Molecular blends of methylated-poly(ethylenimine) and amorphous porous organic cages for SO2 adsorption

Guanghui Zhu; Jan Michael Y. Carrillo; Achintya Sujan; Claudia N. Okonkwo; Sangjae Park; Bobby G. Sumpter; Christopher W. Jones; Ryan P. Lively

doi:10.1039/c8ta02788a

Molecular blends of methylated-poly(ethylenimine) and amorphous porous organic cages for SO₂ adsorption

Guanghui Zhu, Jan Michael Y. Carrillo, Achintya Sujan, Claudia N. Okonkwo, Sangjae Park, Bobby G. Sumpter, Christopher W. Jones, Ryan P. Lively

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

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. 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. These composite materials are evaluated as adsorbents for low concentration SO₂ (200 ppm) adsorption and show good thermal and cyclic stability.

Original language	English
Pages (from-to)	22043-22052
Number of pages	10
Journal	Journal of Materials Chemistry A
Volume	6
Issue number	44
DOIs	https://doi.org/10.1039/c8ta02788a
State	Published - 2018

Funding

This work was supported by the Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center funded by U.S. Department of Energy (US DoE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0012577. This work was performed in part at the Georgia Tech Institute for Electronics and Nanotechnology, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (Grant ECCS-1542174). Computational aspects of this work were performed at the Center for Nanophase Materials Sciences (CNMS), which is a US DOE Office of Science User Facility. Some of the research used resources of the Oak Ridge Leadership Computing Facility (OLCF) at the Oak Ridge National Laboratory (ORNL), which is supported by the Office of Science of the U.S. DOE under Contract DE-AC05-00OR22725.

Funders	Funder number
Center for Understanding and Control of Acid
National Science Foundation	ECCS-1542174
U.S. Department of Energy	DE-AC05-00OR22725
Office of Science
Basic Energy Sciences	DE-SC0012577
Oak Ridge National Laboratory

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title = "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. 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. These composite materials are evaluated as adsorbents for low concentration SO2 (200 ppm) adsorption and show good thermal and cyclic stability.",

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AU - Zhu, Guanghui

AU - Carrillo, Jan Michael Y.

AU - Sujan, Achintya

AU - Okonkwo, Claudia N.

AU - Park, Sangjae

AU - Sumpter, Bobby G.

AU - Jones, Christopher W.

AU - Lively, Ryan P.

PY - 2018

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AB - Porous organic cages (POCs) are emerging porous materials that exhibit intriguing properties in the areas of self-assembly, host-guest interaction, and solution processability. 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. These composite materials are evaluated as adsorbents for low concentration SO2 (200 ppm) adsorption and show good thermal and cyclic stability.

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Molecular blends of methylated-poly(ethylenimine) and amorphous porous organic cages for SO₂ adsorption

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