Fluorine-free polymer binder enables circular manufacturing and recycling of lithium-ion batteries

Abstract Today’s lithium‑ion battery manufacturing heavily relies on polyvinylidene fluoride binder and N‑methyl‑2‑pyrrolidone solvent-based processing, which incurs high cost and hinders environmental sustainability. While bio-derived binders enable aqueous processing, their reliance on hydrogen bonding alone limits mechanical strength and electrochemical stability. Here, we introduce a fluorine‑free, water‑processable binder comprised of polyacrylic acid and carboxymethyl cellulose crosslinked by citric acid. The network integrates hydrogen, covalent, and ionic bonding among binder chains, active particles, and current collectors, providing strong adhesion as well as good oxidative stability and thermal stability. LiFePO 4 positive electrodes fabricated with fluorine‑free binder deliver comparable initial capacity to the control electrodes with polyvinylidene fluoride binder, while providing better cycle stability. This chemistry applies to a wide range of positive and negative electrode materials. Importantly, the fluorine‑free binder further facilitates sustainable direct recycling, demonstrating full recovery of spent positive and negative electrodes to achieve the same level of performance with pristine materials without generating fluorinated residue. Life-cycle analysis shows significant reductions in energy cost and emissions compared with recycling polyvinylidene fluoride-based batteries. This binder strategy endows high performance with circularity, offering a scalable route to sustainable battery manufacturing technologies.