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Title: Atomic layer deposition of lithium zirconium oxides for the improved performance of lithium-ion batteries

Journal Article · · Dalton Transactions
DOI: https://doi.org/10.1039/d1dt03600a · OSTI ID:1889159
 [1];  [2]; ORCiD logo [2]; ORCiD logo [2];  [3];  [4]; ORCiD logo [2]
  1. Univ. of Arkansas, Fayetteville, AR (United States); Northeast Forestry University (China)
  2. Univ. of Arkansas, Fayetteville, AR (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Recently there has been increasing interest to develop lithium-containing films as solid-state electrolytes or surface coatings for lithium-ion batteries (LIBs) and related systems. Here, in this study, we for the first time investigated the thin film growth of lithium zirconium oxides (LixZryO or LZOs) through combining two individual atomic layer deposition (ALD) processes of ZrO2 and LiOH, i.e., sub-ALD of ZrO2 and LiOH. We revealed that the hygroscopic nature of the LiOH component has a big impact on the growth of LZOs. We found that an increased temperature to 225 °C was more effective than an elongated purge to mitigate the adverse effects of physisorbed H2O. We further discovered that, during the resultant LZO super-ALD processes, the growth of sub-ALD LiOH has been promoted while the growth of sub-ALD ZrO2 has been inhibited. In this study, a suite of instruments has been applied to characterize the LZO super-ALD processes and the resultant LZO films, including in situ quartz crystal microbalance (QCM), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM), atomic force microscopy (AFM), synchrotron-based X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Furthermore, we applied the resulting LZO films over LiNi0.6Mn0.2Co0.2O2 (NMC622) cathodes in LIBs and demonstrated that the LZO coating films could evidently improve the lithium-ion insertion and extraction rates of the NMC622 electrodes up to 3.4 and 2.6 times, respectively. The LZO-coated NMC622 cathodes exhibited much better performance than the uncoated NMC622 ones.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704; AC02-06CH11357
OSTI ID:
1889159
Report Number(s):
BNL-223467-2022-JAAM
Journal Information:
Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 7 Vol. 51; ISSN 1477-9226
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (45)

Emerging Applications of Atomic Layer Deposition for Lithium-Ion Battery Studies journal June 2012
Prospect and Reality of Ni-Rich Cathode for Commercialization journal November 2017
La doping and coating enabled by one-step method for high performance Li1.2Mn0.54Ni0.13Co0.13O2 Li-rich cathode journal May 2020
Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries journal October 2019
Controlled synthesis of Zirconium Oxide on graphene nanosheets by atomic layer deposition and its growth mechanism journal February 2013
A perspective on nickel-rich layered oxide cathodes for lithium-ion batteries journal January 2017
Problems and their origins of Ni-rich layered oxide cathode materials journal January 2020
Atomic layer deposition of solid-state electrolytes for next-generation lithium-ion batteries and beyond: Opportunities and challenges journal September 2020
Understanding of performance degradation of LiNi0.80Co0.10Mn0.10O2 cathode material operating at high potentials journal February 2020
Recent progress of surface coating on cathode materials for high-performance lithium-ion batteries journal April 2020
Atomic-scale tuned interface of nickel-rich cathode for enhanced electrochemical performance in lithium-ion batteries journal October 2020
Effect of interface modifications on voltage fade in 0.5Li2MnO3·0.5LiNi0.375Mn0.375Co0.25O2 cathode materials journal March 2014
Plasma enhanced atomic layer deposition of a (nitrogen doped) Ti phosphate coating for improved energy storage in Li-ion batteries journal June 2021
Surface modifications of electrode materials for lithium ion batteries journal February 2006
Atomic Layer Deposition of the Solid Electrolyte LiPON journal July 2015
Atomic Layer Deposition of Aluminum Sulfide: Growth Mechanism and Electrochemical Evaluation in Lithium-Ion Batteries journal October 2017
Highly Reversible Conversion-Type FeOF Composite Electrode with Extended Lithium Insertion by Atomic Layer Deposition LiPON Protection journal October 2017
Surface Modification for Suppressing Interfacial Parasitic Reactions of a Nickel-Rich Lithium-Ion Cathode journal March 2019
Atomic Layer Deposition of Nitrogen-Doped Al Phosphate Coatings for Li-Ion Battery Applications journal May 2020
Understanding the Stabilizing Effects of Nanoscale Metal Oxide and Li–Metal Oxide Coatings on Lithium-Ion Battery Positive Electrode Materials journal September 2021
Atomic Layer Deposition of Lithium Niobium Oxides as Potential Solid-State Electrolytes for Lithium-Ion Batteries journal January 2018
Enhanced Surface Chemical and Structural Stability of Ni-Rich Cathode Materials by Synchronous Lithium-Ion Conductor Coating for Lithium-Ion Batteries journal February 2020
Atomic Layer Deposition of Stable LiAlF 4 Lithium Ion Conductive Interfacial Layer for Stable Cathode Cycling journal July 2017
Atomic Layer Deposition of Gallium Sulfide Films Using Hexakis(dimethylamido)digallium and Hydrogen Sulfide journal December 2013
Ultrathin Lithium-Ion Conducting Coatings for Increased Interfacial Stability in High Voltage Lithium-Ion Batteries journal May 2014
Atomic Layer Deposition: An Overview journal January 2010
Crystallinity-Controlled Synthesis of Zirconium Oxide Thin Films on Nitrogen-Doped Carbon Nanotubes by Atomic Layer Deposition journal June 2012
Mechanistic Study of Lithium Aluminum Oxide Atomic Layer Deposition journal January 2013
Atomic Layer Deposition of Lithium Tantalate Solid-State Electrolytes journal September 2013
Vapor-Phase Atomic-Controllable Growth of Amorphous Li 2 S for High-Performance Lithium–Sulfur Batteries journal October 2014
Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries journal June 2018
Effect of Low-Temperature Al2O3 ALD Coating on Ni-Rich Layered Oxide Composite Cathode on the Long-Term Cycling Performance of Lithium-Ion Batteries journal March 2019
Atomic layer deposition of solid-state electrolyte coated cathode materials with superior high-voltage cycling behavior for lithium ion battery application journal January 2014
Surface modification of cathode materials from nano- to microscale for rechargeable lithium-ion batteries journal January 2010
Interfacing electrolytes with electrodes in Li ion batteries journal January 2011
Controllable synthesis of graphene-based titanium dioxide nanocomposites by atomic layer deposition journal March 2011
Atomic-scale constituting stable interface for improved LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes of lithium-ion batteries journal December 2020
Why do batteries fail? journal February 2016
Atomic Layer Deposition of LiOH and Li conference January 2010
Multifunctional Films Deposited by Atomic Layer Deposition for Tailored Interfaces of Electrochemical Systems journal November 2020
Monitoring the Heterogeneous Reaction of LiH and LiOH with H 2 O and CO 2 by Diffuse Reflectance Infrared Fourier Transform Spectroscopy journal January 1983
The Solid Electrolyte Interphase – The Most Important and the Least Understood Solid Electrolyte in Rechargeable Li Batteries journal December 2009
Atomic layer deposition of zirconium oxide thin films journal November 2019
ALD for clean energy conversion, utilization, and storage journal November 2011
Atomic and molecular layer deposition in pursuing better batteries journal January 2021