期刊
ACS APPLIED MATERIALS & INTERFACES
卷 6, 期 10, 页码 7325-7333出版社
AMER CHEMICAL SOC
DOI: 10.1021/am500728q
关键词
Friedel-Crafts catalysis; microporous organic polymers; gas uptake; selectivity; carbon storage
资金
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education, Science and Technology [2011-0011222]
- KISTI [KSC-2012-C3-059]
- National Research Foundation of Korea [2010-0020414, 2011-0011222] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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 m(2) g(-1), a narrow pore size distribution in the range from 6 to 8 angstrom, 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 CO2 adsorption over N-2 (100) and CH4 (15) at 273 K were obtained. More importantly, as compared with any other porous materials, much higher selectivity for CO2/N-2 (80) and CO2/CH4 (15) was observed at 298 K, showing that these selectivity ratios remain high at elevated temperature. The very high CO2/N-2 selectivity values are ascribed to the binding affinity of abundantly available electron-rich basic heteroatoms, high CO2 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.
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