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Kim, Kwang S.
Center for Superfunctional Materials (CSM)
Research Interests
  • Theoretical/experimental nanosciences, molecular electronics spectroscopy, energy materials

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Highly Stable CO2/N-2 and CO2/CH4 Selectivity in Hyper-Cross-Linked Heterocyclic Porous Polymers

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Title
Highly Stable CO2/N-2 and CO2/CH4 Selectivity in Hyper-Cross-Linked Heterocyclic Porous Polymers
Author
Saleh, MuhammadLee, Han MyoungKemp, K. ChristianKim, Kwang S.
Keywords
carbon storage; Friedel-Crafts catalysis; gas uptake; microporous organic polymers; selectivity
Issue Date
201405
Publisher
AMER CHEMICAL SOC
Citation
ACS APPLIED MATERIALS & INTERFACES, v.6, no.10, pp.7325 - 7333
Abstract
The largest obstacles for landfill/flue gas separation using microporous materials are small adsorption values and low selectivity ratios. This study demonstrates that these adsorption and selectivity challenges can be overcome by utilizing a series of hyper-cross-linked heterocyclic polymer networks. These microporous organic polymers (MOPs) were synthesized in a single step by inexpensive Friedel-Crafts-catalyzed reactions using dimethoxymethane as an external linker. The amorphous networks show moderate Brunauer-Emmett-Teller surface areas up to 1022 m2 g-1, a narrow pore size distribution in the range from 6 to 8 Å, and high physicochemical stability. Owing to the presence of the heteroatomic pore surfaces in the networks, they exhibit maximum storage capacities for CO2 of 11.4 wt % at 273 K and 1 atm. Additionally, remarkable selectivity ratios for CO 2 adsorption over N2 (100) and CH4 (15) at 273 K were obtained. More importantly, as compared with any other porous materials, much higher selectivity for CO2/N2 (80) and CO 2/CH4 (15) was observed at 298 K, showing that these selectivity ratios remain high at elevated temperature. The very high CO 2/N2 selectivity values are ascribed to the binding affinity of abundantly available electron-rich basic heteroatoms, high CO 2 isoteric heats of adsorption (49-38 kJ mol-1), and the predominantly microporous nature of the MOPs. Binding energies calculated using the high level of ab initio theory showed that the selectivity is indeed attributed to the heteroatom-CO2 interactions. By employing an easy and economical synthesis procedure these MOPs with high thermochemical stability are believed to be a promising candidate for selective CO2 capture.
URI
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DOI
http://dx.doi.org/10.1021/am500728q
ISSN
1944-8244
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