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Linking CO<sub>2</sub> Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering [electronic resource].

Published
Washington, D.C. : United States. Dept. of Energy. Office of Basic Energy Sciences, 2015.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description
pages 11,749-11,759 : digital, PDF file
Additional Creators
United States. Department of Energy. Office of Basic Energy. Energy Frontier Research Centers (EFRC), United States. Department of Energy. Office of Basic Energy Sciences, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary
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.
Report Numbers
E 1.99:1386055
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Note
Published through SciTech Connect.
08/26/2015.
Journal of the American Chemical Society 137 36 ISSN 0002-7863 AM
Adam Holewinski; Miles A. Sakwa-Novak; Christopher W. Jones.
Funding Information
SC0012577
View MARC record | catkey: 24046977