Silicon (Si) has been widely investigated as a candidate for lithium-ion batteries (LIBs) due to its extremely high specific capacity. The binders play a key role in fabricating high-performance Si electrodes which usually suffer from the huge volume expansion associated with the alloying and dealloying processes. Here we develop a facile route to prepare a three-dimensional (3D) conductive interpenetrated gel network as a novel binder for high-performance Si anodes through chemically cross-linking of acrylic acid monomer followed by the in situ polymerization of aniline. The excellent electrical conductivity, strong mechanical adhesion and high electrolyte uptake render the conductive gel network a potential binder for high-performance Si anodes. The resultant Si anodes exhibit excellent cycling stability, high Coulombic efficiency and superior rate capability, revealing better electrochemical properties compared to the Si anodes with conventional binders. The 3D conductive gel binder could not only accommodate the volume expansion and maintain electric connectivity, but also assist in the formation of stable solid electrolyte interphase (SEI) films. Such a strategy sheds light on the design of polymer binders in LIBs, especially for high-capacity electrode materials with huge volume changes during long-term cycling.

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Various well-designed nanostructures have been proposed to optimize the electrode systems of lithium-ion batteries for problems like Li(+) diffusion, electron transport, and large volume changes so as to fulfill effective capacity utilization and increase electrode stability. Here, a novel three-dimensional (3D) hybrid Sn-Ni@PEO nanotube array is synthesized as a high performance anode for a lithium-ion battery through a simple one-step electrodeposition for the first time. Superior to the traditional stepwise synthesis processes of heterostructured nanomaterials, this one-step method is more suitable for practical applications. The electrode morphology is well preserved after repeated Li(+) insertion and extraction, indicating that the positive synergistic effect of the alloy nanotube array and 3D ultrathin PEO coating could authentically optimize the current volume-expansion electrode system. The electrochemistry results further confirm that the superiority of the Sn-Ni@PEO nanotube array electrode could largely boost durable high reversible capacities and superior rate performances compared to a Sn-Ni nanowire array. This proposed ternary hybrid structure is proven to be an ideal candidate for the development of high performance anodes for lithium-ion batteries.

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