Sulfated Alginate as an Effective Polymer Binder for High-Voltage LiNi_0.5Mn_1.5O₄ Electrodes in Lithium-Ion Batteries

Although the increasing demand for high-energy-density lithium-ion batteries (LIBs) has inspired extensive research on high-voltage cathode materials, such as LiNi_0.5Mn_1.5O₄ (LNMO), their commercialization is hindered by problems associated with the decomposition of common carbonate solvent-based electrolytes at elevated voltages. To address these problems, we prepared high-voltage LNMO composite electrodes using five polymer binders (two sulfated and two nonsulfated alginate binders and a poly(vinylidene fluoride) conventional binder) and compared their electrochemical performances at ∼5 V vs Li/Li⁺. The effects of binder type on electrode performance were probed by analyzing cycled electrodes using soft/hard X-ray photoelectron spectroscopy and scanning transmission electron microscopy. The best-performing sulfated binder, sulfated alginate, uniformly covers the surface of LNMO and increased its affinity for the electrolyte. The electrolyte decomposition products generated in the initial charge-discharge cycle on the alginate-covered electrode participated in the formation of a protective passivation layer that suppressed further decomposition during subsequent cycles, resulting in enhanced cycling and rate performances. The results of this study provide a basis for the cost-effective and technically undemanding fabrication of high-energy-density LIBs.