Linking CO 2 Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering

Holewinski, Adam; Sakwa-Novak, Miles A.; Jones, Christopher W.

doi:10.1021/jacs.5b06823

Title: Linking CO ₂ Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering

Journal Article · Wed Sep 02 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b06823· OSTI ID:1213924

Holewinski, Adam ^[1]; Sakwa-Novak, Miles A. ^[1]; Jones, Christopher W. ^[1]

School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, Georgia 30332, United States

Composites of poly(ethylenimine) (PEI) and mesoporous silica are effective, reversible adsorbents for CO₂, both from flue gas and in direct air-capture applications. The morphology of the PEI within the silica can strongly impact the overall carbon capture efficiency and rate of saturation. Here, we directly probe the spatial distribution of the supported polymer through small-angle neutron scattering (SANS). Combined with textural characterization from physisorption analysis, the data indicate that PEI first forms a thin conformal coating on the pore walls, but all additional polymer aggregates into plug(s) that grow along the pore axis. This model is consistent with observed trends in amine-efficiency (CO₂/N binding ratio) and pore size distributions, and points to a trade-off between achieving high chemical accessibility of the amine binding sites, which are inaccessible when they strongly interact with the silica, and high accessibility for mass transport, which can be hampered by diffusion through PEI plugs. In conclusion, we illustrate this design principle by demonstrating higher CO₂ capacity and uptake rate for PEI supported in a hydrophobically modified silica, which exhibits repulsive interactions with the PEI, freeing up binding sites.

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Research Organization:: Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012577

OSTI ID:: 1213924

Alternate ID(s):: OSTI ID: 1386055

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Vol. 137 Journal Issue: 36; ISSN 0002-7863

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 108 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (heterogeneous)
defects
membrane
carbon capture
materials and chemistry by design
synthesis (novel materials)
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Title: Linking CO 2 Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering

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Title: Linking CO ₂ Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering