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Title: Non-equilibrium insertion of lithium ions into graphite

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/d1ta02836g· OSTI ID:1787829

Graphite has been regarded as the most important anode material for currently used lithium-ion batteries due to its two-dimensional (2D) nature hosting ionic intercalations. However, the kinetic insertion of Li ions is still not well known microscopically. In this work, we investigate the real-time intercalation process of Li ions using in situ transmission electron microscopy. We observe the lithium insertion process at the atomic scale, in which the graphite layers undergo expansion, forming wrinkles and finally inhomogeneous cracks as the Li ions accumulate, different from the proposed models. Leveraging on theoretical simulations, Li-ion migration driven by an external electrical field is suggested to be induced into the irreversible wrinkled structures. This non-equilibrium behavior that occur in lithium-ion batteries can be more pronounced at a high charging rate, which will practically degrade the capacity of graphite. Furthermore, this work unveils the reaction scenario of the non-equilibrium Li-ion insertion, which benefits the understanding of the performance of graphite-based energy-storage devices.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Key Research and Development Program of China
Grant/Contract Number:
SC0012704; 2020YFB2007400
OSTI ID:
1787829
Report Number(s):
BNL-221635-2021-JAAM
Journal Information:
Journal of Materials Chemistry. A, Vol. 9, Issue 20; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (41)

Lithium Storage in Carbon Nanostructures journal July 2009
Mechanisms for Lithium Insertion in Carbonaceous Materials journal October 1995
Phase diagram of Li x C 6 journal November 1991
In‐situ structural characterizations of electrochemical intercalation of graphite compounds journal October 2019
Density Functional Theory Calculations of Alkali Metal (Li, Na, and K) Graphite Intercalation Compounds journal December 2013
Intercalation Compounds from LiH and Graphite: Relative Stability of Metastable Stages and Thermodynamic Stability of Dilute Stage I d journal March 2015
Direct Real-Time Monitoring of Stage Transitions in Graphite Intercalation Compounds journal March 2013
Operando NMR and XRD study of chemically synthesized LiC oxidation in a dry room environment journal August 2015
Visualizing the chemistry and structure dynamics in lithium-ion batteries by in-situ neutron diffraction journal October 2012
The formation of salts from graphite by strong acids journal January 1938
Intercalation compounds of graphite journal April 1981
The ultramicrostructure of commensurate graphite intercalation compounds journal May 1984
High Rate Capability of Graphite Negative Electrodes for Lithium-Ion Batteries journal January 2005
The kinetic origin of the Daumas-Hérold model for the Li-ion/graphite intercalation system journal August 2018
Understanding undesirable anode lithium plating issues in lithium-ion batteries journal January 2016
In situ detection of lithium metal plating on graphite in experimental cells journal April 2015
Graphite Lithiation under Fast Charging Conditions: Atomistic Modeling Insights journal March 2020
A review on energy chemistry of fast-charging anodes journal January 2020
Identifying rate limitation and a guide to design of fast‐charging Li‐ion battery journal December 2019
Surface structural disordering in graphite upon lithium intercalation/deintercalation journal June 2010
Reversible superdense ordering of lithium between two graphene sheets journal November 2018
Mathematical Modeling of the Lithium Deposition Overcharge Reaction in Lithium-Ion Batteries Using Carbon-Based Negative Electrodes journal January 1999
In Situ Observation of the Electrochemical Lithiation of a Single SnO2 Nanowire Electrode journal December 2010
Visualizing non-equilibrium lithiation of spinel oxide via in situ transmission electron microscopy journal May 2016
On the irreversible sodiation of tin disulfide journal January 2021
Expanded graphite as superior anode for sodium-ion batteries journal June 2014
Overcharging a lithium-ion battery: Effect on the LixC6 negative electrode determined by in situ neutron diffraction journal December 2013
Electron irradiation of nuclear graphite studied by transmission electron microscopy and electron energy loss spectroscopy journal March 2015
Accurate Measurement of Electron Beam Induced Displacement Cross Sections for Single-Layer Graphene journal May 2012
In situ transmission electron microscopy of electrochemical lithiation, delithiation and deformation of individual graphene nanoribbons journal August 2012
Intercalation events visualized in single microcrystals of graphite journal December 2017
Lithium intercalation into bilayer graphene journal January 2019
Large Reversible Li Storage of Graphene Nanosheet Families for Use in Rechargeable Lithium Ion Batteries journal August 2008
Li-insertion in hard carbon anode materials for Li-ion batteries journal September 1999
X-ray diffraction patterns of graphite and turbostratic carbon journal July 2007
Raman Spectrum of Graphite journal August 1970
General equation for the determination of the crystallite size La of nanographite by Raman spectroscopy journal April 2006
Observation of zigzag and armchair edges of graphite using scanning tunneling microscopy and spectroscopy journal May 2005
Lithium-intercalated graphite: Self-consistent electronic structure for stages one, two, and three journal July 1983
Ab Initio Investigations of Lithium Diffusion in Carbon Nanotube Systems journal February 2002
A novel perspective on the formation of the solid electrolyte interphase on the graphite electrode for lithium-ion batteries journal February 2010

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