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Atomistic Origins of High Rate Capability and Capacity of N-Doped Graphene for Lithium Storage

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† International Center for Young Scientists (ICYS), World Premier International (WPI) Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), Namiki 1-1, Tsukuba, Ibaraki 305-0044, Japan
‡ Graduate School of System and Information Engineering, University of Tsukuba, Tennoudai 1-1-1, Tsukuba, 305-8573, Japan
*E-mail: (X.W.) [email protected]
*E-mail: (D.-M.T.) [email protected]
*E-mail: (W.T.) [email protected]
*E-mail: (D.G.) [email protected]
Cite this: Nano Lett. 2014, 14, 3, 1164–1171
Publication Date (Web):January 30, 2014
https://doi.org/10.1021/nl4038592
Copyright © 2014 American Chemical Society
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Abstract

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Distinct from pure graphene, N-doped graphene (GN) has been found to possess high rate capability and capacity for lithium storage. However, there has still been a lack of direct experimental evidence and fundamental understanding of the storage mechanisms at the atomic scale, which may shed a new light on the reasons of the ultrafast lithium storage property and high capacity for GN. Here we report on the atomistic insights of the GN energy storage as revealed by in situ transmission electron microscopy (TEM). The lithiation process on edges and basal planes is directly visualized, the pyrrolic N “hole” defect and the perturbed solid-electrolyte-interface configurations are observed, and charge transfer states for three N-existing forms are also investigated. In situ high-resolution TEM experiments together with theoretical calculations provide a solid evidence that enlarged edge {0002} spacings and surface hole defects result in improved surface capacitive effects and thus high rate capability and the high capacity are owing to short-distance orderings at the edges during discharging and numerous surface defects; the phenomena cannot be understood previously by standard electron or X-ray diffraction analyses.

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High-resolution C1s XPS spectra of GN. The cyclic voltammetric responses of GN and G at the different sweep rates. SAED pattern of the lithiated GN. HRTEM images in the lithiation process of GN. The C–K EELS spectrum of GN at the lithiated state. HRTEM image of pure G, side view, and the corresponding structural scheme constructed by Material Studio software. Comparison of the theoretical capacity of graphite, G and the different types of GN according to DFT calculations. This material is available free of charge via the Internet at http://pubs.acs.org.

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