With the increasing global demand for net-zero carbon emissions, actions to address climate change have gained momentum among policymakers and the public. The urgent need for a sustainable economy is underscored by the mounting waste crisis in landfills and oceans. However, the proliferation of distributed electronic devices poses a significant challenge due to the resulting electronic waste. To combat this issue, the development of sustainable and environmentally friendly materials for these devices is imperative. Cellulose, an abundant and CO2-neutral substance with a long history of diverse applications, holds great potential. By integrating electrically interactive components with cellulosic materials, innovative biobased composites have been created, enabling the fabrication of bulk electroactive paper and the establishment of new, potentially more sustainable manufacturing processes for electronic devices. This review explores recent advances in bulk electroactive paper, including the fundamental interactions between its constituents, manufacturing techniques, and large-scale applications in the field of electronics. Furthermore, it addresses the importance and challenges of scaling up production of electroactive paper, highlighting the need for further research and development.

The transition to a sustainable society is driving the development of green electronic solutions designed to have a minimal environmental impact. One promising route to achieve this goal is to construct electronics from biobased materials like cellulose, which is carbon neutral, non‐toxic, and recyclable. This is especially true for internet‐of‐things devices, which are rapidly growing in number and are becoming embedded in every aspect of our lives. Here, paper‐based sensor circuits are demonstrated, which use triboelectric pressure sensors to help elderly people communicate with the digital world using an interface in the form of an electronic “book”, which is more intuitive to them. The sensors are manufactured by screen printing onto flexible paper substrates, using in‐house developed cellulose‐based inks with non‐hazardous solvents. The triboelectric sensor signal, generated by the contact between a finger and chemically modified cellulose, can reach several volts, which can be registered by a portable microcontroller card and transmitted by Bluetooth to any device with an internet connection. Apart from the microcontroller (which can be easily removed), the whole system can be recycled at the end of life. A triboelectric touch interface, manufactured using printed electronics on flexible paper substrates, using cellulose‐based functional inks is demonstrated. These metal‐free green electronics circuits are implemented in an “electronic book” demonstrator, equipped with wireless communication that can control remote devices, as a step toward sustainable and recyclable internet‐of‐things devices.

Displays are one of the most mature technologies in the field of printed electronics. Their ability to be manufactured in large quantities and at low cost has led to their recent uptake into the consumer market. Within this article this technology is extended to electrochromic display stickers. This is achieved using a recent reverse display architecture screen printed on textile and paper sticker substrates. The electrochromic stickers are comparable to plastic control substrates and show little performance difference even when adhered to curved surfaces. The electrochromic display technology is extended to sticker labels for authentication applications by patterning either the dielectric or the graphical layer. A proof-of-concept prototype emulating a wax seal on an envelope is presented to show that other colors can be implemented in this technology. © 2023 The Authors.

Low-cost, flexible and thin display technology is becoming an interesting field of research as it can accompany the wide range of sensors being developed. Here, the synthesis of poly(dimethylpropylene-dioxythiophene) (PProDOT-Me2) by combining vapor phase polymerization and screen printing is presented. A multilayer architecture using poly(3,4-ethylenedioxythiophene) (PEDOT) and PProDOT-Me2 to allow for electrochromic switching of PProDOT-Me2, thereby eliminating the need for a supporting transparent conductive (metal oxide) layer is introduced. Furthermore, the technology is adapted to a blended architecture, which removes the additional processing steps and results in improved color contrast (∆E* > 25). This blend architecture is extended to other conductive polymers, such as PEDOT and polypyrrole (PPy), to highlight the ability of the technique to adjust the color of all-printed electrochromic displays. As a result, a green color is obtained when combining the blue and yellow states of PEDOT and PPy, respectively. This technology has the potential to pave the way for all-printed multicolored electrochromic displays for further utilization in printed electronic systems in various Internet of Things applications. © 2022 The Authors. 

Manufacturing of electronic devices via printing techniques is often considered to be an environmentally friendly approach, partially due to the efficient utilization of materials. Traditionally, printed electronic components (e.g., sensors, transistors, and displays) are relying on flexible substrates based on plastic materials; this is especially true in electronic display applications where, most of the times, a transparent carrier is required in order to enable presentation of the display content. However, plastic-based substrates are often ruled out in end user scenarios striving toward sustainability. Paper substrates based on ordinary cellulose fibers can potentially replace plastic substrates, but the opaqueness limits the range of applications where they can be used. Herein, electrochromic displays that are manufactured, via screen printing, directly on state-of-the-art fully transparent substrates based on nanocellulose are presented. Several different nanocellulose-based substrates, based on either nanofibrillated or nanocrystalline cellulose, are manufactured and evaluated as substrates for the manufacturing of electrochromic displays, and the optical and electrical switching performances of the resulting display devices are reported and compared. The reported devices do not require the use of metals and/or transparent conductive oxides, thereby providing a sustainable all-printed electrochromic display technology.

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. 

The rise of paper electronics has been accelerated due to the public push for sustainability. Electronic waste can potentially be avoided if certain materials in electronic components can be substituted for greener alternatives such as paper. Within this report, it is demonstrated that conductive polymers poly(3,4-ethylenedoxythiophene) (PEDOT), polypyrrole, and polythiophene, can be synthesized by screen printing combined with vapor phase polymerization on paper substrates and further incorporated into functional electronic components. High patterning resolution (100 µm) is achieved for all conductive polymers, with PEDOT showing impressive sheet resistance values. PEDOT is incorporated as conductive circuitry and as the active material in all-printed electrochromic displays. The conductive polymer circuits allow for functional light emitting diodes, while the electrochromic displays are comparable to commercial displays utilizing PEDOT on plastic substrates. 

By combining the electrochromic (EC) properties of Prussian blue (PB) and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS), complementary EC displays manufactured by slot-die coating and screen printing on flexible plastic substrates are reported. Various display designs have been realized, resulting in displays operating in either transmissive or reflective mode. For the transmission mode displays, the color contrast is enhanced by the complementary switching of the two EC electrodes PB and PEDOT:PSS. Both electrodes are either exhibiting a concurrent colorless or blue appearance. For the displays operating in reflection mode, a white opaque electrolyte is used in conjunction with the EC properties of PB, resulting in a display device switching between a fully white state and a blue-colored state. The developments of the different device architectures, that either operate in reflection or transmission mode, demonstrate a scalable manufacturing approach of all-printed EC displays that may be used in a large variety of Internet of Things applications. © 2022 The Authors. 

Paper electronics is a viable alternative to traditional electronics, leading to more sustainable electronics. Many challenges still require solutions before paper electronics become mainstream. Here, we present a solution to enable the manufacturing of reflective all-printed organic electrochromic displays (OECDs) on paper substrates; devices that are usually printed on transparent substrates, for example, plastics. In order to operate on opaque paper substrates, an architecture for reversely printed OECDs (rOECDs) is developed. In this architecture, the electrochromic layer is printed as the last functional layer and can therefore be viewed from the print side. Square shaped 1 cm2 rOECDs are successfully screen printed on paper, with a high manufacturing yield exceeding 99%, switching times <3 s and high color contrast (ΔE* > 27). Approximately 60% of the color is retained after 15 min in open-circuit mode. Compared to the conventional screen printed OECD architectures, the rOECDs recover approximately three times faster from storage in a dry environment, which is particularly important in systems where storage in low humidity atmosphere is required, for example, in many biosensing applications. Finally, a more complex rOECD with 9 individually addressable segments is successfully screen printed and demonstrated.

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 (&gt;105), switching times (tens of ms) and transconductance values (&gt;100 mS) in standalone transistor devices, in addition to a high amplification factor (&gt;30) upon integration into a screen printed inverter circuit. © 2022 The Authors.