An easy-to-prepare flexible 3D network aqueous binder with gradient hydrogen bonding for high-performance silicon anodes

Although silicon (Si) anode has extremely high specific capacity, the damage to the electrode caused by the huge volume expansion greatly hinders its practical application in lithium-ion batteries. Aiming to alleviate this problem, a high-performance aqueous binder (AMNG) with gradient hydrogen bonding and flexible three-dimensional network structure is prepared by a one-pot method. Compared to the conventional linear polyacrylic acid (PAA) binder, the AMNG binder exhibits enhanced ionic conductivity and stress dissipation for Si nanoparticles, which is able to greatly reduce the side reactions caused by volume changes and considerably improve the electrochemical performance of Si anodes. As a result, the Si nanoparticles using the AMNG binder exhibit an initial discharge capacity as high as 3101 mAh g−1 with a Coulombic efficiency of 89.95%, and a capacity retention of 71.6% for 120 cycles, which are superior to the electrode using PAA, corresponding to 2832 mAh g−1, 88.37% and 28.1%, respectively. More prominently, the practical application of the AMNG binder is evaluated in high-mass-loading Si-based electrodes and even in full cells with LiFePO4, all showing satisfied performance. Therefore, this design approach is valuable as a reference for the preparation of commercial aqueous binders.