Journal article icon

Journal article

Modelling ligand exchange in metal complexes with machine learning potentials

Abstract:
Metal ions are irreplaceable in many areas of chemistry, including (bio)catalysis, self-assembly and charge transfer processes. Yet, modelling their structural and dynamic properties in diverse chemical environments remains challenging for both force fields and ab initio methods. Here, we introduce a strategy to train machine learning potentials (MLPs) using MACE, an equivariant message-passing neural network, for metal–ligand complexes in explicit solvents. We explore the structure and ligand exchange dynamics of Mg2+ in water and Pd2+ in acetonitrile as two illustrative model systems. The trained potentials accurately reproduce equilibrium structures of the complexes in solution, including different coordination numbers and geometries. Furthermore, the MLPs can model structural changes between metal ions and ligands in the first coordination shell, and reproduce the free energy barriers for the corresponding ligand exchange. The strategy presented here provides a computationally efficient approach to model metal ions in solution, paving the way for modelling larger and more diverse metal complexes relevant to biomolecules and supramolecular assemblies.
Publication status:
Published
Peer review status:
Peer reviewed

Actions


Access Document


Publisher copy:
10.1039/d4fd00140k

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
ORCID:
0000-0002-6293-5616
More by this author
Role:
Author
ORCID:
0000-0002-2869-461X
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
ORCID:
0000-0002-6326-9774
More by this author
Role:
Author
ORCID:
0000-0002-8498-3061
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
ORCID:
0000-0002-6062-8209


More from this funder
Funder identifier:
https://ror.org/0439y7842
Grant:
EP/P020267/1


Publisher:
Royal Society of Chemistry
Journal:
Faraday Discussions More from this journal
Volume:
256
Pages:
156-176
Place of publication:
England
Publication date:
2024-08-03
Acceptance date:
2024-07-31
DOI:
EISSN:
1364-5498
ISSN:
1359-6640
Pmid:
39308396


Language:
English
Pubs id:
2032264
Local pid:
pubs:2032264
Deposit date:
2025-02-28

Terms of use



Views and Downloads






If you are the owner of this record, you can report an update to it here: Report update to this record

TO TOP