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Title: Defect-Free MOF-Based Mixed Matrix Membranes Obtained by Corona Crosslinking

Abstract

Functionalized UiO-66 MOF particles were covalently grafted with hydride-terminated polydimethylsiloxane (PDMS) via postsynthetic modification (PSM). These PDMS-coated MOF particles (termed here ‘corona-MOF’) were used in the preparation of mixed- matrix membranes (MMMs). Defect-free MMMs with weight loadings of 50% were achieved with corona-MOF particles, attributed to the improved dispersibility of the corona-MOF particles and covalent linkages between the corona-MOF particles and the polymer matrix. The PDMS MMMs showed distinct separation features in a single-gas permeation test, displaying much higher CO 2 gas permeation with no decrease in selectivity when compared to MMMs prepared with unmodified UiO-66 particles. Single gas separation tests with CO 2, N 2, and propane were performed to probe the separation mechanism of the corona-MOF MMMs, demonstrating that these MMM avoid non-ideal “sieve-in-a-cage” and “plugged sieves” scenarios. Additionally, due to covalent bond formation between both the MOF and the polymer matrix in corona-MOF MMMs, particle aggregation is negligible during film curing, allowing for the formation of flexible, self-standing MMMs of <1 μm in thickness. Low quantities of polymer covalently attached to the MOF surface (<5 wt%) is sufficient to fabricate thin, defect-free, high MOF loading MMMs.

Authors:
 [1];  [2]; ORCiD logo [2]
  1. Univ. of California, San Diego, CA (United States); Asahi Kasei Corp., Shizuoka (Japan)
  2. Univ. of California, San Diego, CA (United States)
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1500171
Grant/Contract Number:  
FG02-08ER46519
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Name: ACS Applied Materials and Interfaces; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Katayama, Yuji, Bentz, Kyle C., and Cohen, Seth M.. Defect-Free MOF-Based Mixed Matrix Membranes Obtained by Corona Crosslinking. United States: N. p., 2019. Web. doi:10.1021/acsami.9b02539.
Katayama, Yuji, Bentz, Kyle C., & Cohen, Seth M.. Defect-Free MOF-Based Mixed Matrix Membranes Obtained by Corona Crosslinking. United States. doi:10.1021/acsami.9b02539.
Katayama, Yuji, Bentz, Kyle C., and Cohen, Seth M.. Mon . "Defect-Free MOF-Based Mixed Matrix Membranes Obtained by Corona Crosslinking". United States. doi:10.1021/acsami.9b02539.
@article{osti_1500171,
title = {Defect-Free MOF-Based Mixed Matrix Membranes Obtained by Corona Crosslinking},
author = {Katayama, Yuji and Bentz, Kyle C. and Cohen, Seth M.},
abstractNote = {Functionalized UiO-66 MOF particles were covalently grafted with hydride-terminated polydimethylsiloxane (PDMS) via postsynthetic modification (PSM). These PDMS-coated MOF particles (termed here ‘corona-MOF’) were used in the preparation of mixed- matrix membranes (MMMs). Defect-free MMMs with weight loadings of 50% were achieved with corona-MOF particles, attributed to the improved dispersibility of the corona-MOF particles and covalent linkages between the corona-MOF particles and the polymer matrix. The PDMS MMMs showed distinct separation features in a single-gas permeation test, displaying much higher CO2 gas permeation with no decrease in selectivity when compared to MMMs prepared with unmodified UiO-66 particles. Single gas separation tests with CO2, N2, and propane were performed to probe the separation mechanism of the corona-MOF MMMs, demonstrating that these MMM avoid non-ideal “sieve-in-a-cage” and “plugged sieves” scenarios. Additionally, due to covalent bond formation between both the MOF and the polymer matrix in corona-MOF MMMs, particle aggregation is negligible during film curing, allowing for the formation of flexible, self-standing MMMs of <1 μm in thickness. Low quantities of polymer covalently attached to the MOF surface (<5 wt%) is sufficient to fabricate thin, defect-free, high MOF loading MMMs.},
doi = {10.1021/acsami.9b02539},
journal = {ACS Applied Materials and Interfaces},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {3}
}

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This content will become publicly available on March 11, 2020
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