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Title: Understanding Small-Molecule Interactions in Metal-Organic Frameworks: Coupling Experiment with Theory

Abstract

Metal-organic frameworks (MOFs) have gained much attention as next generation porous media for various applications, especially gas separations/storage and catalysis. New MOFs are regularly reported; however, to develop better materials in a timely manner for specific applications, the interactions between guest molecules and the internal surface of the framework must first be understood. In this review, we present a combined experimental and theoretical approach that proves essential for the elucidation of small-molecule interactions in a model MOF system known as M 2(dobdc) (dobdc 4– = 2,5-dioxido-1,4-benzenedicarboxylate; M = Mg, Mn, Fe, Co, Ni, Cu, or Zn), a material whose adsorption properties can be readily tuned via chemical substitution. Here, we additionally show that the study of extensive families like this one can provide a platform to test the efficacy and accuracy of developing computational methodologies in slightly varying chemical environments, a task that is necessary for their evolution into viable, robust tools for screening large numbers of materials.

Authors:
 [1];  [2];  [3];  [4];  [3];  [1];  [5];  [1];  [6]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Delaware, Newark, DE (United States)
  5. Univ. of California, Berkeley, CA (United States); Ecole Polytechnique Federale de Lausanne (EPFL), Lausanne (Switzerland)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Ecole Polytechnique Federale de Lausanne (EPFL), Lausanne (Switzerland)
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1459350
Grant/Contract Number:  
FG02-12ER16362; SC0008688
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 38; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal-organic frameworks; density functional theory; gas adsorption; porous; in- situ characterization

Citation Formats

Lee, Jason S., Vlaisavljevich, Bess, Britt, David K., Brown, Craig M., Haranczyk, Maciej, Neaton, Jeffrey B., Smit, Berend, Long, Jeffrey R., and Queen, Wendy L. Understanding Small-Molecule Interactions in Metal-Organic Frameworks: Coupling Experiment with Theory. United States: N. p., 2015. Web. doi:10.1002/adma.201500966.
Lee, Jason S., Vlaisavljevich, Bess, Britt, David K., Brown, Craig M., Haranczyk, Maciej, Neaton, Jeffrey B., Smit, Berend, Long, Jeffrey R., & Queen, Wendy L. Understanding Small-Molecule Interactions in Metal-Organic Frameworks: Coupling Experiment with Theory. United States. doi:10.1002/adma.201500966.
Lee, Jason S., Vlaisavljevich, Bess, Britt, David K., Brown, Craig M., Haranczyk, Maciej, Neaton, Jeffrey B., Smit, Berend, Long, Jeffrey R., and Queen, Wendy L. Thu . "Understanding Small-Molecule Interactions in Metal-Organic Frameworks: Coupling Experiment with Theory". United States. doi:10.1002/adma.201500966. https://www.osti.gov/servlets/purl/1459350.
@article{osti_1459350,
title = {Understanding Small-Molecule Interactions in Metal-Organic Frameworks: Coupling Experiment with Theory},
author = {Lee, Jason S. and Vlaisavljevich, Bess and Britt, David K. and Brown, Craig M. and Haranczyk, Maciej and Neaton, Jeffrey B. and Smit, Berend and Long, Jeffrey R. and Queen, Wendy L.},
abstractNote = {Metal-organic frameworks (MOFs) have gained much attention as next generation porous media for various applications, especially gas separations/storage and catalysis. New MOFs are regularly reported; however, to develop better materials in a timely manner for specific applications, the interactions between guest molecules and the internal surface of the framework must first be understood. In this review, we present a combined experimental and theoretical approach that proves essential for the elucidation of small-molecule interactions in a model MOF system known as M2(dobdc) (dobdc4– = 2,5-dioxido-1,4-benzenedicarboxylate; M = Mg, Mn, Fe, Co, Ni, Cu, or Zn), a material whose adsorption properties can be readily tuned via chemical substitution. Here, we additionally show that the study of extensive families like this one can provide a platform to test the efficacy and accuracy of developing computational methodologies in slightly varying chemical environments, a task that is necessary for their evolution into viable, robust tools for screening large numbers of materials.},
doi = {10.1002/adma.201500966},
journal = {Advanced Materials},
number = 38,
volume = 27,
place = {United States},
year = {2015},
month = {5}
}

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