Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping

Abstract The colloidal stability of nanoparticles (NPs) is significantly affected by complex solvent‐ligand interactions, with poor solvents often inducing NP agglomeration and ligand desorption from the surface. Despite the frequent occurrence of these phenomena in post‐synthetic experiments, the u...

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Main Authors: Akhlak U. Mahmood, Mehedi H. Rizvi, Joseph B. Tracy, Yaroslava G. Yingling
Format: Article
Language:English
Published: Wiley-VCH 2025-08-01
Series:Advanced Materials Interfaces
Subjects:
Online Access:https://doi.org/10.1002/admi.202500234
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author Akhlak U. Mahmood
Mehedi H. Rizvi
Joseph B. Tracy
Yaroslava G. Yingling
author_facet Akhlak U. Mahmood
Mehedi H. Rizvi
Joseph B. Tracy
Yaroslava G. Yingling
author_sort Akhlak U. Mahmood
collection DOAJ
description Abstract The colloidal stability of nanoparticles (NPs) is significantly affected by complex solvent‐ligand interactions, with poor solvents often inducing NP agglomeration and ligand desorption from the surface. Despite the frequent occurrence of these phenomena in post‐synthetic experiments, the underlying mechanisms remain elusive. In this study, dynamic light scattering (DLS), thermogravimetric analysis (TGA), and large‐scale all‐atom molecular dynamics (MD) simulations are used to investigate solvent‐driven oleylamine ligand removal from Fe3O4 NPs. Eight experimentally relevant NP systems under replicated solvent conditions are modeled, enabling direct comparison and yielding deep insights into solvent‐mediated ligand stripping with excellent agreement. These findings reveal that ethanol's ability to strip oleylamine ligands from Fe3O4 NPs is impeded by NP agglomeration, where stripped and interdigitated ligands create a steric barrier, preventing solvent molecules from accessing the NP surface. This effect becomes more pronounced with increasing NP size due to the greater ligand surface density that enhances interdigitation. Moreover, the presence of a threshold concentration of the poor solvent in binary mixtures is identified, below which the maximum number of ligands can be stripped without initiating agglomeration. These insights provide a framework for optimizing solvent‐mediated ligand exchange, with implications for NP applications in catalysis, energy storage, optoelectronics, and biomedical engineering.
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spelling doaj-art-b572d965678041bbb50398168dfe83472025-08-25T08:06:18ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-08-011216n/an/a10.1002/admi.202500234Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand StrippingAkhlak U. Mahmood0Mehedi H. Rizvi1Joseph B. Tracy2Yaroslava G. Yingling3Department of Materials Science and Engineering NC State University Raleigh NC 27695 USADepartment of Materials Science and Engineering NC State University Raleigh NC 27695 USADepartment of Materials Science and Engineering NC State University Raleigh NC 27695 USADepartment of Materials Science and Engineering NC State University Raleigh NC 27695 USAAbstract The colloidal stability of nanoparticles (NPs) is significantly affected by complex solvent‐ligand interactions, with poor solvents often inducing NP agglomeration and ligand desorption from the surface. Despite the frequent occurrence of these phenomena in post‐synthetic experiments, the underlying mechanisms remain elusive. In this study, dynamic light scattering (DLS), thermogravimetric analysis (TGA), and large‐scale all‐atom molecular dynamics (MD) simulations are used to investigate solvent‐driven oleylamine ligand removal from Fe3O4 NPs. Eight experimentally relevant NP systems under replicated solvent conditions are modeled, enabling direct comparison and yielding deep insights into solvent‐mediated ligand stripping with excellent agreement. These findings reveal that ethanol's ability to strip oleylamine ligands from Fe3O4 NPs is impeded by NP agglomeration, where stripped and interdigitated ligands create a steric barrier, preventing solvent molecules from accessing the NP surface. This effect becomes more pronounced with increasing NP size due to the greater ligand surface density that enhances interdigitation. Moreover, the presence of a threshold concentration of the poor solvent in binary mixtures is identified, below which the maximum number of ligands can be stripped without initiating agglomeration. These insights provide a framework for optimizing solvent‐mediated ligand exchange, with implications for NP applications in catalysis, energy storage, optoelectronics, and biomedical engineering.https://doi.org/10.1002/admi.202500234agglomerationcolloidal nanoparticlesligand strippingmolecular dynamics simulationssolvent effectsTGA and DLS
spellingShingle Akhlak U. Mahmood
Mehedi H. Rizvi
Joseph B. Tracy
Yaroslava G. Yingling
Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
Advanced Materials Interfaces
agglomeration
colloidal nanoparticles
ligand stripping
molecular dynamics simulations
solvent effects
TGA and DLS
title Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
title_full Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
title_fullStr Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
title_full_unstemmed Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
title_short Agglomeration of Nanoparticles Inhibits Solvent‐Driven Ligand Stripping
title_sort agglomeration of nanoparticles inhibits solvent driven ligand stripping
topic agglomeration
colloidal nanoparticles
ligand stripping
molecular dynamics simulations
solvent effects
TGA and DLS
url https://doi.org/10.1002/admi.202500234
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AT mehedihrizvi agglomerationofnanoparticlesinhibitssolventdrivenligandstripping
AT josephbtracy agglomerationofnanoparticlesinhibitssolventdrivenligandstripping
AT yaroslavagyingling agglomerationofnanoparticlesinhibitssolventdrivenligandstripping