Dual-Functional Lithiophilic/Sulfiphilic Binary-Metal Selenide Quantum Dots Toward High-Performance Li–S Full Batteries

The commercial viability of lithium–sulfur batteries is still challenged by the notorious lithium polysulfides (LiPSs) shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode. Herein, a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton (3DIO FCSe-QDs@NC) is elaborately designed for both sulfur cathode and Li metal anode. The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble LiPSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors. Simultaneously, the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites. Taking advantage of these merits, the assembled Li–S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability (a low decay rate of 0.014% over 2,000 cycles at 2C). Remarkably, a promising areal capacity of 8.41 mAh cm(−2) can be achieved at the sulfur loading up to 8.50 mg cm(−2) with an ultra-low electrolyte/sulfur ratio of 4.1 μL mg(−1). This work paves the bi-serve host design from systematic experimental and theoretical analysis, which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li–S full batteries. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01037-1.