Embedding MnO@Mn 3 O 4 Nanoparticles in an N‐Doped‐Carbon Framework Derived from Mn‐Organic Clusters for Efficient Lithium Storage

作者：Yanting Chu, Lingyu Guo, Baojuan Xi, Zhenyu Feng, Fangfang Wu, Yue Lin, Jincheng Liu, Di Sun, Jinkui Feng, Yitai Qian, Shenglin Xiong · 发表于：Advanced Materials · 年份：2017 · DOI：10.1002/adma.201704244 · 被引用次数：444 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Extraction and Separation Processes

Abstract The first synthesis of MnO@Mn 3 O 4 nanoparticles embedded in an N‐doped porous carbon framework (MnO@Mn 3 O 4 /NPCF) through pyrolysis of mixed‐valent Mn 8 clusters is reported. The unique features of MnO@Mn 3 O 4 /NPCF are derived from the distinct interfacial structure of the Mn 8 clusters, implying a new methodological strategy for hybrids. The characteristics of MnO@Mn 3 O 4 are determined by conducting high angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) and electron energy loss spectroscopy (EELS) valence‐state analyses. Due to the combined advantages of MnO@Mn 3 O 4 , the uniform distribution, and the NPCF, MnO@Mn 3 O 4 /NPCF displays unprecedented lithium‐storage performance (1500 mA h g −1 at 0.2 A g −1 over 270 cycles). Quantitative analysis reveals that capacitance and diffusion mechanisms account for Li + storage, wherein the former dominates. First‐principles calculations highlight the strong affiliation of MnO@Mn 3 O 4 and the NPCF, which favor structural stability. Meanwhile, defects of the NPCF decrease the diffusion energy barrier, thus enhancing the Li + pseudocapacitive process, reversible capacity, and long cycling performance. This work presents a new methodology to construct composites for energy storage and conversion.