Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials

Abstract Disordered rock-salt oxides and oxyfluorides are promising positive electrode materials for high-performance lithium-ion batteries free of nickel and cobalt. However, conventional synthesis methods rely on post-synthesis pulverization to achieve cycling-appropriate particle sizes, offering...

Full description

Saved in:
Bibliographic Details
Main Authors: Hoda Ahmed, Moohyun Woo, Nicolas Dumaresq, Pablo Trevino Lara, Richie Fong, Sang-Jun Lee, Gregory Lazaris, Nauman Mubarak, Nicolas Brodusch, Dong-Hwa Seo, Raynald Gauvin, George P. Demopoulos, Jinhyuk Lee
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-60946-4
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1849334602322149376
author Hoda Ahmed
Moohyun Woo
Nicolas Dumaresq
Pablo Trevino Lara
Richie Fong
Sang-Jun Lee
Gregory Lazaris
Nauman Mubarak
Nicolas Brodusch
Dong-Hwa Seo
Raynald Gauvin
George P. Demopoulos
Jinhyuk Lee
author_facet Hoda Ahmed
Moohyun Woo
Nicolas Dumaresq
Pablo Trevino Lara
Richie Fong
Sang-Jun Lee
Gregory Lazaris
Nauman Mubarak
Nicolas Brodusch
Dong-Hwa Seo
Raynald Gauvin
George P. Demopoulos
Jinhyuk Lee
author_sort Hoda Ahmed
collection DOAJ
description Abstract Disordered rock-salt oxides and oxyfluorides are promising positive electrode materials for high-performance lithium-ion batteries free of nickel and cobalt. However, conventional synthesis methods rely on post-synthesis pulverization to achieve cycling-appropriate particle sizes, offering limited control over particle microstructure and crystallinity. This accelerates degradation and complicates secondary particle processing. Here we present a synthesis strategy that enhances nucleation while suppressing particle growth and agglomeration across various disordered rock-salt compositions, including lithium–manganese–titanium oxide, lithium–manganese–niobium oxide, and lithium–nickel–titanium oxide systems. Applied to Li1.2Mn0.4Ti0.4O2, this method yields highly crystalline, well-dispersed sub-200 nm particles that form homogeneous electrode films with stable cycling behavior. Tested in cells with lithium metal as the counter electrode, these electrodes deliver ~200 mAh/g with 85% capacity retention relative to the first cycle after 100 cycles (20 mA/g, 1.5–4.8 V), and an average discharge voltage loss of 4.8 mV per cycle, compared to 38.6% retention and 7.5 mV loss per cycle for electrodes derived from pulverized solid-state particles. This approach suggests a route to enhance the performance and durability of disordered rock-salt electrodes for sustainable lithium-ion batteries.
format Article
id doaj-art-4292bb31d31d4b5e97a2ac33fdf0ab60
institution Kabale University
issn 2041-1723
language English
publishDate 2025-07-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-4292bb31d31d4b5e97a2ac33fdf0ab602025-08-20T03:45:31ZengNature PortfolioNature Communications2041-17232025-07-0116111510.1038/s41467-025-60946-4Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materialsHoda Ahmed0Moohyun Woo1Nicolas Dumaresq2Pablo Trevino Lara3Richie Fong4Sang-Jun Lee5Gregory Lazaris6Nauman Mubarak7Nicolas Brodusch8Dong-Hwa Seo9Raynald Gauvin10George P. Demopoulos11Jinhyuk Lee12Department of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityStanford Synchrotron Radiation Lightsource, SLAC National Accelerator LaboratoryDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST)Department of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityDepartment of Mining and Materials Engineering, McGill UniversityAbstract Disordered rock-salt oxides and oxyfluorides are promising positive electrode materials for high-performance lithium-ion batteries free of nickel and cobalt. However, conventional synthesis methods rely on post-synthesis pulverization to achieve cycling-appropriate particle sizes, offering limited control over particle microstructure and crystallinity. This accelerates degradation and complicates secondary particle processing. Here we present a synthesis strategy that enhances nucleation while suppressing particle growth and agglomeration across various disordered rock-salt compositions, including lithium–manganese–titanium oxide, lithium–manganese–niobium oxide, and lithium–nickel–titanium oxide systems. Applied to Li1.2Mn0.4Ti0.4O2, this method yields highly crystalline, well-dispersed sub-200 nm particles that form homogeneous electrode films with stable cycling behavior. Tested in cells with lithium metal as the counter electrode, these electrodes deliver ~200 mAh/g with 85% capacity retention relative to the first cycle after 100 cycles (20 mA/g, 1.5–4.8 V), and an average discharge voltage loss of 4.8 mV per cycle, compared to 38.6% retention and 7.5 mV loss per cycle for electrodes derived from pulverized solid-state particles. This approach suggests a route to enhance the performance and durability of disordered rock-salt electrodes for sustainable lithium-ion batteries.https://doi.org/10.1038/s41467-025-60946-4
spellingShingle Hoda Ahmed
Moohyun Woo
Nicolas Dumaresq
Pablo Trevino Lara
Richie Fong
Sang-Jun Lee
Gregory Lazaris
Nauman Mubarak
Nicolas Brodusch
Dong-Hwa Seo
Raynald Gauvin
George P. Demopoulos
Jinhyuk Lee
Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
Nature Communications
title Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
title_full Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
title_fullStr Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
title_full_unstemmed Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
title_short Nucleation-promoting and growth-limiting synthesis of disordered rock-salt Li-ion cathode materials
title_sort nucleation promoting and growth limiting synthesis of disordered rock salt li ion cathode materials
url https://doi.org/10.1038/s41467-025-60946-4
work_keys_str_mv AT hodaahmed nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT moohyunwoo nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT nicolasdumaresq nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT pablotrevinolara nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT richiefong nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT sangjunlee nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT gregorylazaris nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT naumanmubarak nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT nicolasbrodusch nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT donghwaseo nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT raynaldgauvin nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT georgepdemopoulos nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials
AT jinhyuklee nucleationpromotingandgrowthlimitingsynthesisofdisorderedrocksaltliioncathodematerials