Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation

Stoneburner, Samuel J.; Livermore, Vanessa; McGreal, Meghan E.; Yu, Decai; Vogiatzis, Konstantinos D.; Snurr, Randall Q.; Gagliardi, Laura

doi:10.1021/acs.jpcc.7b02685

Title: Catechol-Ligated Transition Metals: A Quantum Chemical Study on a Promising System for Gas Separation

Journal Article · Fri Apr 07 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b02685· OSTI ID:1477217

^[1]; Livermore, Vanessa ^[1]; McGreal, Meghan E. ^[1]; Yu, Decai ^[2]; Vogiatzis, Konstantinos D. ^[3];

^[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

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.

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Research Organization:: Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Contributing Organization:: Minnesota Supercomputing Institute (MSI) at the University of Minnesota

Grant/Contract Number:: FG02-12ER16362; SC0008688

OSTI ID:: 1477217

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 19; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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