Conjugation of mussel-inspired catechol groups to various polymer backbones results in materials suitable as silicon anode binders. The unique wetness-resistant adhesion provided by the catechol groups allows the silicon nanoparticle electrodes to maintain their structure throughout the repeated volume expansion and shrinkage during lithiation cycling, thus facilitating substantially improved specific capacities and cycle lives of lithium-ion batteries.
Polymeric binders play an important role in electrochemical performance of high-capacity silicon (Si) anodes that usually suffer from severe capacity fading due to unparalleled volume change of Si during cycling. In an effort to find efficient polymeric binders that could mitigate such capacity fading, herein, we introduce polymerized β-cyclodextrin (β-CDp) binder for Si nanoparticle anodes. Unlike one-dimensional binders, hyperbranched network structure of β-CDp presents multidimensional hydrogen-bonding interactions with Si particles and therefore offers robust contacts between both components. Even the Si nanoparticles that lost the original contacts with the binder during cycling recover within the multidimensional binder network, thus creating a self-healing effect. Utilizing these advantageous features, β-CDp-based Si electrode shows markedly improved cycling performance compared to those of other well-known binder cases, especially when combined with linear polymers at an appropriate ratio to form hybrid binders.
The millipede's extraordinary adhesion provides a design principle for silicon anode binders with emphasis on the superstructure and electrostatic charge.
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