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Abstract
The ongoing efforts to optimize Li‐ion batteries led to the interest in intercalation of nanoscale
layered compounds, including bilayer graphene. Its lithium intercalation has been demonstrated recently but the mechanisms underpinning the storage capacity remain poorly understood. Here, using magnetotransport measurements, we report in‐operando intercalation dynamics of bilayer graphene. Unexpectedly, we find four distinct intercalation stages that correspond to well‐defined Li‐ion densities. We refer to these stages as ‘in‐plane’, with no in‐plane analogues in bulk graphite. The fully intercalated bilayers represent a stoichiometric compound C14LiC14 with a Li density of ∼2.7∙1014 cm‐2, notably lower than fully intercalated graphite. Combining the experimental findings and DFT calculations, we show that the critical step in bilayer intercalation is a transition from AB to AA stacking which occurs at a density of ∼0.9∙1014 cm‐2. Our findings reveal the mechanism and limits for electrochemical intercalation of bilayer graphene and suggest possible avenues for increasing the Li storage capacity.
layered compounds, including bilayer graphene. Its lithium intercalation has been demonstrated recently but the mechanisms underpinning the storage capacity remain poorly understood. Here, using magnetotransport measurements, we report in‐operando intercalation dynamics of bilayer graphene. Unexpectedly, we find four distinct intercalation stages that correspond to well‐defined Li‐ion densities. We refer to these stages as ‘in‐plane’, with no in‐plane analogues in bulk graphite. The fully intercalated bilayers represent a stoichiometric compound C14LiC14 with a Li density of ∼2.7∙1014 cm‐2, notably lower than fully intercalated graphite. Combining the experimental findings and DFT calculations, we show that the critical step in bilayer intercalation is a transition from AB to AA stacking which occurs at a density of ∼0.9∙1014 cm‐2. Our findings reveal the mechanism and limits for electrochemical intercalation of bilayer graphene and suggest possible avenues for increasing the Li storage capacity.
| Original language | English |
|---|---|
| Article number | 6933 |
| Journal | Nature Communications |
| Volume | 15 |
| DOIs | |
| Publication status | Published - 13 Aug 2024 |
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CDT in Science and Applications of Graphene and Related Nanomaterial
Grigorieva, I. (PI), Burnett, H. (PGR student), Cusworth, E. (PGR student), Deaconu, D.-A. (PGR student), Dumitriu-Iovanescu, A.-D. (PGR student), Kang, Y.-W. (PGR student), Little, J. (PGR student), Rees, E. (PGR student), Selles, F. (PGR student), Shaker, M. (PGR student), Soong, Y.-C. (PGR student), Swindell, J. (PGR student), Tainton, G. (PGR student), Wood, H. (PGR student), Astles, T. (PGR student), Carl, A. (PGR student), Chen, G. (PGR student), Richard De Latour, H. (PGR student), Dowinton, O. (PGR student), Haskell, S. (PGR student), Hills, K. (PGR student), Hoole, C. (PGR student), Huang, Y. (PGR student), Kalsi, T. (PGR student), Powell, L. (PGR student), Quiligotti, K. (PGR student), Rimmer, J. (PGR student), Smith, L. (PGR student), Thornley, W. (PGR student), Yang, J. (PGR student), Young, W. (PGR student), Zhao, M. (PGR student), Al Busaidi, R. (PGR student), Al Ruqeishi, E. (PGR student), Chadha, A. (PGR student), Chen, M. (PGR student), Dennis, G. (PGR student), Dunn, E. (PGR student), Gamblen, E. (PGR student), Gao, Y. (PGR student), Georgantas, Y. (PGR student), Jiang, Z. (PGR student), Karakasidi, A. (PGR student), Mcellistrim, A. (PGR student), Meehan, M. (PGR student), Okwelogu, E. (PGR student), Taylor, M. (PGR student), Wang, W. (PGR student), Xin, B. (PGR student), Castle, C. (PGR student), Clout, P. (PGR student), Dean, S. D. (PGR student), Fordham, A. (PGR student), Griffin, E. (PGR student), Hardwick, T. (PGR student), Hawkins-Pottier, G. (PGR student), Jones, A. (PGR student), Lewthwaite, K. (PGR student), Monteil, S. (PGR student), Moulsdale, C. (PGR student), Mullan, C. (PGR student), Orts Mercadillo, V. (PGR student), Sanderson, D. (PGR student), Skliueva, I. (PGR student), Skuse, C. (PGR student), Steiner, P. (PGR student), Winstanley, B. (PGR student), Barry, D. (PGR student), Brooks, D. (PGR student), Cai, J. (PGR student), Chen, Y. (PGR student), Chen, C. (PGR student), Draude, A. (PGR student), Emmerson, C. (PGR student), Gavriliuc, V. (PGR student), Greaves, M. (PGR student), Higgins, E. (PGR student), Mcmaster, R. (PGR student), Mcnair, R. (PGR student), O'Brien, C. (PGR student), Peasey, A. (PGR student), Pinter, G. (PGR student), Shao, S. (PGR student), Thomas, D. (PGR student), Thomas, D. (PGR student), Tsim, L. T. B. (PGR student), Wengraf, J. (PGR student), Weston, A. (PGR student), Yu, T. (PGR student), De Libero, H. (PGR student), Chan, K. C. (PGR student), Tan, Y. T. (PGR student) & Thomson, T. (CoI)
1/04/14 → 31/10/25
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