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.

Novel printed electronics are projected to grow and be manufactured in the future in large volumes. In many applications, printed electronics are envisaged as sustainable alternatives to conventional (PCB-based) electronics. One such application is in the semi-quantitative drug detection and point-of-care device called ‘GREENSENSE’ that uses paper-based printed electronics. This paper analyses the carbon footprint of GREENSENSE in order to identify and suggest means of mitigating disproportionately high environmental impacts, labeled ‘sustainability hotspots’, from materials and processes used during production which would be relevant in high-volume applications. Firstly, a life cycle model traces the flow of raw materials (such as paper, CNCs, and nanosilver) through the three ‘umbrella’ processes (circuit printing, component mounting, and biofunctionalization) manufacturing different electronic components (the substrate, conductive inks, energy sources, display, etc) that are further assembled into GREENSENSE. Based on the life cycle model, life cycle inventories are modeled that map out the network of material and energy flow throughout the production of GREENSENSE. Finally, from the environmental impact and sustainability hotspot analysis, both crystalline nanocellulose and nanosilver were found to create material hotspots and they should be replaced in favor of lower-impact materials. Process hotspots are created by manual, lab-, and pilot-scale processes with unoptimized material consumption, energy use, and waste generation; automated and industrial-scale manufacturing can mitigate such process hotspots. © 2023 The Author(s).

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.

Measuring the size of cellulose nanomaterials can be challenging, especially in the case of branched and entangled cellulose nanofibrils (CNFs). The International Organization for Standardization, Technical Committee 6, Task Group 1—Cellulosic Nanomaterials, is exploring opportunities to develop standard methods for the measurement of CNF particle size and particle size distribution. This paper presents a summary of the available measuring techniques, responses from a survey on the measurement needs of CNF companies and researchers, and outcomes from an international workshop on cellulose nanofibril measurement and standardization. Standardization needs differed among groups, with Japanese companies mostly requiring measurements for product specification and production control, and other companies mostly needing measurements for safety/regula-tory purposes and for grade definitions in patents. Among all the companies, average length and width with percen-tiles (D(10), D(50), D(90)) were the most desired measurands. Workshop participants concurred that defining the location(s) on the CNF at which to measure the width and the length is an urgent and complex question. They also agreed that methods are needed for rapid particle size measurement at the nanoscale. Our recommendation within ISO is to start work to revise the definition of CNFs and develop sample preparation and measurement guidelines. It was also recommended that further research be done to reproducibly prepare hierarchical branched CNF structures and characterize them, develop automated image analysis for hierarchical branched CNF structures, and develop a classification system encompassing measurements at multiple size ranges from micro-to nanoscale to fully characterize and distinguish CNF samples. 00327-2022 

Nanocelluloses are anisotropic nanoparticles of semicrystalline assemblies of glucan polymers. They have great potential as renewable building blocks in the materials platform of a more sustainable society. As a result, the research on nanocellulose has grown exponentially over the last decades. To fully utilize the properties of nanocelluloses, a fundamental understanding of their colloidal behavior is necessary. As elongated particles with dimensions in a critical nanosize range, their colloidal properties are complex, with several behaviors not covered by classical theories. In this comprehensive Review, we describe the most prominent colloidal behaviors of nanocellulose by combining experimental data and theoretical descriptions. We discuss the preparation and characterization of nanocellulose dispersions, how they form networks at low concentrations, how classical theories cannot describe their behavior, and how they interact with other colloids. We then show examples of how scientists can use this fundamental knowledge to control the assembly of nanocellulose into new materials with exceptional properties. We hope aspiring and established researchers will use this Review as a guide. © 2023 The Authors. 

Cellulose is the most abundant organic material on our planet which has a key role in our daily life (e.g., paper, packaging). In recent years, the need for replacing fossil-based materials has expanded the application of cellulose and cellulose derivatives including into electronics and sensing. The combination of nanostructures with cellulose nanofibers (CNFs) is expected to create new opportunities for the development of innovative electronic devices. In this paper, we report on a single-step process for the low temperature (<100 °C), environmentally friendly, and fully scalable CNF-templated highly dense growth of zinc oxide (ZnO) nanorods (NRs). More specifically, the effect of the degree of substitution of the CNF (enzymatic CNFs and carboxymethylated CNFs with two different substitution levels) on the ZnO growth and the application of the developed ZnO NRs/CNF nanocomposites in the development of UV sensors is reported herein. The results of this investigation show that the growth and nature of ZnO NRs are strongly dependent on the charge of the CNFs; high charge promotes nanorod growth whereas with low charge, ZnO isotropic microstructures are created that are not attached to the CNFs. Devices manufactured via screen printing/drop-casting of the ZnO NRs/CNF nanocomposites demonstrate a good photo-sensing response with a very stable UV-induced photocurrent of 25.84 µA. This also exhibits excellent long-term stability with fast ON/OFF switching performance under the irradiance of a UV lamp (15 W). 

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.

Research in smart textiles is growing due to the increased demand from the healthcare sector and people's urge to keep track of and analyze the signals and metrics from their bodies. Electrically conductive filaments are the most fundamental material for smart textiles. These filaments can be imbued with functionalities and useful in fields like energy storage, sensing, and actuation. To be able to meet the requirements that the latter applications require, fabrication techniques must be developed to provide better processability and sustainability in a cost-effective manner. Here, a mixture of a conductive polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), and biobased cellulose nanofibrils (CNFs) was used to spin filaments utilizing a water-based process. These filaments show electrical conductivities up to 150 S/cm and tensile stiffness of 20 GPa. Interestingly, the PEDOT aligned to a similar degree as the CNFs during the spinning process without a drawing step, which is hypothesized to be caused by the attachment of PEDOT on the CNFs. Lastly, the filaments were tested in an organic electrochemical transistor (OECT) configuration, which resulted in a working device with an on/off ratio approaching 1500. Furthermore, the OECT exhibited stable behavior when changing temperature (20-80 °C) and relative humidity (40-80%). This aqueous spinning method, resulting in filaments with robust electronic properties in different temperature and humidity environments, show greats promise for future innovative smart textiles.

A new gel polymer electrolyte (GPE) based supercapacitor with an ionic conductivity up to 0.32–0.94 mS cm−2 has been synthesized from a mixture of an ionic liquid (IL) with nanocellulose (NC). The new NC-ionogel was prepared by combining the IL 1-ethyl-3-methylimidazolium dimethyl phosphate (EMIMP) with carboxymethylated cellulose nanofibers (CNFc) at different ratios (CNFc ratio from 1 to 4). The addition of CNFc improved the ionogel properties to become easily printable onto the electrode surface. The new GPE based supercapacitor cell showed good electrochemical performance with specific capacitance of 160 F g−1 and an equivalent series resistance (ESR) of 10.2 Ω cm−2 at a current density of 1 mA cm−2. The accessibility to the full capacitance of the device is demonstrated after the addition of CNFc in EMIMP compared to the pristine EMIMP (99 F g−1 and 14.7 Ω cm−2). © 2022 by the authors.