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Title: Interfacial Li-ion localization in hierarchical carbon anodes

Abstract

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.

Authors:
 [1];  [2];  [1]; ORCiD logo [1]
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  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
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 Org.:
Work for Others (WFO); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1333661
Alternate Identifier(s):
OSTI ID: 1411074
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Carbon
Additional Journal Information:
Journal Volume: 111; Journal Issue: C; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

McNutt, Nicholas W., Rios, Orlando, Maroulas, Vasileios, and Keffer, David J. Interfacial Li-ion localization in hierarchical carbon anodes. United States: N. p., 2016. Web. doi:10.1016/j.carbon.2016.10.061.
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McNutt, Nicholas W., Rios, Orlando, Maroulas, Vasileios, & Keffer, David J. Interfacial Li-ion localization in hierarchical carbon anodes. United States. https://doi.org/10.1016/j.carbon.2016.10.061
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McNutt, Nicholas W., Rios, Orlando, Maroulas, Vasileios, and Keffer, David J. Mon . "Interfacial Li-ion localization in hierarchical carbon anodes". United States. https://doi.org/10.1016/j.carbon.2016.10.061. https://www.osti.gov/servlets/purl/1333661.
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@article{osti_1333661,
title = {Interfacial Li-ion localization in hierarchical carbon anodes},
author = {McNutt, Nicholas W. and Rios, Orlando and Maroulas, Vasileios and Keffer, David J.},
abstractNote = {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.},
doi = {10.1016/j.carbon.2016.10.061},
journal = {Carbon},
number = C,
volume = 111,
place = {United States},
year = {Mon Oct 24 00:00:00 EDT 2016},
month = {Mon Oct 24 00:00:00 EDT 2016}
}
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https://doi.org/10.1016/j.carbon.2016.10.061
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    Works referencing / citing this record:

    A stable cardinality distance for topological classification
    journal, November 2019

    • Maroulas, Vasileios; Micucci, Cassie Putman; Spannaus, Adam
    • Advances in Data Analysis and Classification, Vol. 14, Issue 3
    • DOI: 10.1007/s11634-019-00378-3

    Increasing the revenue from lignocellulosic biomass: Maximizing feedstock utilization
    journal, May 2017

    • Alonso, David Martin; Hakim, Sikander H.; Zhou, Shengfei
    • Science Advances, Vol. 3, Issue 5
    • DOI: 10.1126/sciadv.1603301

    Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function
    journal, February 2018

    • García-Negrón, Valerie; Oyedele, Akinola D.; Ponce, Eduardo
    • Journal of Applied Crystallography, Vol. 51, Issue 1
    • DOI: 10.1107/s1600576717016843

    A Stable Cardinality Distance for Topological Classification
    preprint, January 2018

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