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Epoxide-functionalization of polyethyleneimine for synthesis of stable carbon dioxide adsorbent in temperature swing adsorption.

ABSTRACT: Amine-containing adsorbents have been extensively investigated for post-combustion carbon dioxide capture due to their ability to chemisorb low-concentration carbon dioxide from a wet flue gas. However, earlier studies have focused primarily on the carbon dioxide uptake of adsorbents, and have not demonstrated effective adsorbent regeneration and long-term stability under such conditions. Here, we report the versatile and scalable synthesis of a functionalized-polyethyleneimine (PEI)/silica adsorbent which simultaneously exhibits a large working capacity (2.2?mmol?g(-1)) and long-term stability in a practical temperature swing adsorption process (regeneration under 100% carbon dioxide at 120?°C), enabling the separation of concentrated carbon dioxide. We demonstrate that the functionalization of PEI with 1,2-epoxybutane reduces the heat of adsorption and facilitates carbon dioxide desorption (>99%) during regeneration compared with unmodified PEI (76%). Moreover, the functionalization significantly improves long-term adsorbent stability over repeated temperature swing adsorption cycles due to the suppression of urea formation and oxidative amine degradation.

SUBMITTER: Choi W

PROVIDER: S-EPMC5013602 | biostudies-literature | 2016 Aug

REPOSITORIES: biostudies-literature

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Epoxide-functionalization of polyethyleneimine for synthesis of stable carbon dioxide adsorbent in temperature swing adsorption.

Choi Woosung W Min Kyungmin K Kim Chaehoon C Ko Young Soo YS Jeon Jae Wan JW Seo Hwimin H Park Yong-Ki YK Choi Minkee M

Nature communications 20160830

Amine-containing adsorbents have been extensively investigated for post-combustion carbon dioxide capture due to their ability to chemisorb low-concentration carbon dioxide from a wet flue gas. However, earlier studies have focused primarily on the carbon dioxide uptake of adsorbents, and have not demonstrated effective adsorbent regeneration and long-term stability under such conditions. Here, we report the versatile and scalable synthesis of a functionalized-polyethyleneimine (PEI)/silica adso ...[more]

PMID: 27572662

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Project description:Solvent-assisted ligand incorporation (SALI) of the ditopic linker 5-carboxy-3-(4-carboxybenzyl)thiazolium bromide [(H2PhTz)Br] into the zirconium metal-organic framework NU-1000 [Zr6O4(OH)8(H2O)4(TBAPy)2, where NU = Northwestern University and H4TBAPy = 1,3,6,8-tetrakis(p-benzoic-acid)pyrene], led to the SALIed NU-1000-PhTz material of minimal formula [Zr6O4(OH)6(H2O)2(TBAPy)2(PhTz)]Br. NU-1000-PhTz has been thoroughly characterized in the solid state. As confirmed by powder X-ray diffraction, this material keeps the same three-dimensional architecture of NU-1000 and the dicarboxylic extra linker bridges adjacent [Zr6] nodes ca. 8 Å far apart along the crystallographic c-axis. The functionalized MOF has a BET specific surface area of 1560 m2/g, and it is featured by a slightly higher thermal stability than its parent material (Tdec = 820 vs. 800 K, respectively). NU-1000-PhTz has been exploited for the capture and separation of two pollutant gases: carbon dioxide (CO2) and nitrous oxide (N2O). The high thermodynamic affinity for both gases [isosteric heat of adsorption (Qst) = 25 and 27 kJ mol-1 for CO2 and N2O, respectively] reasonably stems from the strong interactions between these (polar) "stick-like" molecules and the ionic framework. Intriguingly, NU-1000-PhTz shows an unprecedented temperature-dependent adsorption capacity, loading more N2O in the 298 K ≤ T ≤ 313 K range but more CO2 at temperatures falling out of this range. Grand canonical Monte Carlo simulations of the adsorption isotherms confirmed that the preferential adsorption sites of both gases are the triangular channels (micropores) in close proximity to the polar pillar. While CO2 interacts with the thiazolium ring in an "end-on" fashion through its O atoms, N2O adopts a "side-on" configuration through its three atoms simultaneously. These findings open new horizons in the discovery of functional materials that may discriminate between polluting gases through selective adsorption at different temperatures.

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Epoxide-functionalization of polyethyleneimine for synthesis of stable carbon dioxide adsorbent in temperature swing adsorption.

Publications

Epoxide-functionalization of polyethyleneimine for synthesis of stable carbon dioxide adsorbent in temperature swing adsorption.

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