Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation
Abstract
We report that metal-organic frameworks (MOFs) have received a great deal of attention for their potential in atmospheric filtering, and recent work has shown that catecholate linkers can bind metals, creating MOFs with monocatecholate metal centers and abundant open coordination sites. In this study, M-catecholate systems (with M = Mg2+, Sc2+, Ti2+, V2+, Cr2+, Mn2+, Fe2+, Co2+, Ni2+, Cu2+, and Zn2+) were used as computational models of metalated catecholate linkers in MOFs. Nitric oxide (NO) is a radical molecule that is considered an environmental pollutant and is toxic if inhaled in large quantities. Binding NO is of interest in creating atmospheric filters, both at the industrial and personal scale. The binding energies of NO to the metal-catecholate systems were calculated using density functional theory (DFT) and complete active space self-consistent field (CASSCF) followed by second order perturbation (CASPT2). Selectivity was studied by calculating the binding energies of additional guests (CO, NH3, H2O, N2, and CO2). The toxic guests have stronger binding than the benign guests for all metals studied, and NO has significantly stronger binding than other guests for most of the metals studied, suggesting that metal-catecholates are worthy of further study for NO filtration. Finally, certain metal-catecholates also showedmore »
- Authors:
-
[1];
[4];
[1]
- Univ. of Minnesota, Minneapolis, MN (United States). Department of Chemistry, Minnesota Supercomputing Institute, and Chemical Theory Center
- The Dow Chemical Company, Midland, MI (United States). Core Research and Development
- Univ. of Tennessee, Knoxville, TN (United States). Department of Chemistry
- Northwestern Univ., Evanston, IL (United States). Department of Chemical & Biological Engineering
- Publication Date:
- Research Org.:
- Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- Contributing Org.:
- Minnesota Supercomputing Institute (MSI) at the University of Minnesota
- OSTI Identifier:
- 1477217
- Grant/Contract Number:
- FG02-12ER16362; SC0008688
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 19; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Stoneburner, Samuel J., Livermore, Vanessa, McGreal, Meghan E., Yu, Decai, Vogiatzis, Konstantinos D., Snurr, Randall Q., and Gagliardi, Laura. Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b02685.
Stoneburner, Samuel J., Livermore, Vanessa, McGreal, Meghan E., Yu, Decai, Vogiatzis, Konstantinos D., Snurr, Randall Q., & Gagliardi, Laura. Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation. United States. https://doi.org/10.1021/acs.jpcc.7b02685
Stoneburner, Samuel J., Livermore, Vanessa, McGreal, Meghan E., Yu, Decai, Vogiatzis, Konstantinos D., Snurr, Randall Q., and Gagliardi, Laura. Fri .
"Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation". United States. https://doi.org/10.1021/acs.jpcc.7b02685. https://www.osti.gov/servlets/purl/1477217.
@article{osti_1477217,
title = {Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation},
author = {Stoneburner, Samuel J. and Livermore, Vanessa and McGreal, Meghan E. and Yu, Decai and Vogiatzis, Konstantinos D. and Snurr, Randall Q. and Gagliardi, Laura},
abstractNote = {We report that metal-organic frameworks (MOFs) have received a great deal of attention for their potential in atmospheric filtering, and recent work has shown that catecholate linkers can bind metals, creating MOFs with monocatecholate metal centers and abundant open coordination sites. In this study, M-catecholate systems (with M = Mg2+, Sc2+, Ti2+, V2+, Cr2+, Mn2+, Fe2+, Co2+, Ni2+, Cu2+, and Zn2+) were used as computational models of metalated catecholate linkers in MOFs. Nitric oxide (NO) is a radical molecule that is considered an environmental pollutant and is toxic if inhaled in large quantities. Binding NO is of interest in creating atmospheric filters, both at the industrial and personal scale. The binding energies of NO to the metal-catecholate systems were calculated using density functional theory (DFT) and complete active space self-consistent field (CASSCF) followed by second order perturbation (CASPT2). Selectivity was studied by calculating the binding energies of additional guests (CO, NH3, H2O, N2, and CO2). The toxic guests have stronger binding than the benign guests for all metals studied, and NO has significantly stronger binding than other guests for most of the metals studied, suggesting that metal-catecholates are worthy of further study for NO filtration. Finally, certain metal-catecholates also showed potential for separation of N2 and CO2 via N2 activation, which could be relevant for carbon capture or ammonia synthesis.},
doi = {10.1021/acs.jpcc.7b02685},
journal = {Journal of Physical Chemistry. C},
number = 19,
volume = 121,
place = {United States},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}
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