title: Hydration structure of CO2-absorbed 2-aminoethanol studied by neutron diffraction with the 14N/15N isotopic substitution method.
abstract: Neutron diffraction measurements were carried out for CO2-absorbed aqueous 11 mol % 2-aminoethanol (MEA) D2O solutions (corresponding to 30 wt % MEA solution) in order to obtain information on both the intramolecular structure and intermolecular hydration structure of the MEA carbamate molecule in the aqueous solution. Neutron scattering cross sections observed for (MEA)0.11(D2O)0.89, (MEA)0.11(D2O)0.89(CO2)0.06, and (MEA)0.11(D2O)0.89(DCl)0.11 solutions with different (14)N/(15)N ratios were used to derive the first-order difference function, ΔN(Q), which involves environmental structural information around the nitrogen atom of the MEA molecule. Intramolecular geometry and intermolecular hydration structure of MEA, protonated MEA (MEAD(+)), and MEA carbamate (MEA-CO2) molecules were obtained through the least-squares fitting of the observed Δ(N)(Q) in the high-Q region and the intermolecular difference function, Δ(N)(inter)(Q), respectively. In the aqueous solution, the MEA molecule takes the gauche conformation (dihedral angle, ∠NCCO = 45 ± 3°), suggesting that an intramolecular hydrogen bond is formed. On the other hand, values of the dihedral angle ∠NCCO determined for MEAD(+) and MEA-CO2 molecules were 193 ± 4° and 214 ± 8°, respectively. These results imply that the intermolecular hydrogen bonds are dominated for MEAD(+) and MEA-CO2 molecules. The intermolecular nearest neighbor N···O(D2O) distance for the MEA molecule was determined to be 3.13 ± 0.01 Å, which suggests weak intermolecular interaction between the amino-nitrogen atom of MEA and water molecules in the first hydration shell. The nearest-neighbor N···O(D2O) distances for MEAD(+) and MEA-CO2 molecules, 2.79 ± 0.03 and 2.87 ± 0.04 Å, clearly indicate strong hydrogen bonds are formed among the amino group of these molecules and neighboring water molecules.
authors.affiliation: Department of Material and Biological Chemistry, Faculty of Science, Yamagata University , 1-4-12 Kojirakawa-machi, Yamagata 990-8560, Japan.
authors.forename: Yasuo
authors.initials: Y
authors.lastname: Kameda
authors.forename: Hiroshi
authors.initials: H
authors.lastname: Deguchi
authors.forename: Hirotoshi
authors.initials: H
authors.lastname: Furukawa
authors.forename: Yoshiyuki
authors.initials: Y
authors.lastname: Kubota
authors.forename: Yasuyuki
authors.initials: Y
authors.lastname: Yagi
authors.forename: Yoshihiro
authors.initials: Y
authors.lastname: Imai
authors.forename: Noriko
authors.initials: N
authors.lastname: Yamazaki
authors.forename: Noriko
authors.initials: N
authors.lastname: Watari
authors.forename: Takuya
authors.initials: T
authors.lastname: Hirata
authors.forename: Nobuyuki
authors.initials: N
authors.lastname: Matubayasi