Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles

Blake G. Hudson; Diamond T. Jones; Victoria M. Rivera Bustillo; Joseph W. Bennett; Sara E. Mason

doi:10.1021/acs.jpcc.3c02764

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Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles

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Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles

Blake G. Hudson, Diamond T. Jones, Victoria M. Rivera Bustillo, Joseph W. Bennett and Sara E. Mason

Journal of physical chemistry. C, Vol.127(43), pp.21022-21032

10/25/2023

DOI: 10.1021/acs.jpcc.3c02764

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Abstract

The transformations of complex metal oxides in aqueous settings must be studied to form a chemical understanding of how technologically relevant nanomaterials impact the environment upon disposal. Owing to the inherent heterogeneity and structural complexity of the ternary intercalation material Li(NixMnyCo1-x-y)O2 (NMC), the mechanisms of chemical processes at the solid–water interface are challenging to model. Here, density functional theory (DFT) + solvent ion methodology is used to study the energetics of stepwise release of two surface metals following unique pathways. The study spans different combinations of metal removal and also considers unique patterns of defects formed by modeling the NMC surface in supercells. The approach here also considers the equilibration of the surface with the surroundings between successive metal removals. A key finding is that a second metal removal prefers to proceed at a metal lattice site adjacent to the initial defect, and this is attributed in part to how the resulting slab with two metal vacancies maintains the most antiferromagnetic couplings between the remaining Ni/Mn.

Details

Title: Subtitle: Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles
Creators: Blake G. Hudson - University of Iowa
Diamond T. Jones - University of Iowa
Victoria M. Rivera Bustillo - Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States
Joseph W. Bennett - University of Iowa
Sara E. Mason - University of Iowa
Resource Type: Journal article
Publication Details: Journal of physical chemistry. C, Vol.127(43), pp.21022-21032
DOI: 10.1021/acs.jpcc.3c02764
ISSN: 1932-7447
eISSN: 1932-7455
Grant note: DOI: 10.13039/100008893, name: University of Iowa; DOI: 10.13039/100000001, name: National Science Foundation, award: CHE-2001611
Language: English
Date published: 10/25/2023
Academic Unit: Chemistry
Record Identifier: 9984502959302771

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