Multifunctional Heterostructured Fe3O4‐FeTe@MCM Electrocatalyst Enabling High‐Performance Practical Lithium‐Sulfur Batteries Via Built‐in Electric Field

Abstract The development of capable of simultaneously modulating the sluggish electrochemical kinetics, shuttle effect, and lithium dendrite growth is a promising strategy for the commercialization of lithium‐sulfur batteries. Consequently, an elaborate preparation method is employed to create a host material consisting of multi‐channel carbon microspheres (MCM) containing highly dispersed heterostructure Fe 3 O 4 ‐FeTe nanoparticles. The Fe 3 O 4 ‐FeTe@MCM exhibits a spontaneous built‐in electric field (BIEF) and possesses both lithophilic and sulfophilic sites, rendering it an appropriate host material for both positive and negative electrodes. Experimental and theoretical results reveal that the existence of spontaneous BIEF leads to interfacial charge redistribution, resulting in moderate polysulfide adsorption which facilitates the transfer of polysulfides and diffusion of electrons at heterogeneous interfaces. Furthermore, the reduced conversion energy barriers enhanced the catalytic activity of Fe 3 O 4 ‐FeTe@MCM for expediting the bidirectional sulfur conversion. Moreover, regulated Li deposition behavior is realized because of its high conductivity and remarkable lithiophilicity. Consequently, the battery exhibited long‐term stability for 500 cycles with 0.06% capacity decay per cycle at 5 C, and a large areal capacity of 7.3 mAh cm −2 (sulfur loading: 9.73 mg cm −2 ) at 0.1 C. This study provides a novel strategy for the rational fabrication of heterostructure hosts for practical Li‐S batteries.