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Title: Interfacial Li-ion localization in hierarchical carbon anodes

Journal Article · · Carbon
 [1];  [2];  [1]; ORCiD logo [1]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
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An understanding of the nanoscale structure and energetics of carbon composites is critical for their applications in electric energy storage. Here, we study the properties of carbon anodes synthesized from low-cost renewable lignin biopolymers for use in energy storage applications such as Li-ion batteries. The anodes possess both nanoscale and mesoscale order, consisting of carbon nanocrystallites distributed within an amorphous carbon matrix. Molecular dynamics simulations of an experimentally validated model of the anode is used to elucidate the nature of Li-ion storage. We report the discovery of a novel mechanism of Li-ion storage, one in which Li+ is not intercalated between layers of carbon (as is the case in graphitic anodes), but rather is localized at the interface of crystalline carbon domains. In particular, the effects of Li-ion binding energy on the Li-Li, Li-H, and Li-C pair distribution functions are revealed, along with the effect on charge distribution. As a result, the atomic environments surrounding the Li-ions are grouped on the basis of ion energy and then convolved into archetypal structural motifs that reveal deep insight into the geometry of ion localization in disordered systems.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Manufacturing Demonstration Facility (MDF); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Critical Materials Institute (CMI)
Sponsoring Organization:
Work for Others (WFO); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1333661
Alternate ID(s):
OSTI ID: 1411074
Journal Information:
Carbon, Vol. 111, Issue C; ISSN 0008-6223
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

References (19)

Materials and processing for lithium-ion batteries journal September 2008
Highly Robust Lithium Ion Battery Anodes from Lignin: An Abundant, Renewable, and Low-Cost Material journal August 2013
Carbon–carbon composite as anodes for lithium-ion battery systems journal June 2001
Defect-induced plating of lithium metal within porous graphene networks journal April 2014
Mechanisms for Lithium Insertion in Carbonaceous Materials journal October 1995
Lithium Insertion in High Capacity Carbonaceous Materials journal January 1995
Lithium Insertion in Disordered Carbon−Hydrogen Alloys:  Intercalation vs Covalent Binding journal January 1996
Ab Initio Molecular Dynamics Investigation of Singlet C2H2Li2: Determination of the Ground State Structure and Observation of LiH Intermediates journal January 1995
Structural analysis of lignin-derived carbon composite anodes journal September 2014
Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids journal January 1996
ReaxFF:  A Reactive Force Field for Hydrocarbons journal October 2001
Reactive Molecular Dynamics: Numerical Methods and Algorithmic Techniques journal January 2012
Reactive Force Field Study of Li/C Systems for Electrical Energy Storage journal April 2015
Binding and Diffusion of Lithium in Graphite: Quantum Monte Carlo Benchmarks and Validation of van der Waals Density Functional Methods journal November 2014
Self-weakening in lithiated graphene electrodes journal March 2013
Rapid estimation of elastic constants by molecular dynamics simulation under constant stress journal April 2004
Canonical dynamics: Equilibrium phase-space distributions journal March 1985
Fast Parallel Algorithms for Short-Range Molecular Dynamics journal March 1995
Operando NMR and XRD study of chemically synthesized LiC oxidation in a dry room environment journal August 2015

Cited By (4)

A stable cardinality distance for topological classification journal November 2019
Increasing the revenue from lignocellulosic biomass: Maximizing feedstock utilization journal May 2017
Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function journal February 2018
A Stable Cardinality Distance for Topological Classification preprint January 2018

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