Sustainable electrical energy storage is one of the most important scientific endeavors of this century. Battery and supercapacitor technologies are here crucial, but typically the current state of the art suffers from either lack of large-scale production possibilities, sustainability or insufficient performance and hence cannot match growing demands in society. Paper and cellulosic materials are mature scalable templates for industrial roll-to-roll production. Organic materials, such as conducting polymers, and carbon derivatives are materials that can be synthesized or derived from abundant sources. Here, we report the combination of cellulose, PEDOT:PSS and carbon derivatives for bulk supercapacitor electrodes adapted for printed electronics. Cellulose provides a mesoscopic mesh for the organization of the active ingredients. Furthermore, the PEDOT:PSS in combination with carbon provides superior device characteristics when comparing to the previously standard combination of activated carbon and carbon black. PEDOT:PSS acts as a mixed ion-electron conducting glue, which physically binds activated carbon particles together, while at the same time facilitating swift transport of both electrons and ions. A surprisingly small amount (10%) of PEDOT:PSS is needed to achieve an optimal performance. This work shows that cellulose added to PEDOT:PSS-carbon enables high-performing, mechanically stable, printed supercapacitor electrodes using a combination of printing methods.

Conventional electronics have been highlighted as a very unsustainable technology; hazardous wastes are produced both during their manufacturing but also, due to their limited recyclability, during their end of life cycle (e.g. disposal in landfill). In recent years additive manufacturing processes (i.e. screen printing) have attracted significant interest as a more sustainable approach to electronic manufacturing (printed electronics). Despite the field of printed electronics addressing some of the issues related to the manufacturing of electronics, many components and inks are still considered hazardous to the environment and are difficult to recycle. Here we present the development of a low environmental impact carbon ink based on a non-hazardous solvent and a cellulosic matrix (nanocellulose) and its implementation in electrochromic displays (ECDs) and supercapacitors. As part of the reported work, a different protocol for mixing carbon and cellulose nanofibrils (rotation mixing and high shear force mixing), nanocellulose of different grades and different carbon: nanocellulose ratios were investigated and optimized. The rheology profiles of the different inks showed good shear thinning properties, demonstrating their suitability for screen-printing technology. The printability of the developed inks was excellent and in line with those of reference commercial carbon inks. Despite the lower electrical conductivity (400 S m-1 for the developed carbon ink compared to 1000 S m-1 for the commercial inks), which may be explained by their difference in composition (carbon content, density and carbon derived nature) compared to the commercial carbon, the developed ink functioned adequately as the counter electrode in all screen-printed ECDs and even allowed for improved supercapacitors compared to those utilizing commercial carbon inks. In this sense, the supercapacitors incorporating the developed carbon ink in the current collector layer had an average capacitance = 97.4 mF cm-2 compared to the commercial carbon ink average capacitance = 61.6 mF cm-2. The ink development reported herein provides a step towards more sustainable printed green electronics. © 2021 The Author(s).

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. © 2022 The Author(s). 

Large area manufacturing of printed electronic components on ~A4-sized substrates is demonstrated by the combination of screen printing and vapor phase polymerization (VPP) into poly(3,4-ethylenedioxythiophene) (PEDOT). The oxidant layer required for the polymerization process is screen printed, and the resulting conductive polymer patterns are manufactured at high resolution (100 µm). Successful processing of several common oxidant species is demonstrated, and the thickness can be adjusted by altering the polymerization time. By comparing the polymer films of this work to a commercial PEDOT:PSS (PEDOT doped with poly(styrene sulfonate)) screen printing ink shows improved surface roughness (26 vs 69 nm), higher conductivity (500 vs 100 S cm–1) and better resolution (100 vs 200 µm). Organic electrochemical transistors, in which the transistor channel is polymerized into PEDOT through VPP, are also demonstrated to further emphasize on the applicability of this manufacturing approach. The resulting transistor devices are not only functional, they also show remarkable switching behavior with respect to ON current levels (–70 mA at –1 V), ON/OFF ratios (>105), switching times (tens of ms) and transconductance values (>100 mS) in standalone transistor devices, in addition to a high amplification factor (>30) upon integration into a screen printed inverter circuit. © 2022 The Authors. 

Nanostructured wood veneer with added electroactive functionality combines structural and functional properties into eco-friendly, low-cost nanocomposites for electronics and energy technologies. Here, we report novel conducting polymer-impregnated wood veneer electrodes where the native lignin is preserved, but functionalized for redox activity and used as an active component. The resulting electrodes display a well-preserved structure, redox activity, and high conductivity. Wood samples were sodium sulfite-treated under neutral conditions at 165 °C, followed by the tailored distribution of PEDOT:PSS, not previously used for this purpose. The mild sulfite process introduces sulfonic acid groups inside the nanostructured cell wall, facilitating electrostatic interaction on a molecular level between the residual lignin and PEDOT. The electrodes exhibit a conductivity of up to 203 S m−1 and a specific pseudo-capacitance of up to 38 mF cm−2, with a capacitive contribution from PEDOT:PSS and a faradaic component originating from lignin. We also demonstrate an asymmetric wood pseudo-capacitor reaching a specific capacitance of 22.9 mF cm−2 at 1.2 mA cm−2 current density. This new wood composite design and preparation scheme will support the development of wood-based materials for use in electronics and energy storage.