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Title: Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries

Abstract

This work describes the synthesis of aluminum sulfide (AlSx) thin films by atomic layer deposition (ALD) using tris(dimethylamido)aluminum and hydrogen sulfide. We employed a suite of in situ measurement techniques to explore the ALD AlSx growth mechanism, including quartz crystal microbalance, quadrupole mass spectrometry, and Fourier transform infrared spectroscopy. A variety of ex situ characterization techniques were used to determine the growth characteristics, morphology, elemental composition, and crystallinity of the resultant AlSx films. This study revealed that the AlSx growth was self-limiting in the temperature range 100–250 °C, and the growth per cycle decreased linearly with increasing temperature from ~0.45 Å/cycle at 100 °C to ~0.1 Å/cycle at 250 °C. The AlSx films were amorphous in this temperature range. We conducted electrochemical testing to evaluate the ALD AlSx as a potential anode material for lithium-ion batteries (LIBs). Finally, the ALD AlSx exhibited reliable cyclability over 60 discharge–charge cycles with a sustainable discharge capacity of 640 mAh/g at a current density of 100 mA/g in the voltage window of 0.6–3.5 V.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2]
  1. Univ. of Arkansas, Fayetteville, AR (United States). Department of Mechanical Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1415984
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 21; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Meng, Xiangbo, Cao, Yanqiang, Libera, Joseph A., and Elam, Jeffrey W. Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries. United States: N. p., 2017. Web. https://doi.org/10.1021/acs.chemmater.7b02175.
Meng, Xiangbo, Cao, Yanqiang, Libera, Joseph A., & Elam, Jeffrey W. Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries. United States. https://doi.org/10.1021/acs.chemmater.7b02175
Meng, Xiangbo, Cao, Yanqiang, Libera, Joseph A., and Elam, Jeffrey W. Sun . "Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries". United States. https://doi.org/10.1021/acs.chemmater.7b02175. https://www.osti.gov/servlets/purl/1415984.
@article{osti_1415984,
title = {Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries},
author = {Meng, Xiangbo and Cao, Yanqiang and Libera, Joseph A. and Elam, Jeffrey W.},
abstractNote = {This work describes the synthesis of aluminum sulfide (AlSx) thin films by atomic layer deposition (ALD) using tris(dimethylamido)aluminum and hydrogen sulfide. We employed a suite of in situ measurement techniques to explore the ALD AlSx growth mechanism, including quartz crystal microbalance, quadrupole mass spectrometry, and Fourier transform infrared spectroscopy. A variety of ex situ characterization techniques were used to determine the growth characteristics, morphology, elemental composition, and crystallinity of the resultant AlSx films. This study revealed that the AlSx growth was self-limiting in the temperature range 100–250 °C, and the growth per cycle decreased linearly with increasing temperature from ~0.45 Å/cycle at 100 °C to ~0.1 Å/cycle at 250 °C. The AlSx films were amorphous in this temperature range. We conducted electrochemical testing to evaluate the ALD AlSx as a potential anode material for lithium-ion batteries (LIBs). Finally, the ALD AlSx exhibited reliable cyclability over 60 discharge–charge cycles with a sustainable discharge capacity of 640 mAh/g at a current density of 100 mA/g in the voltage window of 0.6–3.5 V.},
doi = {10.1021/acs.chemmater.7b02175},
journal = {Chemistry of Materials},
number = 21,
volume = 29,
place = {United States},
year = {2017},
month = {10}
}

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