Polyacrylonitrile Based Triblock Copolymer Binder Enabling Excellent Performance toward LiNi_0.5Mn_1.5O₄ and Sulfur Based Batteries

There is an urgent need for lithium-ion batteries with high energy density to meet the increasing demand for advanced devices and ecofriendly electric vehicles. Spinel LiNi_0.5Mn_1.5O₄ (LNMO) is the most promising cathode material for achieving high energy density due to its high operating voltage (4.75 V vs Li/Li⁺) and impressive capacity of 147 mAh g^-1. However, the binders conventionally used are prone to high potential and oxidation at the cathode side, resulting in a loss of the ability to bond active material and conductive agent integrity. This can lead to severe capacity fading and irreversible battery failure. This study demonstrates that incorporating acrylic anhydride and methyl methacrylate into conventional acrylonitrile through solution polymerization improves the binding energy and voltage resistance. The results indicate that the triblock poly(acrylonitrile-methyl methacrylate-acrylic anhydride) (PAMA) binder has a much higher peeling strength (0.506 N cm^-1) compared to its polyvinylidene fluoride (PVDF) counterpart (0.3 N cm^-1), making it a more feasible strategy. When assembled with LiNi_0.5Mn_1.5O₄, the PAMA based electrode maintains a capacity retention of 70.7% after 800 cycles at 0.1 C, which is significantly higher than the 33.9% retention of the PVDFbased electrode. This is due to the large number of polar groups, including ─C≡N and ─C═O, on PAMA, which are conducive to adsorbing lithium polysulfide. The S@PAMA electrode is tested and maintained a capacity value of 628.7 mAh g^-1 after long-term cycling, confirming its ability to effectively suppress the shuttle effect.