Association and diffusion of Li+ in carboxymethylcellulose solutions with application to environmentally friendly Li-ion batteries: a combined Molecular Dynamics and NMR study

Carboxymethylcellulose (CMC) has been proposed as a polymeric binder for the electrodes in environmentally friendly Li-ion batteries. Its physical properties and interaction with Li+ ions in water are interesting from the point of view of electrode preparationprocessability in water is one of the main reasons for its environmental friendlinessbut also for its possible application in aqueous Li-ion batteries. We combine MD simulations and variable-time PFGSE-NMR spectroscopy to investigate Li+ transport in CMC-based solutions. Both simulation and experiment show that, at concentrations such that Li-CMC has a gel like consistency, the Li+ diffusion coefficient is still very close to that in water. These ions interact preferentially with CMC’s carboxylate groups, giving rise to a rich variety of coordination patterns. However, the diffusion of Li+ in these systems is essentially unrestricted, with a fast, nanosecond-scale exchange of the ions between CMC and the aqueous environment.