Abstract

Rechargeable magnesium batteries (rMBs) are promising techniques suitable for large-scale energy storage systems with low-cost and high safety. However, their development is severely hindered by strong coulombic effect between bivalent Mg 2+ and cathode materials. In this work, two dimensional hierarchical nano-micro hybrids are synthesized by in-situ generating VS 4 nanosheets on carbon-coated Ti 3 C 2 MXene matrix (denoted as VS 4 @Ti 3 C 2 /C). A high-performance rMB system is built by using the hierarchical nano-micro hybrids cathode, magnesium foil anode, and 0.25 M methylpyrrolidinium chloride in 0.25 M 2PhMgCl-AlCl 3 /tetrahydrofuran as the electrolyte. The existence of V–C bond proves that VS 4 is anchored on the surface of Ti 3 C 2 via a strong chemical bond, rather than simply by adsorption. The unique hierarchical nano-micro structure improves the accessibility of the electrolyte and reduces the charge transfer resistance, leading to a high discharge capacity of 492 mA h g −1 at 50 mA g −1 , an outstanding rate performance of 129 mA h g −1 at 1000 mA g −1 , and excellent cycling performance (over 900 cycles at 500 mA g −1 ). Moreover, reversible intercalation of MgCl + into VS 4 @Ti 3 C 2 /C is revealed by investigating the evolution of the hybrids during different electrochemical states. This study will shed light on designing high-performance MXene-based cathode materials for multivalent batteries. • VS 4 @Ti 3 C 2 /C hierarchical nano-micro hybrids are synthesized by hydrothermal. • VS 4 @Ti 3 C 2 /C shows outstanding rate performance and excellent cycle stability. • The working mechanism of VS 4 @Ti 3 C 2 /C in rMBs is investigated.

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