Large-Scale Compatible Roll-to-Roll Coating of Paper Electrodes and Their Compatibility as Lithium-Ion Battery Anodes

A recyclability perspective is essential in the sustainable development of energy storage devices, such as lithium-ion batteries (LIBs), but the development of LIBs prioritizes battery capacity and energy density over recyclability, and hence, the recycling methods are complex and the recycling rate is low compared to other technologies. To improve this situation, the underlying battery design must be changed and the material choices need to be made with a sustainable mindset. A suitable and effective approach is to utilize bio-materials, such as paper and electrode composites made from graphite and cellulose, and adopt already existing recycling methods connected to the paper industry. To address this, we have developed a concept for fabricating fully disposable and resource-efficient paper-based electrodes with a large-scale roll-to-roll coating operation in which the conductive material is a nanographite and microcrystalline cellulose mixture coated on a paper separator. The overall best result was achieved with coated roll 08 with a coat weight of 12.83(22) g/m² and after calendering, the highest density of 1.117(97) g/cm³, as well as the highest electrical conductivity with a resistivity of 0.1293(17) mΩ·m. We also verified the use of this concept as an anode in LIB half-cell coin cells, showing a specific capacity of 147 mAh/g, i.e., 40% of graphite's theoretical performance, and a good long-term stability of battery capacity over extended cycling. This concept highlights the potential of using paper as a separator and strengthens the outlook of a new design concept wherein paper can both act as a separator and a substrate for coating the anode material.