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Title: Interactions on External MOF Surfaces: Desorption of Water and Ethanol from CuBDC Nanosheets

Abstract

The external surfaces of metal-organic framework (MOF) materials are difficult to experimentally isolate due to the high porosities of these materials. MOF surface surrogates in the form of copper benzenedicarboxylate (CuBDC) nanosheets were synthesized using a bottomup approach and the surface interactions of water and ethanol were investigated by temperature programmed desorption (TPD). A method of analysis of diffusion-influenced TPD was developed to measure the desorption properties of these porous materials. This approach also allows the extraction of diffusion coefficients from TPD data. The transmission Fourier transform infrared spectra, powder X-ray diffraction patterns and TPD data indicate that water desorbs from CuBDC nanosheets with activation energies of 44±2 kJ/mol at edge sites and 58 ± 1 kJ/mol at external surface and internal and pore sites. Ethanol desorbs with activation energies of 58 ± 1 kJ/mol at internal pore sites and 66 ± 0.4 kJ/mol at external surface sites. Co-adsorption of water and ethanol was also investigated. The presence of ethanol was found to inhibit the desorption of water that results in a water desorption process with an activation energy of 68 ± 0.7 kJ/mol.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
  2. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
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)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1469893
Grant/Contract Number:  
[SC0012577]
Resource Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
[ Journal Volume: 33; Journal Issue: 39; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis]; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; catalysis (heterogeneous); defects; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Elder, Alexander C., Aleksandrov, Alexandr B., Nair, Sankar, and Orlando, Thomas M. Interactions on External MOF Surfaces: Desorption of Water and Ethanol from CuBDC Nanosheets. United States: N. p., 2017. Web. doi:10.1021/acs.langmuir.7b01987.
Elder, Alexander C., Aleksandrov, Alexandr B., Nair, Sankar, & Orlando, Thomas M. Interactions on External MOF Surfaces: Desorption of Water and Ethanol from CuBDC Nanosheets. United States. doi:10.1021/acs.langmuir.7b01987.
Elder, Alexander C., Aleksandrov, Alexandr B., Nair, Sankar, and Orlando, Thomas M. Wed . "Interactions on External MOF Surfaces: Desorption of Water and Ethanol from CuBDC Nanosheets". United States. doi:10.1021/acs.langmuir.7b01987. https://www.osti.gov/servlets/purl/1469893.
@article{osti_1469893,
title = {Interactions on External MOF Surfaces: Desorption of Water and Ethanol from CuBDC Nanosheets},
author = {Elder, Alexander C. and Aleksandrov, Alexandr B. and Nair, Sankar and Orlando, Thomas M.},
abstractNote = {The external surfaces of metal-organic framework (MOF) materials are difficult to experimentally isolate due to the high porosities of these materials. MOF surface surrogates in the form of copper benzenedicarboxylate (CuBDC) nanosheets were synthesized using a bottomup approach and the surface interactions of water and ethanol were investigated by temperature programmed desorption (TPD). A method of analysis of diffusion-influenced TPD was developed to measure the desorption properties of these porous materials. This approach also allows the extraction of diffusion coefficients from TPD data. The transmission Fourier transform infrared spectra, powder X-ray diffraction patterns and TPD data indicate that water desorbs from CuBDC nanosheets with activation energies of 44±2 kJ/mol at edge sites and 58 ± 1 kJ/mol at external surface and internal and pore sites. Ethanol desorbs with activation energies of 58 ± 1 kJ/mol at internal pore sites and 66 ± 0.4 kJ/mol at external surface sites. Co-adsorption of water and ethanol was also investigated. The presence of ethanol was found to inhibit the desorption of water that results in a water desorption process with an activation energy of 68 ± 0.7 kJ/mol.},
doi = {10.1021/acs.langmuir.7b01987},
journal = {Langmuir},
number = [39],
volume = [33],
place = {United States},
year = {2017},
month = {9}
}

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