Silicon-based
materials are the desirable anodes for next-generation
lithium-ion batteries; however, the large volume change of Si during
the charging/discharging process causes electrode fracture and an
unstable solid–electrolyte interphase (SEI) layer, which severely
impair their stability and Coulombic efficiency. Herein, a bundle
of silicon nanoparticles is encapsulated in robust micrometer-sized
MXene frameworks, in which the MXene nanosheets are precrumpled by
capillary compression force to effectively buffer the stress induced
by the volume change, and the abundant covalent bonds (Ti–O–Ti)
between adjacent nanosheets formed through a facile thermal self-cross-linking
reaction further guarantee the robustness of the MXene architecture.
Both factors stabilize the electrode structure. Moreover, the abundant
fluorine terminations on MXene nanosheets contribute to an in situ formation of a highly compact, durable, and mechanically
robust LiF-rich SEI layer outside the frameworks upon cycling, which
not only shuts down the parasitic reaction between Si and an organic
electrolyte but also enhances the structural stability of MXene frameworks.
Benefiting from these merits, the as-prepared anodes deliver a high
specific capacity of 1797 mA h g–1 at 0.2 A g–1 and a high capacity retention of 86.7% after 500
cycles at 2 A g–1 with an average Coulombic efficiency
of 99.6%. Significantly, this work paves the way for other high-capacity
electrode materials with a strong volume effect.
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