Predicting Partial Atomic Charges in Metal–Organic Frameworks: An Extension to Ionic MOFs
Journal Article
·
· Journal of Physical Chemistry. C
- Northwestern University, Evanston, IL (United States)
- Northwestern University, Evanston, IL (United States); Wroclaw University of Science and Technology (Poland)
Molecular simulation is an invaluable tool to predict and understand the usage of metal–organic frameworks (MOFs) for gas storage and separation applications. Accurate partial atomic charges, commonly obtained from density functional theory (DFT) calculations, are often required to model the electrostatic interactions between the MOF and adsorbates, especially when the adsorbates have dipole or quadrupole moments, such as water and CO2. Machine learning (ML) models have been previously employed to predict partial charges and avoid the computational cost associated with DFT calculations. However, previous ML models suffer from small training data sets, which limit their scope of application. In this work, we introduce two novel machine learning models, PACMOF2-neutral and PACMOF2-ionic, aimed at predicting the density-derived electrostatic and chemical (DDEC6) partial atomic charges for both neutral and ionic MOFs. These models not only yield DFT-level accuracy at a fraction of the computational cost but also demonstrate a remarkable improvement in prediction of adsorption, as validated with grand canonical Monte Carlo simulations. Furthermore, the robustness and fast computational time of the PACMOF2 models, along with their transferability to other porous materials such as covalent organic frameworks and zeolites, underscores their potential in high-throughput screening of MOFs for diverse applications.
- Research Organization:
- University of Minnesota, Minneapolis, MN (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Energy Research Scientific Computing Center (NERSC)
- Grant/Contract Number:
- SC0023454; AC02-05CH11231
- OSTI ID:
- 3010670
- Alternate ID(s):
- OSTI ID: 3007976
OSTI ID: 2510815
- Journal Information:
- Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 40 Vol. 128; ISSN 1932-7455; ISSN 1932-7447
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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