Carrageenans as Sustainable Water-Processable Binders for High-Voltage NMC811 Cathodes

[Image: see text] Poly(vinylidene fluoride) (PVDF) is the most common binder for cathode electrodes in lithium-ion batteries. However, PVDF is a fluorinated compound and requires toxic N-methyl-2-pyrrolidone (NMP) as a solvent during the slurry preparation, making the electrode fabrication process environmentally unfriendly. In this study, we propose the use of carrageenan biopolymers as a sustainable source of water-processable binders for high-voltage NMC811 cathodes. Three types of carrageenan (Carr) biopolymers were investigated, with one, two, or three sulfonate groups (SO(3)(–)), namely, kappa, iota, and lambda carrageenans, respectively. In addition to the nature of carrageenans, this article also reports the optimization of the cathode formulations, which were prepared by using between 5 wt % of the binder to a lower amount of 2 wt %. Processing of the aqueous slurries and the nature of the binder, in terms of the morphology and electrochemical performance of the electrodes, were also investigated. The Carr binder with 3SO(3)(–) groups (3SO(3)(–)Carr) exhibited the highest discharge capacities, delivering 133.1 mAh g(–1) at 3C and 105.0 mAh g(–1) at 5C, which was similar to the organic-based PVDF electrode (136.1 and 108.7 mAh g(–1), respectively). Furthermore, 3SO(3)(–)Carr reached an outstanding capacity retention of 91% after 90 cycles at 0.5C, which was attributed to a homogeneous NMC811 and a conductive carbon particle dispersion, superior adhesion strength to the current collector (17.3 ± 0.7 N m(–1) vs 0.3 ± 0.1 N m(–1) for PVDF), and reduced charge-transfer resistance. Postmortem analysis unveiled good preservation of the NMC811 particles, while the 1SO(3)(–)Carr and 2SO(3)(–)Carr electrodes showed damaged morphologies.