Ultra-thin nanosheets decorated in-situ S-doped 3D interconnected carbon network as interlayer modified Li-S batteries separator for accelerating adsorption-catalytic synergistic process of LiPSs.

This study provides a promising strategy for designing separator modified materials to solve the shuttle effect of soluble LiPSs in Li-S batteries. [Display omitted] • A composite material consisting of the 3D connected carbon network and ultra-thin NiCo-LDH nanosheets was devised and manufactured. • The DFT calculations further provided a comprehensive demonstration of the synergy adsorption and catalytic conversion processes. • Li-S batteries that were assembled using modified separators demonstrated remarkable electrochemical performance. The shuttle effect of soluble lithium polysulfides (LiPSs) is primarily responsible for the unstable performance of lithium-sulfur (Li-S) batteries, which has severely impeded their continued development. In order to solve this problem, a special strategy is proposed. Specifically, ultra-thin NiCo based layered double hydroxides (named LDH or NiCo-LDH) nanosheets are implanted into a pre-designed 3D interconnected carbon networks (SPC) to obtain porous composite materials (named SPC-LDH). During the operation of the battery, the 3D interconnected porous carbon mesh was the first to rapidly adsorb LiPSs, and then the LDH on the surface of the carbon mesh was used to realize the catalytic conversion of LiPSs. This facilitates the electrochemical conversion reaction between S substances while addressing the "shuttle effect". As a result, the battery maintains a discharge capacity of 1401.9, 1114.3, 975.5, 880.7, 760.4 and 679.6 mAh g−1 at the current densities of 0.1, 0.2, 0.5, 1, 2 and 3C, respectively. After 200 cycles at 2C, the battery's capacity stays at 732.9 mAh g−1, meaning that the average rate of capacity decay is only 0.007 % per cycle. Moreover, in-situ XRD demonstrates the critical function of PP/SPC-LDH separators in inhibiting LiPSs and encouraging Li 2 S transformation. The strong affinity of SPC-LDH for Li 2 S 6 is also confirmed by density functional theory (DFT) calculation, offering more theoretical support for the synergistic adsorption process. This work offers a compelling method to develop modified separator materials that can counteract the "shuttle effect" in Li-S batteries. [ABSTRACT FROM AUTHOR]