The development of rechargeable lithium-ion battery (LIB) technology has facilitated the shift toward electric vehicles and grid storage solutions. This technology is currently undergoing significant development to meet industrial applications for portable electronics and provide our society with "greener" electricity. The large increase in LIB production following the growing demand from the automotive sector has led to the establishment of gigafactories worldwide, thus increasing the substantial consumption of fossil-based and non-sustainable materials, such as polyvinylidene fluoride and/or styrene-butadiene rubber as binders in cathode and anode formulations. Furthermore, the use of raw resources, such as Li, Ni, and Mn in cathode active materials and graphite and nanosilicon in anodes, necessitates further efforts to enhance battery efficiency. To foster a global sustainable transition in LIB manufacturing and reduce reliance on non-sustainable materials, the implementation of bio-based binder solutions for electrodes in LIBs is crucial. Bio-based binders such as cellulose, lignin, alginate, gums, starch, and others can address environmental concerns and can enhance LIBs' performance. This review aims to provide an overview of the current progress in the development and application of bio-based binders for LIB electrode manufacturing, highlighting their significance toward sustainable development.

Due to growing concerns about the environmental impacts of fossil fuels and the capacity and resilience of energy grids around the world, engineers and policymakers are increasingly turning their attention to energy storage solutions1. In turn, the huge demand for materials for such storage systems will require a considerable energy input in extraction, processing and materials formulation, and new and sustainable electrochemical systems need to be developed2. Current report is the result of the exploration work where the circularity and environmental potentials of biobased energy storage solutions were analysed in the form of iterative interviews with stakeholders along the energy storage and packaging value chains, complemented by literature research. The work was performed within the scope of Digital Cellulose Center (DCC) research center3 in the sub-project 1 “Circularity of DCC materials” of the Theme 1: Design for a circular bioeconomy. Totally three systems were selected and analysed in the form of three respective case studies: • Case study I: Biobased battery (Chemical energy storage system) • Case study II: Biobased printed supercapacitor (Electrochemical energy storage system) • Case study III: Intelligent packaging (Chemical or electrochemical energy storage for fiber-based packaging) Each case study was put into the life cycle context where aspects such as legislation, circularity potential and potential environmental impact were discovered. The biobased battery for large-scale grid storage applications was classified as an industrial battery with collection rate requirement of 75% at end-of-life, of which 50% to be materially recycled. The biobased printed supercapacitor was classified as an electric and electronic equipment (EEE) with collection rate requirement of 65%, of which recovery and recycling / preparing for reuse targets vary between 55% - 85% depending on application. The material recycling target for the fiber-based intelligent packaging is 85% since being perceived as a paper-based packaging it would enter paper packaging recycling stream rather than entering the recycling stream of Waste electrical and electronic equipment (WEEE). In next steps of this exploratory journey, the compositions of the respective energy storage solutions were identified, including biobased content and recycling potential on the short- and long-term, compared to their benchmark solutions where possible. Today, the material recycling processes for batteries and WEEE are strongly economically driven: the material components that are considered as valuable by recyclers are mainly base metals (e.g., aluminium, steel) and to low extent critical raw materials (e.g., cobalt, nickel). The biobased energy storage solutions though do not contain any critical raw materials and use base metals to a less extent. This is a dilemma where the material value of the biobased, renewable materials (more sustainable materials by origin) is not favourable in the end-of-life processes of today and therefore will be lost (i.e., incinerated). A more balanced approach to such dilemma is urged in order to facilitate both economic and environmental incentives in the energy storage value cycles. Current Battery and WEEE directives do not promote the recycling of materials that are critical or have a high environmental burden, which in practice results in loss of those materials, not least due to lack of economy in recycling processes. Moreover, the legislation needs to be adapted in order to meet innovative development in the area. It can be relevant to introduce a cross-sectoral category ‘Biobased energy storage solutions’ in the upcoming legislation with the aim to encourage use of more abundant, biobased materials and thus decouple energy storage applications from use of critical raw materials.

A single coating formulation for multifunctional composites, such as a gas barrier against both oxygen and water vapour, is the holy grail for the packaging industry. Since the last decade, graphene has been touted as the ideal barrier material in composites due to its morphology and impermeability to all gases. However, this prospect is limited by either poor dispersion of graphene or excess surfactants to aid the dispersion, both leading to shortcuts that allow gas permeation through the composite. Here, we demonstrate a combined gas barrier with starch-graphene composite films made from a single formulation of surfactant-free starch nanoparticle-stabilized graphene dispersion (2.97 mg mL−1). Hence, the incorporated graphene reduces the permeability of both the oxygen and the water vapour by over 70% under all the relative humidity conditions tested. Moreover, these films are foldable and electrically conductive (9.5 S m−1). Our surfactant-free approach of incorporating graphene into an industrially important biopolymer is highly relevant to the packaging industry, thus offering cost-effective and water-based solution depositions of multifunctional composite films for wide-ranging applications, such as gas barriers in food packaging. © 2022, The Author(s).

A general formulation engineering method is adopted in this study to produce a highly concentrated (≈3 mg mL−1) inkjet printable starch–graphene ink in aqueous media. Photonic annealing of the starch–graphene ink is validated for rapid post-processing of printed films. The experimental results demonstrate the role of starch as dispersing agent for graphene in water and photonic pulse energy in enhancing the electrical properties of the printed graphene patterns, thus leading to an electrical conductivity of ≈2.4 × 104 S m−1. The curing mechanism is discussed based on systematic material studies. The eco-friendly and cost-efficient approach presented in this work is of technical potential for the scalable production and integration of conductive graphene inks for widespread applications in printed and flexible electronics. 

Developing high specific energy Lithium-ion (Li-ion) batteries is of vital importance to boost the production of efficient electric vehicles able to meet the customers’ expectation related to the electric range of the vehicle. One possible pathway to high specific energy is to increase the operating voltage of the Li-ion cell. Cathode materials enabling operation above 4.2 V are available. The stability of the positive electrode-electrolyte interface is still the main bottleneck to develop high voltage cells. Moreover, important research efforts are devoted to the substitution of graphite anodes with Li metal: this would improve the energy density of the cell dramatically. The use of metallic lithium is prevented by the dendrite growth during charge, with consequent safety problems. To suppress the formation of dendrites solid-state electrolytes are considered the most promising approach. For these reasons the present review summarizes the most recent research efforts in the field of high voltage solid-state electrolytes for high energy density Li-ion cells.

Attention to graphene dispersions in water with the aid of natural polymers is increasing with improved awareness of sustainability. However, the function of biopolymers that can act as dispersing agents in graphene dispersions is not well understood. In particular, the use of starch to disperse pristine graphene materials deserves further investigation. Here, we report the processing conditions of aqueous graphene dispersions using unmodified starch. We have found that the graphene content of the starch-graphene dispersion is dependent on the starch fraction. The starch-graphene sheets are few-layer graphene with a lateral size of 3.2 μm. Furthermore, topographical images of these starch-graphene sheets confirm the adsorption of starch nanoparticles with a height around 5 nm on the graphene surface. The adsorbed starch nanoparticles are ascribed to extend the storage time of the starch-graphene dispersion up to 1 month compared to spontaneous aggregation in a nonstabilized graphene dispersion without starch. Moreover, the ability to retain water by starch is reduced in the presence of graphene, likely due to environmental changes in the hydroxyl groups responsible for starch-water interactions. These findings demonstrate that starch can disperse graphene with a low oxygen content in water. The aqueous starch-graphene dispersion provides tremendous opportunities for environmental-friendly packaging applications. © 2021 American Chemical Society.

Nanocellulose (NC)-based hybrid coatings and films containing CeO2 and SiO2 nanoparticles (NPs) to impart UV screening and hardness properties, respectively, were prepared by solvent casting. The NC film-forming component (75 wt % of the overall solids) was composed entirely of cellulose nanocrystals (CNCs) or of CNCs combined with cellulose nanofibrils (CNFs). Zeta potential measurements indicated that the four NP types (CNC, CNF, CeO2, and SiO2) were stably dispersed in water and negatively charged at pH values between 6 and 9. The combination of NPs within this pH range ensured uniform formulations and homogeneous coatings and films, which blocked UV light, the extent of which depended on film thickness and CeO2 NP content, while maintaining good transparency in the visible spectrum (∼80%). The addition of a low amount of CNFs (1%) reduced the film hardness, but this effect was compensated by the addition of SiO2 NPs. Chiral nematic self-assembly was observed in the mixed NC film; however, this ordering was disrupted by the addition of the oxide NPs. The roughness of the hybrid coatings was reduced by the inclusion of oxide NPs into the NC matrix perhaps because the spherical oxide NPs were able to pack into the spaces between cellulose fibrils. We envision these hybrid coatings and films in barrier applications, photovoltaics, cosmetic formulations, such as sunscreens, and for the care and maintenance of wood and glass surfaces, or other surfaces that require a smooth, hard, and transparent finish and protection from UV damage.

Nanoporous zirconia with high surface area and crystallinity has a wide range of industrial applications, such as in inorganic exchangers for ion exchange columns, catalyst substrates, and packing material for HPLC. Spherical particles of crystalline nanoporous zirconia are highly desired in various industries due to easy handling of the materials in a fluidized bed. Here, spray drying was adopted to produce spherical nanoporous zirconia powders in both laboratory scale and pilot plant scale. Effect of salts on spray-dried ZrO2 powders and their crystallization behavior was studied. It was found that addition of salts to the zirconia precursors has a huge effect on the crystallization of nanoporous zirconia powders. These results have a great impact on the development of microspheres of nanocrystalline ZrO2 and potentially open up a new opportunity to the low-cost production of porous ceramic microspheres with the salt templating method, in general.

Colloidal dispersions of cerium oxide nanoparticles are of importance for numerous applications including as catalysts, chemical mechanical polishing agents and additives for UV protective and anticorrosion coatings. Here, concentrated oleate-coated cerium oxide nanoparticles (CeO2 NPs) with a uniform size have been produced by solventless thermolysis of cerium-oleate powder under low pressure at 320 °C and subsequently dispersed in hexane. Unlike any previously reported colloidal synthesis process for ceria nanoparticles, this process does not involve any toxic high boiling point organic solvent that requires subsequent removal at high cost. Although the process is very simple, highly concentrated cerium oxide nanoparticles with more than 17 wt% solid content and 70% of the theoretical yield can be easily obtained. Moreover, the size, shape and crystallinity of cerium oxide nanoparticles can be tailored by changing the thermal decomposition temperature and reaction time. Moreover, the new synthesis route developed in this study allows the synthesis of clean and dispersible ceria nanoparticles at a relatively low cost in a single step. The prepared ceria nanoparticles have an excellent UV absorption property and remain transparent to visible light, thus having the potential to replace potentially hazardous organic compounds in UV absorbing clear coatings. As a proof of concept, the prepared dispersions of cerium oxide nanoparticles in hexane were formulated into a solvent borne binder base to develop clear UV protecting coatings for light sensitive substrates. The general synthesis strategy presented in this study is generally applicable for the low-cost production of a concentrated dispersion of metal oxide nanoparticles with minimal environmental impact.

Nanocomposite coatings are of great interest as barrier coatings since synergy effects between matrix and additive properties can be achieved. This, however, requires favorable additive-matrix interactions to provide a strong interphase (interface region). In this work we elucidate the properties of two environmentally benign nanocomposite coatings based on a waterborne acrylate formulation with additives from renewable sources, i.e. either cellulose nanocrystals, CNC; or, alternatively, cellulose nanofibrils, CNF. We focus on the corrosion protective properties of these coatings and discuss the reason why the nanocomposite with CNC displays favorable corrosion protection properties whereas that with CNF does not. To this end we utilized scanning electron microscopy, water contact angle measurement, Fourier transform infrared spectroscopy and electrochemical impedance spectroscopy techniques to investigate the microstructure, surface wetting, interactions between cellulosic materials and matrix as well as corrosion protective properties of both composite coatings.