Ordered Mesoporous Carbon Grafted MXene Catalytic Heterostructure as Li-Ion Kinetic Pump toward High-Efficient Sulfur/Sulfide Conversions for Li-S Battery.

Lithium-sulfur (Li-S) batteries exhibit unparalleled theoretical capacity and energy density than conventional lithium ion batteries, but they are hindered by the dissatisfactory "shuttle effect" and the sluggish conversion kinetics owing to the low lithium ion transport kinetics, resulting in rapid capacity fading. Herein, a catalytic two-dimensional heterostructure composite is prepared by evenly grafting mesoporous carbon on the MXene nanosheet (denoted as OMC--MXene), serving as interfacial kinetic accelerators in Li-S batteries. In this design, the grafted mesoporous carbon in the heterostructure can not only prevent the stack of MXene nanosheets with the enhanced mechanical property but also offer a facilitated pump for accelerating ion diffusion. Meanwhile, the exposed defect-rich OMC--MXene heterostructure inhibits the polysulfide shuttling with chemical interactions between OMC--MXene and polysulfides and thus simultaneously enhances the electrochemical conversion kinetics and efficiency, as fully investigated by in situ/ex situ characterizations. Consequently, the cells with OMC--MXene ion pumps achieve a high cycling capacity (966 mAh g at 0.2 C after 200 cycles), a superior rate performance (537 mAh g at 5 C), and an ultralow decaying rate of 0.047% per cycle after 800 cycles at 1 C. Even employed with a high sulfur loading of 7.08 mg cm under lean electrolyte, an ultrahigh areal capacity of 4.5 mAh cm is acquired, demonstrating a future practical application.