Synergistic Interface and Mesopore Engineering with More and Quicker Ion Storage for Enhanced Performance of Lithium‐Ion Battery

Abstract Designing hetero‐nanostructures is widely recognized as an effective modification strategy to obtain ZnO/Co₃O₄ anode materials with superior electrochemical properties. However, the lithium‐ion storage behavior of ZnO/Co₃O₄ has not reached a satisfied performance. Herein, based on our previous DFT results that the interface of ZnO(110)/Co₃O₄(220) hetero‐nanostructure possesses fast reaction kinetics because of more negative surface adsorption energy and lower diffusion barrier energy of lithium ions, we developed ZnO(110)/Co₃O₄(220)@C hetero‐nanostructures with both abundant interfaces and uniform mesopores structure derived from 2D MOF precursor. Especially, ZnO/Co₃O₄@C hybrid materials with ZnO(110)/Co₃O₄(220) hetero‐nanostructure show strong electronic interactions and the widen distance of the crystal plane at the interface, resulting in stable hetero‐nanostructures with faster ion diffusion channel and more active sites. Moreover, this material possesses uniform mesopores and 2D structure, which enables quicker transport capability and cycling longevity for lithium‐ion storage. Impressively, when ZnO/Co₃O₄@C was used as anodes in lithium‐ion batteries, the electrodes deliver improved initial specific capacities (1,630.5 and 1,496.9 mAh g⁻¹ at 0.2 and 0.5 A g⁻¹), excellent capacity retention (1,758.3 mAh g⁻¹ after 370 cycles at 0.2 A g⁻¹, and 607.7 mAh g⁻¹ up to 650 cycles at 5 A g⁻¹), and superior rate capacity (937 and 468 mAh g⁻¹ at 1.0 and 5.0 A g⁻¹ after 360 cycles).