Metal–Organic Coordination Strategy for Obtaining Metal‐Decorated Mo‐Based Complexes: Multi‐dimensional Structural Evolution and High‐Rate Lithium‐Ion Battery Applications

Multi‐dimensional metal oxides have attracted great attention in diverse applications due to their intriguing performances. However, their structural design remains challenging, particularly that based on organic chelation chemistry. Although metal–organic complexes with different architectures have been reported, their structure formation mechanisms are not well understood because of the complex chelation processes. Herein, we introduce a new metal–organic coordination strategy to construct metal‐decorated (Ni, Co, Mn) Mo‐based complexes ranging from 2D nanopetals to 3D microflowers. The chelating process of the metal–organic complex can be tuned by a surfactant, giving rise to different structures, and then a further metal can be appended. Thus, different metal (oxide)‐decorated MoO2/C‐N structures were designed, enabling an extremely high lithium storage capability of 1018 mA h g−1 and rate capacities of up to 10 A g−1 over 1000 cycles. Relationships between electrochemical behavior and structure have been analyzed kinetically. A high‐rate lithium‐ion battery has been assembled from Ni‐MoO2/C‐N and an Ni‐rich layered oxide as the anode and cathode, respectively. We believe that this general metal–organic coordination strategy should be applicable to other multi‐functional materials with superior capabilities.