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Title: Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading

Abstract

Lithium metal is considered the "holy grail" of next-generation battery anodes. However, severe parasitic reactions at the lithium—electrolyte interface deplete the liquid electrolyte and the uncontrolled formation of high surface area and dendritic lithium during cycling causes rapid capacity fading and battery failure. Engineering a dendrite-free lithium metal anode is therefore critical for the development of longlife batteries using lithium anodes. In this study, we deposit a Lithium Metal Alucone-coated Uthnun conformal, organic/inorganic hybrid coating, for the first time, directly on lithium metal using molecular layer deposition (MLD) to alleviate these problems. This hybrid organic/inorganic film with high cross-linking structure can stabilize lithium against dendrite growth and minimize side reactions, as indicated by scanning electron microscopy. We discovered that the alucone coating yielded several times longer cycle life at high current rates compared to the uncoated lithium and achieved a steady Coulombic efficiency of 99.5%, demonstrating that the highly crosslinking structured material with great mechanical properties and good flexibility can effectively suppress dendrite formation. The protected Li was further evaluated in lithium—sulfur (Li—S) batteries with a high sulfur mass loading of —5 mg/cm2. After 140 cycles at a high current rate of —1 mA/cm2, alucone-coated Li—S batteries delivered a capacitymore » of 657.7 mAh/g, 39.5% better than that of a bare lithium—sulfur battery. These findings suggest that flexible coating with high cross-linking structure by MLD is effective to enable lithium protection and offers a very promising avenue for improved performance in the real applications of Li—S batteries.« less

Authors:
 [1];  [2]; ORCiD logo [2];  [1];  [3];  [3]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Illinois, Chicago, IL (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1473942
Report Number(s):
SAND-2018-9889J
Journal ID: ISSN 1944-8244; 667715
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 8; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Chen, Lin, Huang, Zhennan, Shahbazian-Yassar, Reza, Libera, Joseph A., Klavetter, Kyle C., Zavadil, Kevin R., and Elam, Jeffrey W. Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading. United States: N. p., 2018. Web. https://doi.org/10.1021/acsami.7b15879.
Chen, Lin, Huang, Zhennan, Shahbazian-Yassar, Reza, Libera, Joseph A., Klavetter, Kyle C., Zavadil, Kevin R., & Elam, Jeffrey W. Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading. United States. https://doi.org/10.1021/acsami.7b15879
Chen, Lin, Huang, Zhennan, Shahbazian-Yassar, Reza, Libera, Joseph A., Klavetter, Kyle C., Zavadil, Kevin R., and Elam, Jeffrey W. Tue . "Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading". United States. https://doi.org/10.1021/acsami.7b15879. https://www.osti.gov/servlets/purl/1473942.
@article{osti_1473942,
title = {Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading},
author = {Chen, Lin and Huang, Zhennan and Shahbazian-Yassar, Reza and Libera, Joseph A. and Klavetter, Kyle C. and Zavadil, Kevin R. and Elam, Jeffrey W.},
abstractNote = {Lithium metal is considered the "holy grail" of next-generation battery anodes. However, severe parasitic reactions at the lithium—electrolyte interface deplete the liquid electrolyte and the uncontrolled formation of high surface area and dendritic lithium during cycling causes rapid capacity fading and battery failure. Engineering a dendrite-free lithium metal anode is therefore critical for the development of longlife batteries using lithium anodes. In this study, we deposit a Lithium Metal Alucone-coated Uthnun conformal, organic/inorganic hybrid coating, for the first time, directly on lithium metal using molecular layer deposition (MLD) to alleviate these problems. This hybrid organic/inorganic film with high cross-linking structure can stabilize lithium against dendrite growth and minimize side reactions, as indicated by scanning electron microscopy. We discovered that the alucone coating yielded several times longer cycle life at high current rates compared to the uncoated lithium and achieved a steady Coulombic efficiency of 99.5%, demonstrating that the highly crosslinking structured material with great mechanical properties and good flexibility can effectively suppress dendrite formation. The protected Li was further evaluated in lithium—sulfur (Li—S) batteries with a high sulfur mass loading of —5 mg/cm2. After 140 cycles at a high current rate of —1 mA/cm2, alucone-coated Li—S batteries delivered a capacity of 657.7 mAh/g, 39.5% better than that of a bare lithium—sulfur battery. These findings suggest that flexible coating with high cross-linking structure by MLD is effective to enable lithium protection and offers a very promising avenue for improved performance in the real applications of Li—S batteries.},
doi = {10.1021/acsami.7b15879},
journal = {ACS Applied Materials and Interfaces},
number = 8,
volume = 10,
place = {United States},
year = {2018},
month = {1}
}

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Cited by: 19 works
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Figures / Tables:

Figure 1 Figure 1: Schematic synthesis and characterization of alucone. (a) Schematic of the first cycle of alucone MLD beginning with a hydroxylated surface. (b) Facile MLD process directly coats alucone on lithium metal, forming highly cross-linking-structured alucone on the lithium foil. (c) Transmission electron microscopy (TEM) image of molecular-layer-deposited alucone filmmore » on 100 nm Si02 nanospheres. (d) Energy-dispersive Xray spectroscopy (EDS) mapping of molecular-layer-deposited alucone film on 100 nm SiO2, nanospheres.« less

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Works referencing / citing this record:

Rational design of spontaneous reactions for protecting porous lithium electrodes in lithium–sulfur batteries
journal, July 2019


Rational design of spontaneous reactions for protecting porous lithium electrodes in lithium–sulfur batteries
journal, July 2019


High Dielectric, Robust Composite Protective Layer for Dendrite‐Free and LiPF 6 Degradation‐Free Lithium Metal Anode
journal, September 2019

  • Jang, Eun Kwang; Ahn, Jinhyeok; Yoon, Sukeun
  • Advanced Functional Materials, Vol. 29, Issue 48
  • DOI: 10.1002/adfm.201905078

A Novel Organic “Polyurea” Thin Film for Ultralong-Life Lithium-Metal Anodes via Molecular-Layer Deposition
journal, December 2018


Atomic and Molecular Layer Deposition for Superior Lithium-Sulfur Batteries: Strategies, Performance, and Mechanisms
journal, May 2018

  • Sun, Qian; Lau, Kah Chun; Geng, Dongsheng
  • Batteries & Supercaps, Vol. 1, Issue 2
  • DOI: 10.1002/batt.201800024

Recent developments and insights into the understanding of Na metal anodes for Na-metal batteries
journal, January 2018

  • Zhao, Yang; Adair, Keegan R.; Sun, Xueliang
  • Energy & Environmental Science, Vol. 11, Issue 10
  • DOI: 10.1039/c8ee01373j

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.