skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Linking Silica Support Morphology to the Dynamics of Aminopolymers in Composites

Abstract

A combined computational and experimental approach is used to elucidate the effect of silica support morphology on polymer dynamics and CO 2 adsorption capacities in aminopolymer/silica composites. Furthermore, simulations are based on coarse-grained molecular dynamics simulations of aminopolymer composites where a branched aminopolymer, representing poly(ethylenimine) (PEI), is impregnated into different silica mesoporous supports. The morphology of the mesoporous supports varies from hexagonally packed cylindrical pores representing SBA-15, double gyroids representing KIT-6 and MCM-48, and cagelike structures representing SBA-16. In parallel, composites of PEI and the silica supports SBA-15, KIT-6, MCM-48, and SBA-16 are synthesized and characterized, including measuring their CO 2 uptake. Simulations predict that a 3D pore morphology, such as those of KIT-6, MCM-48, and SBA-16, will have faster segmental mobility and have lower probability of primary amine and surface silanol associations, which should translate to higher CO 2 uptake in comparison to a 2D pore morphology such as that of SBA-15. We found that KIT-6 has higher CO 2 uptake than SBA-15 at equivalent PEI loading, even though both supports have similar surface area and pore volume. But, this is not the case for the MCM-48 support, which has smaller pores, and SBA-16, whose pore structure rapidly degradesmore » after PEI impregnation.« less

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1376602
Grant/Contract Number:
AC05-00OR22725; SC0012577
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 33; Journal Issue: 22; 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

Citation Formats

Carrillo, Jan-Michael Y., Potter, Matthew E., Sakwa-Novak, Miles A., Pang, Simon H., Jones, Christopher W., and Sumpter, Bobby G. Linking Silica Support Morphology to the Dynamics of Aminopolymers in Composites. United States: N. p., 2017. Web. doi:10.1021/acs.langmuir.7b00283.
Carrillo, Jan-Michael Y., Potter, Matthew E., Sakwa-Novak, Miles A., Pang, Simon H., Jones, Christopher W., & Sumpter, Bobby G. Linking Silica Support Morphology to the Dynamics of Aminopolymers in Composites. United States. doi:10.1021/acs.langmuir.7b00283.
Carrillo, Jan-Michael Y., Potter, Matthew E., Sakwa-Novak, Miles A., Pang, Simon H., Jones, Christopher W., and Sumpter, Bobby G. 2017. "Linking Silica Support Morphology to the Dynamics of Aminopolymers in Composites". United States. doi:10.1021/acs.langmuir.7b00283.
@article{osti_1376602,
title = {Linking Silica Support Morphology to the Dynamics of Aminopolymers in Composites},
author = {Carrillo, Jan-Michael Y. and Potter, Matthew E. and Sakwa-Novak, Miles A. and Pang, Simon H. and Jones, Christopher W. and Sumpter, Bobby G.},
abstractNote = {A combined computational and experimental approach is used to elucidate the effect of silica support morphology on polymer dynamics and CO2 adsorption capacities in aminopolymer/silica composites. Furthermore, simulations are based on coarse-grained molecular dynamics simulations of aminopolymer composites where a branched aminopolymer, representing poly(ethylenimine) (PEI), is impregnated into different silica mesoporous supports. The morphology of the mesoporous supports varies from hexagonally packed cylindrical pores representing SBA-15, double gyroids representing KIT-6 and MCM-48, and cagelike structures representing SBA-16. In parallel, composites of PEI and the silica supports SBA-15, KIT-6, MCM-48, and SBA-16 are synthesized and characterized, including measuring their CO2 uptake. Simulations predict that a 3D pore morphology, such as those of KIT-6, MCM-48, and SBA-16, will have faster segmental mobility and have lower probability of primary amine and surface silanol associations, which should translate to higher CO2 uptake in comparison to a 2D pore morphology such as that of SBA-15. We found that KIT-6 has higher CO2 uptake than SBA-15 at equivalent PEI loading, even though both supports have similar surface area and pore volume. But, this is not the case for the MCM-48 support, which has smaller pores, and SBA-16, whose pore structure rapidly degrades after PEI impregnation.},
doi = {10.1021/acs.langmuir.7b00283},
journal = {Langmuir},
number = 22,
volume = 33,
place = {United States},
year = 2017,
month = 5
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 11, 2018
Publisher's Version of Record

Save / Share: