Abundant Lithiophilic VO2/V8C7 Heterostructures Boost Charge Transfer toward High‐Rate Lithium Storage

Abstract The construction of a heterogeneous structure on an electrode can enhance its absorption energy, thereby improving ionic diffusion and reaction kinetics. Herein, hyperdispersed VO 2 /V 8 C 7 nano‐heterostructures anchored on carbon nanofibers (VO 2 /V 8 C 7 @CNF), which are further utilized as a lithium anode are successfully developed. The self‐supported VO 2 /V 8 C 7 @CNF electrode features a synergistic effect, resulting from its well‐dispersed nano‐heterostructure, induced hetero‐interfacial electric field, and conspicuous lithiophilicity. This anode thus facilitates rapid Li + ions diffusion and charge transfer, resulting in high‐rate performance and uniform Li deposition. It exhibits a reversible specific capacity of as high as 674.8 mA h g −1 at a current density of 0.1 A g −1 and maintains a high‐rate capability of 205.3 mA h g −1 at a current density of as high as 5.0 A g −1 even after undergoing 1000 charge/discharge cycles. The Li‐ion nucleation overpotential on this anode is significantly reduced to 27 mV. The hyperdispersed nano‐heterostructure strategy offers a universal blueprint for the fabrication of high‐performance anodes not only for lithium and other batteries.