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Title: Diamine-Appended Mg 2 (dobpdc) Nanorods as Phase-Change Fillers in Mixed-Matrix Membranes for Efficient CO 2/N 2 Separations

Abstract

Despite the availability of chemistries to tailor the pore architectures of microporous polymer membranes for chemical separations, trade-offs in permeability and selectivity with functional group manipulations nevertheless persist, which ultimately places an upper bound on membrane performance. We introduce a new design strategy to uncouple these attributes of the membrane. Key to our success is the incorporation of phase-change metal-organic frameworks (MOFs) into the polymer matrix, which can be used to increase the solubility of a specific gas in the membrane, and thereby its permeability. We further show that it is necessary to scale the size of the phase-change MOF to nanoscopic dimensions, in order to take advantage of this effect in a gas separation. Our observation of an increase in solubility and permeability of only one of the gases during steady-state permeability measurements suggests fast exchange between free and chemisorbed gas molecules within the MOF pores. While the kinetics of this exchange in phase-change MOFs are not yet fully understood, their role in enhancing the efficacy and efficiency of the separation is clearly a compelling new direction for membrane technology.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  4. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1454495
Grant/Contract Number:  
AC02-05CH11231; SC0001015
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 11; Related Information: © 2017 American Chemical Society.; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2/N2 separations; gas separations; mixed-matrix membranes; MOF nanocrystals; phase-change MOFs

Citation Formats

Maserati, Lorenzo, Meckler, Stephen M., Bachman, Jonathan E., Long, Jeffrey R., and Helms, Brett A. Diamine-Appended Mg2 (dobpdc) Nanorods as Phase-Change Fillers in Mixed-Matrix Membranes for Efficient CO2/N2 Separations. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b03106.
Maserati, Lorenzo, Meckler, Stephen M., Bachman, Jonathan E., Long, Jeffrey R., & Helms, Brett A. Diamine-Appended Mg2 (dobpdc) Nanorods as Phase-Change Fillers in Mixed-Matrix Membranes for Efficient CO2/N2 Separations. United States. https://doi.org/10.1021/acs.nanolett.7b03106
Maserati, Lorenzo, Meckler, Stephen M., Bachman, Jonathan E., Long, Jeffrey R., and Helms, Brett A. Wed . "Diamine-Appended Mg2 (dobpdc) Nanorods as Phase-Change Fillers in Mixed-Matrix Membranes for Efficient CO2/N2 Separations". United States. https://doi.org/10.1021/acs.nanolett.7b03106. https://www.osti.gov/servlets/purl/1454495.
@article{osti_1454495,
title = {Diamine-Appended Mg2 (dobpdc) Nanorods as Phase-Change Fillers in Mixed-Matrix Membranes for Efficient CO2/N2 Separations},
author = {Maserati, Lorenzo and Meckler, Stephen M. and Bachman, Jonathan E. and Long, Jeffrey R. and Helms, Brett A.},
abstractNote = {Despite the availability of chemistries to tailor the pore architectures of microporous polymer membranes for chemical separations, trade-offs in permeability and selectivity with functional group manipulations nevertheless persist, which ultimately places an upper bound on membrane performance. We introduce a new design strategy to uncouple these attributes of the membrane. Key to our success is the incorporation of phase-change metal-organic frameworks (MOFs) into the polymer matrix, which can be used to increase the solubility of a specific gas in the membrane, and thereby its permeability. We further show that it is necessary to scale the size of the phase-change MOF to nanoscopic dimensions, in order to take advantage of this effect in a gas separation. Our observation of an increase in solubility and permeability of only one of the gases during steady-state permeability measurements suggests fast exchange between free and chemisorbed gas molecules within the MOF pores. While the kinetics of this exchange in phase-change MOFs are not yet fully understood, their role in enhancing the efficacy and efficiency of the separation is clearly a compelling new direction for membrane technology.},
doi = {10.1021/acs.nanolett.7b03106},
url = {https://www.osti.gov/biblio/1454495}, journal = {Nano Letters},
issn = {1530-6984},
number = 11,
volume = 17,
place = {United States},
year = {2017},
month = {10}
}

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Works referencing / citing this record:

Enhancement of CO 2 binding and mechanical properties upon diamine functionalization of M 2 (dobpdc) metal–organic frameworks
journal, January 2018


Advanced Porous Materials in Mixed Matrix Membranes
journal, July 2018


Advanced Porous Materials in Mixed Matrix Membranes
journal, July 2018


Enhancement of CO 2 binding and mechanical properties upon diamine functionalization of M 2 (dobpdc) metal–organic frameworks
journal, January 2018