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Hui J, Burgess M, Zhang J, et al. Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution. ACS Nano. 2016;10(4):4248-57doi: 10.1021/acsnano.5b07692.
Hui, J., Burgess, M., Zhang, J., & Rodríguez-López, J. (2016). Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution. ACS nano, 10(4), 4248-57. https://doi.org/10.1021/acsnano.5b07692
Hui, Jingshu, et al. "Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution." ACS nano vol. 10,4 (2016): 4248-57. doi: https://doi.org/10.1021/acsnano.5b07692
Hui J, Burgess M, Zhang J, Rodríguez-López J. Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution. ACS Nano. 2016 Apr 26;10(4):4248-57. doi: 10.1021/acsnano.5b07692. Epub 2016 Mar 14. PMID: 26943950.
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ACS Nano. 2016 Apr 26;10(4):4248-57. doi: 10.1021/acsnano.5b07692. Epub 2016 Mar 14.

Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution.

ACS nano

Jingshu Hui, Mark Burgess, Jiarui Zhang, Joaquín Rodríguez-López

Affiliations

  1. Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign , 1304 West Green Street, Urbana, Illinois 61801, United States.
  2. Department of Chemistry, University of Illinois at Urbana-Champaign , 600 South Mathews Avenue, Urbana, Illinois 61801, United States.

PMID: 26943950 DOI: 10.1021/acsnano.5b07692

Abstract

A fundamental question facing electrodes made out of few layers of graphene (FLG) is if they display chemical properties that are different to their bulk graphite counterpart. Here, we show evidence that suggests that lithium ion intercalation on FLG, as measured via stationary voltammetry, shows a strong dependence on the number of layers of graphene that compose the electrode. Despite its extreme thinness and turbostratic structure, Li ion intercalation into FLG still proceeds through a staging process, albeit with different signatures than bulk graphite or multilayer graphene. Single-layer graphene does not show any evidence of ion intercalation, while FLG with four graphene layers displays limited staging peaks, which broaden and increase in number as the layer number increases to six. Despite these mechanistic differences on ion intercalation, the formation of a solid-electrolyte interphase (SEI) was observed on all electrodes. Scanning electrochemical microscopy (SECM) in the feedback mode was used to demonstrate changes in the surface conductivity of FLG during SEI evolution. Observation of ion intercalation on large area FLG was conditioned to the fabrication of "ionic channels" on the electrode. SECM measurements using a recently developed Li-ion sensitive imaging technique evidenced the role of these channels in enabling Li-ion intercalation through localized flux measurements. This work highlights the impact of nanostructure and microstructure on macroscopic electrochemical behavior and provides guidance to the mechanistic control of ion intercalation using graphene, an atomically thin interface where surface and bulk reactivity converge.

Keywords: Li intercalation; SECM; SEI; graphene; layer number dependence; staging mechanism

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