Stable silicon anodes realized by multifunctional dynamic cross-linking structure with self-healing chemistry and enhanced ionic conductivity for lithium-ion batteries

Silicon anodes have attracted enormous attention with the merits of outstanding theoretical capacity for high-energy-density lithium-ion batteries. However, the drastic volume variation will destroy the structural integrity of the electrode system during the alloying/dealloying process. Herein, base...

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Veröffentlicht in:Nano energy 2022-08, Vol.99, p.107334, Article 107334
Hauptverfasser: Wan, Xin, Mu, Tiansheng, Shen, Baicheng, Meng, Qi, Lu, Guangchong, Lou, Shuaifeng, Zuo, Pengjian, Ma, Yulin, Du, Chunyu, Yin, Geping
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Sprache:eng
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Zusammenfassung:Silicon anodes have attracted enormous attention with the merits of outstanding theoretical capacity for high-energy-density lithium-ion batteries. However, the drastic volume variation will destroy the structural integrity of the electrode system during the alloying/dealloying process. Herein, based on the supramolecular self-assembly, a multifunctional dynamic cross-linking strategy with self-healing chemistry and enhanced ionic conductivity for silicon electrode network structure is rationally designed by amino-functionalized silicon (Si-NH2) and dopamine-modified poly(acrylic acid) (PAA-DA). Dynamic reversible hydrogen bonds and ionic bonds are formed by random cross-linking of the primitives carried by the material, which endow the electrode with rapid self-healing ability and strong adhesion, and provide a continuous internal pathway for the electrode system. Moreover, the presence of polar groups can beneficially heighten the transport kinetics of lithium ions. The prepared Si-NH2@PAA-DA electrode displays excellent high-rate capability with a reversible capacity of 2671.6 mAh g−1 at 1 C (1 C = 4000 mA g−1) and superior cycle stability (2160.1 mAh g−1 after 100 cycles at 400 mA g−1). Therefore, this design idea with dynamic reversible and multi-crosslink network structure provides in-depth insights for the advancement of the next-generation high-energy-density batteries. [Display omitted] •Multifunctional dynamic cross-linking strategy (Si-NH2@PAA-DA) with self-healing chemistry and enhanced ionic conductivity for silicon electrodes is successfully designed.•Multiple dynamic supramolecular interactions (hydrogen bond and ionic bond) can effectively dissipate the stress-energy of volume change and relieve the mechanical cracking of the electrode.•The presence of polar groups can beneficially heighten the transport kinetics of lithium ions.•Si-NH2@PAA-DA electrode exhibits outstanding cycling stability and rate performance.
ISSN:2211-2855
DOI:10.1016/j.nanoen.2022.107334