TY - JOUR
T1 - A CO2-selective molecular gate of poly(amidoamine) dendrimer immobilized in a poly(ethylene glycol) network
AU - Taniguchi, Ikuo
AU - Urai, Hiromi
AU - Kai, Teruhiko
AU - Duan, Shuhong
AU - Kazama, Shingo
N1 - Funding Information:
This work was financially supported by the Japanese Ministry of Economy, Trade and Industry . The authors acknowledge Mr. Kazuto Hoshino and Ms. Yayoi Taniguchi (Rigaku) for the skillful technique on SAXS measurements and helpful discussions.
PY - 2013/10/1
Y1 - 2013/10/1
N2 - A polymeric membrane composed of poly(amidoamine) (PAMAM) dendrimer immobilized in a poly(ethylene glycol) (PEG) network expresses excellent CO2 separation properties over smaller H2. The preferential CO2 permeation can be explained by specific interaction between CO2 and primary amine of the dendrimer, which enhances CO2 solubility into the polymeric membrane. CO2 forms carbamate with the amines or bicarbonate in the presence of water determined by inverse-gate decoupled 13C NMR. The resulting carbamate ion pair works to form a quasi-crosslinking, which would suppress H2 permeation by a CO2-selective Molecular Gate, while bicarbonate ion can be a major moving species to pass through the polymeric membrane. Attenuated total reflection (ATR) indicates the formation of carbamate. Small-angle X-ray scattering (SAXS) reveals increase in scattering intensity under CO2 atmosphere due to the formation of scattering particles, which can be a cluster of the dendrimer-CO2 crosslinks. Tensile testing of the membrane exhibits increase in both Young's modulus and elongation-to-break by CO2 treatment, suggesting that the crosslinking is reversible and rearrangeable. Differential scanning calorimetry (DSC) also shows an exothermic peak at 120°C, which is associated with dissociation of the crosslinks.
AB - A polymeric membrane composed of poly(amidoamine) (PAMAM) dendrimer immobilized in a poly(ethylene glycol) (PEG) network expresses excellent CO2 separation properties over smaller H2. The preferential CO2 permeation can be explained by specific interaction between CO2 and primary amine of the dendrimer, which enhances CO2 solubility into the polymeric membrane. CO2 forms carbamate with the amines or bicarbonate in the presence of water determined by inverse-gate decoupled 13C NMR. The resulting carbamate ion pair works to form a quasi-crosslinking, which would suppress H2 permeation by a CO2-selective Molecular Gate, while bicarbonate ion can be a major moving species to pass through the polymeric membrane. Attenuated total reflection (ATR) indicates the formation of carbamate. Small-angle X-ray scattering (SAXS) reveals increase in scattering intensity under CO2 atmosphere due to the formation of scattering particles, which can be a cluster of the dendrimer-CO2 crosslinks. Tensile testing of the membrane exhibits increase in both Young's modulus and elongation-to-break by CO2 treatment, suggesting that the crosslinking is reversible and rearrangeable. Differential scanning calorimetry (DSC) also shows an exothermic peak at 120°C, which is associated with dissociation of the crosslinks.
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U2 - 10.1016/j.memsci.2013.05.017
DO - 10.1016/j.memsci.2013.05.017
M3 - Article
AN - SCOPUS:84878830450
SN - 0376-7388
VL - 444
SP - 96
EP - 100
JO - Journal of Membrane Science
JF - Journal of Membrane Science
ER -