Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure as anode for high performance of lithium-ion batteries

Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure (NTLP) was designed and fabricated through hydrothermal template self-assembly method using polystyrene (PS) nanospheres as structural guiding templates and ethylenediamine (EDA) as a nitrogen resource for in-situ N-doping. NTLP exhibits significantly improved electrochemical performance of lithium-ion storage including a highly reversible capacity of 1147 ​mA ​h g−1 at 0.1 ​A ​g−1, and favorable rate capability of 258 ​mA ​h g−1 even at a large current density of 5 ​A ​g−1. Moreover, the reversible capacity is retained at 501 ​mA ​h g−1 after 1100 cycles at 1 ​A ​g−1. PS template effectively alleviates the aggregation of graphene membrane, meanwhile forms peculiar thousand-layered cake structure with high specific surface area and well-controlled pores. Precisely owing to the unique structure with three-dimensionally (3D) interconnected holey graphene network and the introduction of abundant N-doping (about 7 atom%) into the graphene walls, NTLP significantly enhances the electrochemical activity and effectively accelerates the diffusions of both lithium-ions and electrons. The high performance strongly indicates that NTLP possesses a promising perspective for lithium-ion batteries with excellent electronic conductivity, efficient transport pathways of electrons and ions as well as superior reversible lithium storage capacity. Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure (NTLP) was designed and fabricated through hydrothermal template self-assembly method using polystyrene (PS) nanospheres as structural guiding templates and ethylenediamine (EDA) as a nitrogen resource for in-situ N-doping. [Display omitted] •Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure (NTLP) was prepared via hydrothermal and calcination processes in the presence of polystyrene (PS) nanospheres and ethylenediamine (EDA).•The unique structure of NTLP not only improves electronic conductivity, but also accelerates ionic diffusion.•NTLP as anode material for lithium-ion batteries exhibits superior electrochemical performance.