CO 2 Dynamics in Pure and Mixed-Metal MOFs with Open Metal Sites

Marti, Robert M.; Howe, Joshua D.; Morelock, Cody R.; Conradi, Mark S.; Walton, Krista S.; Sholl, David S.; Hayes, Sophia E.

doi:10.1021/acs.jpcc.7b07179

Title: CO ₂ Dynamics in Pure and Mixed-Metal MOFs with Open Metal Sites

Journal Article · Wed Oct 04 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b07179· OSTI ID:1396742

^[1]; Howe, Joshua D. ^[2]; Morelock, Cody R. ^[2]; Conradi, Mark S. ^[3];

^[2];

^[1]

Department of Chemistry, Washington University, One Brookings Drive, Saint Louis, Missouri 63130, United States
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW, Atlanta, Georgia 30332, United States
Department of Chemistry, Washington University, One Brookings Drive, Saint Louis, Missouri 63130, United States, Department of Physics, Washington University, One Brookings Drive, Saint Louis, Missouri 63130, United States, ABQMR, 2301 Yale Boulevard SE, Albuquerque, New Mexico 87106, United States

Metal–organic frameworks (MOFs), such as MOF-74, can have open metal sites to which adsorbates such as CO₂ preferentially bind. ¹³C NMR of ¹³CO₂ is highly informative about the binding sites present in Mg-MOF-74. We used this technique to investigate loadings between ~0.88 and 1.15 molecules of CO₂ per metal in Mg-MOF-74 at 295 K. ¹³C lineshapes recorded as a function of loading can be understood in terms of the dependence of the CO₂ NMR frequency on the angle (θ) with respect to the CO₂ axis and the channel of the MOF, reflected in the Legendre polynomial, P₂. In the fast motion limit, the NMR spectra reveal the time-averaged value of P₂, where θ is the angle between the instantaneous CO₂ axis and the channel axis. DFT calculations were used to determine a weighted average of P₂ in this regime and are in good agreement with experimental data. Static variable temperature ¹³C NMR from cryogenic temperatures to room temperature was used to investigate ¹³CO₂ binding in Mg-MOF-74 loaded at two levels (~0.88 and 1.08 molecules of CO₂ per metal), revealing temperature-dependent lineshapes. We have investigated the effect of partial substitution of Cd for Mg in Mg-MOF-74 on the ¹³CO₂ variable temperature NMR spectra. The chemical shift anisotropy (CSA) that leads to characteristic lineshapes of ¹³C indicates that incorporation of Cd leads to weaker binding energies for adsorbed CO₂.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME); Georgia Institute of Technology, Atlanta, GA (United States); Energy Frontier Research Center (EFRC). Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012577

OSTI ID:: 1396742

Alternate ID(s):: OSTI ID: 1413259

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 121 Journal Issue: 46; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 51 works

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Title: CO ₂ Dynamics in Pure and Mixed-Metal MOFs with Open Metal Sites