Isotope‐Labeling Inspired Lattice‐Inherited Rhenium Single‐Atom Regulating Local Electronic Microenvironment of Dual‐Phase MoS 2 /MoP Nanotubes for Accelerated Sulfur Redox Kinetics

ABSTRACT Simultaneously regulating the local electronic microenvironment of dual phases in heterostructures remains a significant challenge. Herein, we propose a lattice‐inherited single‐atom strategy to construct Re‐doped MoS 2 /MoP dual phases, where Re atoms remain atomically dispersed throughout the MoS 2 to MoP transformation. This strategy enables concurrent regulation of the diffusion of MoS 2 and catalytic MoP phases, thereby overcoming the intrinsic adsorption, diffusion, and catalytic limitations of individual phases in conventional dual‐phase heterostructures. DFT calculations reveal that, in Re‐MoS 2 , Re incorporation induces reconfiguration of surface S 3 p orbitals, weakening Li‐S orbital overlap and lowering Li + diffusion barrier. In Re‐MoP, unpaired delocalized electrons upshift the d ‐band center and strengthen interfacial charge coupling, thereby accelerating polysulfide redox kinetics. Meanwhile, the dual‐phase distribution of Re atoms enhances the built‐in electric field, promoting directional polysulfide migration toward catalytic domains. Structurally, the constructed hetero‐nanotube catalysts, featuring ultrathin Re‐doped MoS 2 /MoP coaxially encapsulating carbon nanotubes, ensure intimate face‐to‐face contact and efficient electron transport. The cell exhibits remarkable cycling stability (0.035% decay over 1000 cycles at 5 C) and achieves a high areal capacity of 9.16 mAh cm −2 at 10.59 mg cm −2 sulfur loading. This work opens a new avenue for enhancing heterostructure synergistic effects, extending beyond Li‐S batteries to other multi‐electron‐transfer systems.