Molecular Blends of Methylated-Poly(ethylenimine) and Amorphous Porous Organic Cages for SO2 Adsorption
Abstract
Porous organic cages (POCs) are emerging porous materials that exhibit intriguing properties in the areas of self-assembly, host-guest interaction, and solution processability. Here in this work, we explore the applicability of POCs as molecular porous supports for polymeric amines. We find that primary amines in poly(ethylenimine) (PEI) can undergo metathesis with the imine bonds present in POCs, resulting in non-porous products. This problem can be overcome by transforming the primary amines in PEI to tertiary amines via methylation. The methylated PEI (mPEI) forms homogeneous composites with amorphous scrambled porous organic cages (ASPOCs) without undesired reactions or phase separation. The microscopic structure of the composites is studied using molecular dynamics simulations. Finally, these composite materials are evaluated as adsorbents for low concentration SO2 (200 ppm) adsorption and show good thermal and cyclic stability.
- Authors:
-
[2];
[2];
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Sciences and Engineering Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); 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)
- OSTI Identifier:
- 1439925
- Alternate Identifier(s):
- OSTI ID: 1441050
- Grant/Contract Number:
- AC05-00OR22725; SC0012577; ECCS-1542174
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 44; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhu, Guanghui, Carrillo, Jan-Michael Y., Sujan, Achintya, N. Okonkwo, Claudia, Park, Sangjae, Sumpter, Bobby G., Jones, Christopher W., and Lively, Ryan. Molecular Blends of Methylated-Poly(ethylenimine) and Amorphous Porous Organic Cages for SO2 Adsorption. United States: N. p., 2018.
Web. doi:10.1039/c8ta02788a.
Zhu, Guanghui, Carrillo, Jan-Michael Y., Sujan, Achintya, N. Okonkwo, Claudia, Park, Sangjae, Sumpter, Bobby G., Jones, Christopher W., & Lively, Ryan. Molecular Blends of Methylated-Poly(ethylenimine) and Amorphous Porous Organic Cages for SO2 Adsorption. United States. https://doi.org/10.1039/c8ta02788a
Zhu, Guanghui, Carrillo, Jan-Michael Y., Sujan, Achintya, N. Okonkwo, Claudia, Park, Sangjae, Sumpter, Bobby G., Jones, Christopher W., and Lively, Ryan. Wed .
"Molecular Blends of Methylated-Poly(ethylenimine) and Amorphous Porous Organic Cages for SO2 Adsorption". United States. https://doi.org/10.1039/c8ta02788a. https://www.osti.gov/servlets/purl/1439925.
@article{osti_1439925,
title = {Molecular Blends of Methylated-Poly(ethylenimine) and Amorphous Porous Organic Cages for SO2 Adsorption},
author = {Zhu, Guanghui and Carrillo, Jan-Michael Y. and Sujan, Achintya and N. Okonkwo, Claudia and Park, Sangjae and Sumpter, Bobby G. and Jones, Christopher W. and Lively, Ryan},
abstractNote = {Porous organic cages (POCs) are emerging porous materials that exhibit intriguing properties in the areas of self-assembly, host-guest interaction, and solution processability. Here in this work, we explore the applicability of POCs as molecular porous supports for polymeric amines. We find that primary amines in poly(ethylenimine) (PEI) can undergo metathesis with the imine bonds present in POCs, resulting in non-porous products. This problem can be overcome by transforming the primary amines in PEI to tertiary amines via methylation. The methylated PEI (mPEI) forms homogeneous composites with amorphous scrambled porous organic cages (ASPOCs) without undesired reactions or phase separation. The microscopic structure of the composites is studied using molecular dynamics simulations. Finally, these composite materials are evaluated as adsorbents for low concentration SO2 (200 ppm) adsorption and show good thermal and cyclic stability.},
doi = {10.1039/c8ta02788a},
journal = {Journal of Materials Chemistry. A},
number = 44,
volume = 6,
place = {United States},
year = {Wed May 30 00:00:00 EDT 2018},
month = {Wed May 30 00:00:00 EDT 2018}
}
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Cited by: 18 works
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Figures / Tables:
Scheme 1: Synthesis of ASPOC CC1234 from 4 equivalents of triformylbenzene, 2 equivalents of ethylenediamine and 4 equivalents of (1R,2R)-1,2-cyclohexanediamine; which results in the formation of a mixture of cages.
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Works referencing / citing this record:
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.