In-plane staging in lithium-ion intercalation of bilayer graphene

Thomas Astles, James G. McHugh, Rui Zhang, Qian Guo, Madeleine Howe, Zefei Wu, Kornelia Indykiewicz, Alex Summerfield, Zachary A. H. Goodwin, Sergey Slizovskiy, Daniil Domaretskiy, Andre K. Geim, Vladimir Falko () and Irina V. Grigorieva ()
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Thomas Astles: University of Manchester
James G. McHugh: University of Manchester
Rui Zhang: University of Manchester
Qian Guo: University of Manchester
Madeleine Howe: University of Manchester
Zefei Wu: University of Manchester
Kornelia Indykiewicz: University of Manchester
Alex Summerfield: University of Manchester
Zachary A. H. Goodwin: University of Manchester
Sergey Slizovskiy: University of Manchester
Daniil Domaretskiy: University of Manchester
Andre K. Geim: University of Manchester
Vladimir Falko: University of Manchester
Irina V. Grigorieva: University of Manchester

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract The ongoing efforts to optimize rechargeable 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. Transitions between the stages occur rapidly (within 1 sec) over the entire device area. 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.

Date: 2024
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DOI: 10.1038/s41467-024-51196-x

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