Improving the Electrochemical Property of Silicon Anodes through Hydrogen-Bonding Cross-Linked Thiourea-Based Polymeric Binders

Binders play a crucial role in the development of silicon (Si) anodes for lithium-ion batteries with high specific energy. The large volume change of Si (∼300%) during repeated discharge and charge processes causes the destruction and separation of electrode materials from the copper (Cu) current collector and ultimately results in poor cycling performance. In the present study, we design and prepare hydrogen-bonding cross-linked thiourea-based polymeric binders (denoted CMC-co-SN) in consideration of their excellent binding interaction with the Cu current collector and low cost as well. The CMC-co-SN binders are formed through in situ thermopolymerization of chain-type carboxymethylcellulose sodium (CMC) with thiourea (SN) in the drying process of Si electrode disks. A tight and physical interlocked layer between the CMC-co-SN binder and Cu current collector is derived from a dendritic nonstoichiometric copper sulfide (Cu_xS) layer on the interface and enhances the binding of electrode materials with the Cu current collector. When applying the CMC-co-SN binders to micro- (∼3 μm) (μSi) and nano- (∼50 nm) (nSi) Si particles, the Si anodes exhibit high initial Coulomb efficiency (91.5% for μSi and 83.2% for nSi) and excellent cyclability (1121 mA h g^-1 for μSi after 140 cycles and 1083 mA h g^-1 for nSi after 300 cycles). The results demonstrate that the CMC-co-SN binders together with a physical interlocked layer have significantly improved the electrochemical performance of Si anodes through strong binding forces with the current collector to maintain electrode integrity and avoid electric contact loss.