Accelerating Charge‐Transfer Kinetics via Triggering Electron Spin Polarization in Open‐Hollow MoS 2 Nanospheres for Ultrafast Lithium Storage

ABSTRACT The development of ultrafast‐charging MoS 2 anodes is fundamentally constrained by sluggish charge‐transfer kinetics. This study addresses this limitation by triggering electron spin polarization through atomic‐scale Co doping within open‐hollow MoS 2 nanospheres. Structurally, the open‐hollow design minimizes ion diffusion distances and accommodates volume changes of MoS 2 , providing a robust foundation for rapid ion flux. Electronically, Co incorporation enhances S 3p–Mo 4d–Co 3d orbital hybridization, triggering a marked electron spin polarization that reduces kinetic barriers for insertion and conversion reactions. Post‐conversion stage, in situ generated metallic Co nanoparticles (Co 0 ) act as dynamic mediators for spin‐polarized electron transfer. Specifically, the injection of spin‐polarized electrons into Co° creates a spin‐polarized surface capacitance, boosting charge storage at the Co 0 /Li 2 S interfaces. Conversely, the release of these electrons promotes a Co 0 ‐catalyzed construction of solid electrolyte interphase, prioritizing conductive LiF species while suppressing Li 2 CO 3 , facilitating ion transport at the electrode‐electrolyte interfaces. Consequently, the MoS 2 ‐based anode exhibits an impressive ultrafast‐charging capability of 30 C (1044.1 mAh g −1 ) and maintains stability over 10 000 cycles at 15 C with a final capacity of 874.7 mAh g −1 . This work demonstrates that triggering electron spin polarization represents a transformative approach to overcoming kinetic barriers in next‐generation ultrafast‐charging batteries.