This work pioneers an in situ gas-phase conversion strategy to construct VS2@V2Tx heterostructures within a MWCNT network. The integrated architecture establishes interpenetrating electron/ion highways, enabling an ultra-thick electrode (300 µm) to achieve a high areal capacity of 13.6 mAh cm−2 with exceptional cycling stability, demonstrating great promise for high-energy-density batteries.
ABSTRACT
Achieving high areal capacity is critical for advancing lithium-ion batteries (LIBs) toward high-energy-density applications. However, prevailing thick electrode architectures inevitably suffer from sluggish charge transport kinetics and mechanical degradation. Here, we pioneer an in situ gas-phase conversion strategy to directly grow metallic VS2 nanosheets on V2CTx MXene within a multi-walled carbon nanotube (MWCNT) network. This integrated architecture simultaneously establishes interpenetrating electron/ion highways—enabling full lithiation in ultra-thick electrodes (12-fold higher Li+ concentration compare to the traditional electrode)—and enhances mechanical toughness, thus achieving exceptional cycling stability under high current densities. Such TMDC–MXene heterostructure exhibit an impressive specific capacity of 1046 mAh g−1 and areal capacity of 13.6 mAh cm−2, with the thickness of 300 µm, representing only 12.8% gravimetric capacity decay despite 333% increased electrode thickness. Moreover, the resulting electrode maintains excellent cycling stability, retaining a capacity of 1.8 mAh cm−2 even at high current density of 6.4 mA cm−2, alongside 81% capacity retention over 600 cycles at 2C in LiFePO4 full-cells.
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