Journal
ADVANCED ENERGY MATERIALS
Volume 10, Issue 20, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201903110
Keywords
high areal capacity; high initial Coulombic efficiency; lithium-ion batteries; Si anodes; trifunctional binders
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High-capacity electrode materials play a vital role for high-energy-density lithium-ion batteries. Silicon (Si) has been regarded as a promising anode material because of its outstanding theoretical capacity, but it suffers from an inherent volume expansion problem. Binders have demonstrated improvements in the electrochemical performance of Si anodes. Achieving ultrahigh-areal-capacity Si anodes with rational binder strategies remains a significant challenge. Herein, a binder-lithiated strategy is proposed for ultrahigh-areal-capacity Si anodes. A hard/soft modulated trifunctional network binder (N-P-LiPN) is constructed by the partially lithiated hard polyacrylic acid as a framework and partially lithiated soft Nafion as a buffer via the hydrogen binding effect. N-P-LiPN has strong adhesion and mechanical properties to accommodate huge volume change of the Si anode. In addition, lithium-ions are transferred via the lithiated groups of N-P-LiPN, which significantly enhances the ionic conductivity of the Si anode. Hence, the Si@N-P-LiPN electrodes achieve the highest initial Coulombic efficiency of 93.18% and a stable cycling performance for 500 cycles at 0.2 C. Specially, Si@N-P-LiPN electrodes demonstrate an ultrahigh-areal-capacity of 49.59 mAh cm(-2). This work offers a new approach for inspiring the battery community to explore novel binders for next-generation high-energy-density storage devices.
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