Comprehensive Understanding of High Polar Polyacrylonitrile as an Effective Binder for Li-Ion Battery Nano-Si Anodes.

Well-defined polyacrylonitriles (PANs) with different molecular weights were synthesized through an activator regenerated by electron-transfer atom-transfer radical polymerization method and employed as binders in silicon negative electrode for lithium-ion batteries. Compared with poly(vinylidene fluoride) and carboxyl methyl cellulose as binders, the electrode performance of PANs is well-improved. Specifically, at 100 mA g(-1) from 0.01 to 1.5 V, the initial discharge capacity of PAN100-based electrode is 4147.8 mA h g(-1) and still remains about 1639.6 mA h g(-1) over 50 cycles. A comprehensive understanding on the improvement mechanism is preliminarily discussed. The results indicate that the superior performance largely depends on the higher lithium ion diffusion efficiency in PAN which results from the weak interaction between lithium ions and PAN polymer chain, and the hydrogen bonds among the nitrile group (C≡N) of PAN, Si nanoparticles, and the current collector, which will lead to an efficient coating of PAN with the Si particles and well-improved adhesion strength, synergistically depressing the structural deterioration of silicon electrodes.