Bi‐Directional H‐Bonding Modulated Soft/Hard Polyethylene Glycol‐Polyaniline Coated Si‐Anode for High‐Performance Li‐Ion Batteries

Ultrahigh-capacity silicon (Si) anodes are essential for the escalating energy demands driven by the booming e-transportation and energy storage field. However, their practical applications are strictly hampered by their intrinsically low electroconductivity, sluggish Li-ion diffusion, and undesirably large volume change. Herein, a high-performance Si anode, comprised of a modulated soft/hard coating of polyethylene glycol (PEG) (as Li-ion conductor) and polyaniline (PANI) (as electron conductor) on the surface of Si nanoparticles (NPs) through H-bonding network, is introduced. In this design, the abundant ─OH groups of soft PEG allow it to uniformly cover Si NPs while the hard PANI binds to PEG through its ─N─H group, thus constructing a tight connectin between Si and PEG-PANI (PP). Consequently, the elastic PP allows Si@PP to accommodate the huge volume expansion while possessing fine electronic/ionic conductivity. Therefore, the Si@PP anode exhibits a high initial Coulombic efficiency of 90.5% and a stable capacity of 1871 mAh g-1 after 100 cycles at 1 A g-1 with a retention of 85.7%. Additionally, the Si@PP anode also demonstrates a high areal capacity of 3.01 mAh cm-2 after 100 cycles at 0.5 A g-1 . This work reveals a scalable interface design of multi-layer multifunctional coatings for high-performance electrode materials in next-generation Li-ion batteries.