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Title: DMOF-1 as a Representative MOF for SO2 Adsorption in Both Humid and Dry Conditions

Abstract

The mixed-ligand metal–organic framework (MOF) DMOF-1 has been successfully synthesized via ligand: 2,3,5,6-tetramethylterephthalic acid (TM), 9,10-anthracenedicarboxylic acid (ADC), 1,4-naphthalenedicarboxylic acid (NDC), 2,5-dimethyl terephthalic acid (DM), and metal (Zn, Cu, Ni, Co) substitutions to develop structure–property relationships for adsorption of water and SO2, an acid gas commonly found in flue gas streams at ppm-level concentrations. The substitution of bulky ligands, TM and ADC, resulted in not only improved water stability but also stability toward dry SO2, whereas substitution with NDC and DM did not provide water or SO2 stability. ADC-functionalized Zn–DMOF exhibited the greatest stability under humid SO2 exposure of the ligand-functionalized materials that were tested. Metal substitution of Cu into the DMOF–TM structure resulted in the greatest stability of the M–DMOF–TM samples upon exposure to humid SO2, and Ni–DMOF–TM provided the second most stable material. Finally, these results follow the prediction of the Irving–Williams series of metal node/ligand bond strengths.

Authors:
 [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Research Org.:
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)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566518
Grant/Contract Number:  
SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 41; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); defects; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Hungerford, Julian, Bhattacharyya, Souryadeep, Tumuluri, Uma, Nair, Sankar, Wu, Zili, and Walton, Krista S. DMOF-1 as a Representative MOF for SO2 Adsorption in Both Humid and Dry Conditions. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b06819.
Hungerford, Julian, Bhattacharyya, Souryadeep, Tumuluri, Uma, Nair, Sankar, Wu, Zili, & Walton, Krista S. DMOF-1 as a Representative MOF for SO2 Adsorption in Both Humid and Dry Conditions. United States. https://doi.org/10.1021/acs.jpcc.8b06819
Hungerford, Julian, Bhattacharyya, Souryadeep, Tumuluri, Uma, Nair, Sankar, Wu, Zili, and Walton, Krista S. Fri . "DMOF-1 as a Representative MOF for SO2 Adsorption in Both Humid and Dry Conditions". United States. https://doi.org/10.1021/acs.jpcc.8b06819. https://www.osti.gov/servlets/purl/1566518.
@article{osti_1566518,
title = {DMOF-1 as a Representative MOF for SO2 Adsorption in Both Humid and Dry Conditions},
author = {Hungerford, Julian and Bhattacharyya, Souryadeep and Tumuluri, Uma and Nair, Sankar and Wu, Zili and Walton, Krista S.},
abstractNote = {The mixed-ligand metal–organic framework (MOF) DMOF-1 has been successfully synthesized via ligand: 2,3,5,6-tetramethylterephthalic acid (TM), 9,10-anthracenedicarboxylic acid (ADC), 1,4-naphthalenedicarboxylic acid (NDC), 2,5-dimethyl terephthalic acid (DM), and metal (Zn, Cu, Ni, Co) substitutions to develop structure–property relationships for adsorption of water and SO2, an acid gas commonly found in flue gas streams at ppm-level concentrations. The substitution of bulky ligands, TM and ADC, resulted in not only improved water stability but also stability toward dry SO2, whereas substitution with NDC and DM did not provide water or SO2 stability. ADC-functionalized Zn–DMOF exhibited the greatest stability under humid SO2 exposure of the ligand-functionalized materials that were tested. Metal substitution of Cu into the DMOF–TM structure resulted in the greatest stability of the M–DMOF–TM samples upon exposure to humid SO2, and Ni–DMOF–TM provided the second most stable material. Finally, these results follow the prediction of the Irving–Williams series of metal node/ligand bond strengths.},
doi = {10.1021/acs.jpcc.8b06819},
journal = {Journal of Physical Chemistry. C},
number = 41,
volume = 122,
place = {United States},
year = {Fri Sep 21 00:00:00 EDT 2018},
month = {Fri Sep 21 00:00:00 EDT 2018}
}

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