High-Level Heteroatom Doped Two-Dimensional Carbon Architectures for Highly Efficient Lithium-Ion Storage

Abstract

In this work, high-level heteroatom doped two-dimensional hierarchical carbon architectures (H-2D-HCA) are developed for highly efficient Li-ion storage applications. The achieved H-2D-HCA possesses a hierarchical 2D morphology consisting of tiny carbon nanosheets vertically grown on carbon nanoplates and containing a hierarchical porosity with multiscale pore size. More importantly, the H-2D-HCA shows abundant heteroatom functionality, with sulfur (S) doping of 0.9% and nitrogen (N) doping of as high as 15.5%, in which the electrochemically active N accounts for 84% of total N heteroatoms. In addition, the H-2D-HCA also has an expanded interlayer distance of 0.368 nm. When used as lithium-ion battery anodes, it shows excellent Li-ion storage performance. Even at a high current density of 5 A g−1, it still delivers a high discharge capacity of 329 mA h g−1 after 1,000 cycles. First principle calculations verifies that such unique microstructure characteristics and high-level heteroatom doping nature can enhance Li adsorption stability, electronic conductivity and Li diffusion mobility of carbon nanomaterials. Therefore, the H-2D-HCA could be promising candidates for next-generation LIB anodes.

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“…Even discharge capacity highly reached as high as 748 mAh g À1 after 400 cycles at 2 A g À1 . In particular, they [112] further increased the concentration of N to develop 2D hierarchical carbon architectures with high heteroatom doping (H-2D-HCA). Compared with 2D-HCA, H-2D-HCA showed a higher doping degree (0.9% of S and 15.5% of N), a higher proportion of electrochemically active N (up to 84%) and interlayer distance (enlarged by 0.368 nm).…”

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