the preparation of NC/PEDOT:PSS composites and their fabrication in the form of electronic nanopapers, filaments, and conductive aerogels. We also discuss the molecular interaction between NC and PEDOT:PSS and the factors that affect the bonding properties. Finally, we address their potential applications in energy storage and harvesting, sensors, actuators, and bioelectronics.

Osmotic energy generated from the salinity gradient is a kind of clean and renewable energy source, where the ion-exchange membranes play a critical role in its operation. The nanofluidic technique is emerging to overcome the limitations of high resistance and low mass transport of traditional ion-exchange membranes and thus improve osmotic power conversion. However, the currently reported nanofluidic materials suffer from high cost and complicated fabrication processes, which limits their practical application. Here, we report low-cost nanocellulose membranes that can be facilely prepared by a chemical cross-linking approach. The obtained membranes exhibit excellent ion transport characteristics as high-performance nanofluidic osmotic power generators. The control of cross-linker dosage enables the simultaneous tunability of the surface charge density and size of nanofluidic channels created between the interwoven cellulose nanofibrils. The maximum osmotic power generated by the membrane is reached when the cross-linker weight content is 20 wt %. Furthermore, the cross-linked nanocellulose membranes exhibit long-term working stability in osmotic energy harvesting under a wide range of pH values (3.2-9.7). This nanocellulose membrane derived from green and sustainable natural materials demonstrates a promising potential for renewable osmotic energy harvesting.

Organic electronic circuits based on organic electrochemical transistors (OECTs) are attracting great attention due to their printability, flexibility, and low voltage operation. Inverters are the building blocks of digital logic circuits (e.g., NAND gates) and analog circuits (e.g., amplifiers). However, utilizing OECTs in electronic logic circuits is challenging due to the resulting low voltage gain and low output voltage levels. Hence, inverters capable of operating at relatively low supply voltages, yet offering high voltage gain and larger output voltage windows than the respective input voltage window are desired. Herein, inverters realized from poly(3,4-ethylenedioxythiophene):polystyrene sulfonate-based OECTs are designed and explored, resulting in logic inverters exhibiting high voltage gains, enlarged output voltage windows, and tunable switching points. The inverter designs are based on multiple screen-printed OECTs and a resistor ladder, where one OECT is the driving transistor while one or two additional OECTs are used as variable resistors in the resistor ladder. The inverters performances are investigated in terms of voltage gain, output voltage levels, and switching point. Inverters, operating at +/-2.5 V supply voltage and an input voltage window of 1 V, that can achieve an output voltage window with similar to 110% increment and a voltage gain up to 42 are demonstrated.

The global efforts in electrifying our society drive the demand for low-cost and sustainable energy storage solutions. In the present work, a novel material concept was investigated to enable fabrication of several 10 meter-long rolls of supercapacitor paper electrodes on a pilot-scale paper machine. The material concept was based on cationized, cellulose-rich wood-derived fibres, conducting polymer PEDOT:PSS, and activated carbon filler particles. Cationic fibres saturated with anionic PEDOT:PSS provide a conducting scaffold hosting the activated carbon, which functions as the active charge-storage material. The response from further additives was systematically investigated for several critical paper properties. Cellulose nanofibrils were found to improve mechanical properties, while carbon black enhanced both the conductivity and the storage capacity of the activated carbon, reaching a specific capacitance of 67 F g(-1). This pilot trial shows that "classical" papermaking methods are fit for the purpose and provides valuable insights on how to further advance bio-based energy storage solutions for large-scale applications.