Amine Dynamics in Diamine-Appended Mg2(dobpdc) Metal–Organic Frameworks

Xu, Jun; Liu, Yifei Michelle; Lipton, Andrew S.; Ye, Jinxing; Hoatson, Gina L.; Milner, Phillip J.; McDonald, Thomas M.; Siegelman, Rebecca L.; Forse, Alexander C.; Smit, Berend; Long, Jeffrey R.; Reimer, Jeffrey A.

doi:10.1021/acs.jpclett.9b02883

Title: Amine Dynamics in Diamine-Appended Mg₂(dobpdc) Metal–Organic Frameworks

Journal Article · Wed Oct 30 00:00:00 EDT 2019 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.9b02883· OSTI ID:1602785

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Nankai Univ., Tianjin (China); Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Univ. of California, Berkeley, CA (United States); East China Univ. of Science and Technology, Shanghai (China)
College of William and Mary, Williamsburg, VA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Univ. of California, Berkeley, CA (United States); Valais Ecole Polytechnique Fédérale de Lausanne (EPFL), Sion (Switzerland)

In this work, variable-temperature ¹⁵N solid-state NMR spectroscopy is used to uncover the dynamics of three diamines appended to the metal–organic framework Mg₂(dobpdc) (dobpdc^4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate), an important family of CO₂ capture materials. The results imply both bound and free amine nitrogen environments exist when diamines are coordinated to the framework open Mg²⁺ sites. There are rapid exchanges between two nitrogen environments for all three diamines, the rates and energetics of which are quantified by ¹⁵N solid-state NMR data and corroborated by density functional theory calculations and molecular dynamics simulations. The activation energy for the exchange provides a measure of the metal–amine bond strength. The unexpected negative correlation between the metal–amine bond strength and CO₂ adsorption step pressure reveals that metal–amine bond strength is not the only important factor in determining the CO₂ adsorption properties of diamine-appended Mg₂(dobpdc) metal–organic frameworks.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Institutes of Health (NIH); National Science foundation (NSF); National Institute of General Medical Sciences (NIGMS); National Natural Science Foundation of China (NSFC); State Key Laboratory of Fine Chemicals

Grant/Contract Number:: AC05-76RL01830; SC0001015; S10OD023532; AC02-05CH11231

OSTI ID:: 1602785

Alternate ID(s):: OSTI ID: 1605261

Report Number(s):: PNNL-SA-131857

Journal Information:: Journal of Physical Chemistry Letters, Vol. 10, Issue 22; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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Title: Amine Dynamics in Diamine-Appended Mg2(dobpdc) Metal–Organic Frameworks

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Title: Amine Dynamics in Diamine-Appended Mg₂(dobpdc) Metal–Organic Frameworks