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Title: Functionalizing the Surface of Lithium-Metal Anodes

Abstract

Metal-air batteries are an important aspect of many beyond lithium ion research efforts. However, as our understanding of how molecular oxygen can act as a rechargeable cathode has progressed; the problems associated with how these materials at various states of charge interact with the lithium metal anode are only beginning to come to the surface. In this study we have devised a method to coat the surface a lithium with a functional group to act as either an anchor for further derivation studies or be polymerized to create a nanometer thick polymer coating attached to the surface by silane groups. These stable films, formed by polymerization of vinyl substituents, lower cell impedance at the electrode and over the first 50 cycles, increase cycling efficiency and demonstrate lower capacity fade.

Authors:
 [1];  [1];  [2];  [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Northern Illinois Univ., DeKalb, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1392338
Grant/Contract Number:
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemPlusChem
Additional Journal Information:
Journal Volume: 80; Journal Issue: 2; Journal ID: ISSN 2192-6506
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium; polymers; silanes; batteries; coating; electrochemistry; lithium metal; lithium metal, coating, batteries; surface chemistry

Citation Formats

Buonaiuto, Megan, Neuhold, Susanna, Schroeder, David J., Lopez, Carmen M., and Vaughey, John T.. Functionalizing the Surface of Lithium-Metal Anodes. United States: N. p., 2014. Web. doi:10.1002/cplu.201402084.
Buonaiuto, Megan, Neuhold, Susanna, Schroeder, David J., Lopez, Carmen M., & Vaughey, John T.. Functionalizing the Surface of Lithium-Metal Anodes. United States. doi:10.1002/cplu.201402084.
Buonaiuto, Megan, Neuhold, Susanna, Schroeder, David J., Lopez, Carmen M., and Vaughey, John T.. Wed . "Functionalizing the Surface of Lithium-Metal Anodes". United States. doi:10.1002/cplu.201402084. https://www.osti.gov/servlets/purl/1392338.
@article{osti_1392338,
title = {Functionalizing the Surface of Lithium-Metal Anodes},
author = {Buonaiuto, Megan and Neuhold, Susanna and Schroeder, David J. and Lopez, Carmen M. and Vaughey, John T.},
abstractNote = {Metal-air batteries are an important aspect of many beyond lithium ion research efforts. However, as our understanding of how molecular oxygen can act as a rechargeable cathode has progressed; the problems associated with how these materials at various states of charge interact with the lithium metal anode are only beginning to come to the surface. In this study we have devised a method to coat the surface a lithium with a functional group to act as either an anchor for further derivation studies or be polymerized to create a nanometer thick polymer coating attached to the surface by silane groups. These stable films, formed by polymerization of vinyl substituents, lower cell impedance at the electrode and over the first 50 cycles, increase cycling efficiency and demonstrate lower capacity fade.},
doi = {10.1002/cplu.201402084},
journal = {ChemPlusChem},
number = 2,
volume = 80,
place = {United States},
year = {Wed Sep 03 00:00:00 EDT 2014},
month = {Wed Sep 03 00:00:00 EDT 2014}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 5works
Citation information provided by
Web of Science

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  • Lithium (Li) metal batteries (LMBs) are regarded as the most promising power sources for electric vehicles. Besides the Li dendrite growth and low Li Coulombic efficiency, how to well match Li metal anode with a high loading (normally over 3.0 mAh cm-2) cathode is another key challenge to achieve the real high energy density battery. In this work, we systematically investigate the effects of the Li metal capacity usage in each cycle, manipulated by varying the cathode areal loading, on the stability of Li metal anode and the cycling performance of LMBs using the LiNi1/3Mn1/3Co1/3O2 (NMC) cathode and an additive-containingmore » dual-salt/carbonate-solvent electrolyte. It is demonstrated that the Li||NMC cells show decent long-term cycling performance even with NMC areal capacity loading up to ca. 4.0 mAh cm-2 and at a charge current density of 1.0 mA cm-2. The increase of the Li capacity usage in each cycle causes variation in the components of the solid electrolyte interphase (SEI) layer on Li metal anode and generates more ionic conductive species from this electrolyte. Further study reveals for the first time that the degradation of Li metal anode and the thickness of SEI layer on Li anode show linear relationship with the areal capacity of NMC cathode. Meanwhile, the expansion rate of consumed Li and the ratio of SEI thickness to NMC areal loading are kept almost the same value with increasing cathode loading, respectively. These fundamental findings provide new perspectives on the rational evaluation of Li metal anode stability for the development of rechargeable LMBs.« less
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  • We report that lithium (Li) metal batteries (LMBs) have recently attracted extensive interest in the energy-storage field after silence from the public view for several decades. However, many challenges still need to be overcome before their practical application, especially those that are related to the interfacial instability of Li metal anodes. Here, we reveal for the first time that the thickness of the degradation layer on the metallic Li anode surface shows a linear relationship with Li areal capacity utilization up to 4.0 mAh cm -2 in a practical LMB system. The increase in Li capacity utilization in each cyclemore » causes variations in the morphology and composition of the degradation layer on the Li anode. Under high Li capacity utilization, the current density for charge (i.e., Li deposition) is identified to be a key factor controlling the corrosion of the Li metal anode. Lastly, these fundamental findings provide new perspectives for the development of rechargeable LMBs.« less
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    Cited by 8