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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 Laboratory (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:
Journal Article: 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. doi: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. 2017. "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},
url = {https://www.osti.gov/biblio/1415984}, journal = {Chemistry of Materials},
issn = {0897-4756},
number = 21,
volume = 29,
place = {United States},
year = {Sun Oct 01 00:00:00 EDT 2017},
month = {Sun Oct 01 00:00:00 EDT 2017}
}

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Cited by: 33 works
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Works referenced in this record:

Metal sulfide nanostructures: synthesis, properties and applications in energy conversion and storage
journal, January 2012


Unsupported transition metal sulfide catalysts: From fundamentals to industrial application
journal, April 2007


Catalytic Properties of Single Layers of Transition Metal Sulfide Catalytic Materials
journal, January 2006


Gallium Sulfide-Single-Walled Carbon Nanotube Composites: High-Performance Anodes for Lithium-Ion Batteries
journal, July 2014


Atomic Layer Deposition of Gallium Sulfide Films Using Hexakis(dimethylamido)digallium and Hydrogen Sulfide
journal, December 2013


Atomic Layer Deposition of Metal Sulfide Materials
journal, January 2015


Atomic Layer Deposition of MnS: Phase Control and Electrochemical Applications
journal, January 2016


Atomic layer deposition for nanomaterial synthesis and functionalization in energy technology
journal, January 2017


(Invited) Atomic Layer Deposition of Nanophase Materials for Electrical Energy Storage
journal, September 2015


Two-dimensional MoS2: Properties, preparation, and applications
journal, March 2015


Controlled synthesis of transition metal dichalcogenide thin films for electronic applications
journal, April 2014


Growth, Optical and Structural Characterization of Layered GaS Films Prepared by Reactive RF Sputtering Method
journal, July 2005


Characterization of molecular beam epitaxy grown GaS film for GaAs surface passivation
journal, April 1999


Gallium sulfide thin film grown on GaAs(1 0 0) by microwave glow discharge
journal, March 1997


Atomic layer deposition of aluminum sulfide thin films using trimethylaluminum and hydrogen sulfide
journal, January 2015

  • Sinha, Soumyadeep; Mahuli, Neha; Sarkar, Shaibal K.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 1
  • https://doi.org/10.1116/1.4903951

Synthesis and Surface Engineering of Complex Nanostructures by Atomic Layer Deposition
journal, November 2007


Atomic Layer Deposition: An Overview
journal, January 2010


Surface chemistry of atomic layer deposition: A case study for the trimethylaluminum/water process
journal, June 2005


Crystallinity of inorganic films grown by atomic layer deposition: Overview and general trends
journal, January 2013


Atomic Layer Deposition of Nanostructured Materials for Energy and Environmental Applications
journal, January 2012


Emerging Applications of Atomic Layer Deposition for Lithium-Ion Battery Studies
journal, June 2012


Atomic layer deposition for photovoltaics: applications and prospects for solar cell manufacturing
journal, June 2012


Ultrathin Lithium-Ion Conducting Coatings for Increased Interfacial Stability in High Voltage Lithium-Ion Batteries
journal, May 2014


Coking- and Sintering-Resistant Palladium Catalysts Achieved Through Atomic Layer Deposition
journal, March 2012


Atomic layer deposition: medical and biological applications
journal, February 2013


Atomic layer deposition: A versatile technique for plasmonics and nanobiotechnology
journal, January 2012


ALD tungsten NEMS switches and tunneling devices
journal, April 2011


Tailoring nanoporous materials by atomic layer deposition
journal, January 2011


Atomic Layer Epitaxy
journal, August 1985


Atomic layer epitaxy
journal, January 1989


Molecular Level Insights into Atomic Layer Deposition of CdS by Quantum Chemical Calculations
journal, September 2010


AFM studies of polycrystalline calcium sulfide thin films grown by atomic layer deposition
journal, April 1999


Atomic Layer Deposition of SrS and BaS Thin Films Using Cyclopentadienyl Precursors
journal, May 2002


Atomic layer deposition of Cu2S for future application in photovoltaics
journal, March 2009


In 2 S 3 Atomic Layer Deposition and Its Application as a Sensitizer on TiO 2 Nanotube Arrays for Solar Energy Conversion
journal, April 2010


Atomic layer deposition of tungsten disulphide solid lubricant thin films
journal, December 2004


Atomic Layer Deposition of Titanium Disulfide Thin Films
journal, April 2007


Atomic Layer Deposition of Lead Sulfide Thin Films for Quantum Confinement
journal, August 2009


Atomic Layer Deposition of Tin Monosulfide Thin Films
journal, September 2011


Vapor-Phase Atomic-Controllable Growth of Amorphous Li 2 S for High-Performance Lithium–Sulfur Batteries
journal, October 2014


Vapor-Phase Atomic Layer Deposition of Co 9 S 8 and Its Application for Supercapacitors
journal, August 2015


Atomic Layer Deposited MoS 2 as a Carbon and Binder Free Anode in Li-ion Battery
journal, November 2014


Deposition of ultra thin CuInS 2 absorber layers by ALD for thin film solar cells at low temperature (down to 150 °C)
journal, January 2015


Atomic Layer Deposition of Li x Al y S Solid-State Electrolytes for Stabilizing Lithium-Metal Anodes
journal, April 2016


Electrochemical characteristics of aluminum sulfide for use in lithium secondary batteries
journal, December 2010


Viscous flow reactor with quartz crystal microbalance for thin film growth by atomic layer deposition
journal, August 2002


GaPO4 Sensors for Gravimetric Monitoring during Atomic Layer Deposition at High Temperatures
journal, June 2005


Indium Oxide ALD Using Cyclopentadienyl Indium and Mixtures of H 2 O and O 2
journal, October 2011


Atomic layer deposition of ultrathin and conformal Al2O3 films on BN particles
journal, August 2000


Transmission infrared spectroscopy of high area solid surfaces. A useful method for sample preparation
journal, June 1992


Infrared Studies of the Surface and Gas Phase Reactions Leading to the Growth of Titanium Nitride Thin Films from Tetrakis(dimethylamido)titanium and Ammonia
journal, December 1992


Fourier transform infrared spectroscopy studies on thermal decomposition of tetrakis-dimethyl-amido zirconium for chemical vapor deposition of ZrN
journal, December 2004


SiO 2 Atomic Layer Deposition Using Tris(dimethylamino)silane and Hydrogen Peroxide Studied by in Situ Transmission FTIR Spectroscopy
journal, April 2009


Reactions of methylamines at the Si(100)-2×1 surface
journal, June 2001


Chemistry of Diffusion Barrier Film Formation:  Adsorption and Dissociation of Tetrakis(dimethylamino)titanium on Si(100)-2 × 1
journal, March 2007


Infrared Spectroscopic Study of Decomposition of Ti(N(CH[sub 3])[sub 2])[sub 4]
journal, January 2001


Surface chemistry of precursors for film growth: pentakisdimethylamido tantalum
journal, April 1999


SH-Stretching Vibrational Spectra of Ethanethiol and tert- Butylthiol
journal, May 2009


Core electron binding energies in some Group IIIA, VB, and VIB compounds
journal, October 1973


XPS analysis of AlN thin films deposited by plasma enhanced atomic layer deposition
journal, October 2014


Ellipsometry and XPS comparative studies of thermal and plasma enhanced atomic layer deposited Al 2 O 3 -films
journal, January 2013


Atomic layer deposition of ZnS via in situ production of H2S
journal, July 2010


Superior cycle stability of nitrogen-doped graphene nanosheets as anodes for lithium ion batteries
journal, August 2011


Formation and Growth of Surface Films on Graphitic Anode Materials for Li-Ion Batteries
journal, January 2005


Works referencing / citing this record:

Metal Fluorides as Lithium-Ion Battery Materials: An Atomic Layer Deposition Perspective
journal, August 2018


Atomic layer deposition of ZnO/TiO2 nanolaminates as ultra-long life anode material for lithium-ion batteries
journal, August 2019


Atomic layer deposited zinc oxysulfide anodes in Li-ion batteries: an efficient solution for electrochemical instability and low conductivity
journal, January 2018


A revisit to atomic layer deposition of zinc oxide using diethylzinc and water as precursors
journal, December 2018


Atomic layer deposition of ZnO/TiO2 nanolaminates as ultra-long life anode material for lithium-ion batteries
journal, August 2019