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Chemistry. 2018 Feb 9;24(9):2126-2136. doi: 10.1002/chem.201703428. Epub 2017 Nov 6.

General Synthesis of Transition-Metal Oxide Hollow Nanospheres/Nitrogen-Doped Graphene Hybrids by Metal-Ammine Complex Chemistry for High-Performance Lithium-Ion Batteries.

Chen J1,2, Wu X1,3, Gong Y1,2, Wang P1,2, Li W1,2, Mo S1,2, Peng S1,2, Tan Q1, Chen Y1,3.

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State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Beijing, 100190, P.R. China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Center for Excellence in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, P.R. China.


We present a general and facile synthesis strategy, on the basis of metal-ammine complex chemistry, for synthesizing hollow transition-metal oxides (Co3 O4 , NiO, CuO-Cu2 O, and ZnO)/nitrogen-doped graphene hybrids, potentially applied in high-performance lithium-ion batteries. The oxygen-containing functional groups of graphene oxide play a prerequisite role in the formation of hollow transition-metal oxides on graphene nanosheets, and a significant hollowing process occurs only when forming metal (Co2+ , Ni2+ , Cu2+ , or Zn2+ )-ammine complex ions. Moreover, the hollowing process is well correlated with the complexing capacity between metal ions and NH3 molecules. The significant hollowing process occurs for strong metal-ammine complex ions including Co2+ , Ni2+ , Cu2+ , and Zn2+ ions, and no hollow structures formed for weak and/or noncomplex Mn2+ and Fe3+ ions. Simultaneously, this novel strategy can also achieve the direct doping of nitrogen atoms into the graphene framework. The electrochemical performance of two typical hollow Co3 O4 or NiO/nitrogen-doped graphene hybrids was evaluated by their use as anodic materials. It was demonstrated that these unique nanostructured hybrids, in contrast with the bare counterparts, solid transition-metal oxides/nitrogen-doped graphene hybrids, perform with significantly improved specific capacity, superior rate capability, and excellent capacity retention.


complex chemistry; lithium-ion batteries; nitrogen-doped graphene; synthesis design; transition metals


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