NDLI: Understanding the Li-storage in few layers graphene with respect to bulk graphite: experimental, analytical and computational study

Content Provider	Royal Society of Chemistry (RSC)
Author	Sonia, Farjana J. Mukhopadhyay, Amartya Jangid, Manoj K. Johari, Priya Ananthoju, Balakrishna Aslam, M.
Copyright Year	2017
Abstract	In order to understand, clarify and provide confirmations in the contexts of the prevalent confusions concerning Li-storage in graphenic carbon (viz. the reduced dimensional scale of graphitic carbon), electrochemical lithiation/delithiation has been performed with CVD-grown fairly pristine well-ordered few-layer graphene films (FLG; ∼7 layers; as a model material). Chronopotentiograms and cyclic voltammograms recorded with the FLG present distinct features corresponding to the transformation between different Li-GICs (i.e., ‘staging’) below 0.3 V against Li/Li+, thus confirming that ‘classical’ Li-intercalation does occur even at such reduced dimensional (nano)scale. Nevertheless, even in this lower potential window (our main focus here), Li-storage in FLG involves contributions from both diffusion- and surface-controlled mechanisms. The Li-capacities recorded with FLG just within this lower potential window, and also upon subtracting any possible contribution from the Cu current collector, were still ∼3–4 times greater than those obtained with similarly grown thicker bulk graphite films (TBG: ∼450 nm; Li-capacity recorded: ∼380 mA h g−1). Contrary to the usual belief, the excess Li-capacity of FLG cannot be explained by the presence of extrinsic/intrinsic defects, which are nearly negligible in the FLG films under consideration. Simulation of Li-storage in graphene via DFT indicated that the excess capacity (after formation of the LiC6 configuration) is associated with additional stable Li-storage on the outer graphene surfaces in the forms of more than one Li-layer (but different from Li-plating) and segregation close to the ‘stepped’ (exposed) edges of the inner graphene layers (but not exactly at the edge sites). Overall, such predicted Li-storage mechanisms are in agreement with the experimentally observed contributions from both ‘classical’ Li-intercalation and surface-controlled processes (even at potentials below 0.3 V), which primarily account for the excess Li-capacities recorded with graphenic carbon.
Starting Page	8662
Ending Page	8679
Page Count	18
File Format	HTM / HTML PDF
ISSN	20507488
Volume Number	5
Issue Number	18
Journal	Journal of Materials Chemistry A
DOI	10.1039/c7ta01978e
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Carbon Electrochemistry Graphene Cyclic voltammetry Classical mechanics Diffusion Graphite
Content Type	Text
Resource Type	Article
Subject	Chemistry Renewable Energy, Sustainability and the Environment Materials Science

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