Hydrogen-Bonded Porous Coordination Polymers:  Structural Transformation, Sorption Properties, and Particle Size from Kinetic Studies

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  • Kazuhiro Uemura
    Contribution from the Environmental Science and Engineering, Graduate School of Science and Engineering, Yamaguchi University, Tokiwadai 2-16-1, Ube-shi, Yamaguchi 755-8611, Japan, Department of Chemistry, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan, and Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishigyo-ku, Kyoto 615-8510, Japan
  • Kazuya Saito
    Contribution from the Environmental Science and Engineering, Graduate School of Science and Engineering, Yamaguchi University, Tokiwadai 2-16-1, Ube-shi, Yamaguchi 755-8611, Japan, Department of Chemistry, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan, and Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishigyo-ku, Kyoto 615-8510, Japan
  • Susumu Kitagawa
    Contribution from the Environmental Science and Engineering, Graduate School of Science and Engineering, Yamaguchi University, Tokiwadai 2-16-1, Ube-shi, Yamaguchi 755-8611, Japan, Department of Chemistry, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan, and Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishigyo-ku, Kyoto 615-8510, Japan
  • Hidetoshi Kita
    Contribution from the Environmental Science and Engineering, Graduate School of Science and Engineering, Yamaguchi University, Tokiwadai 2-16-1, Ube-shi, Yamaguchi 755-8611, Japan, Department of Chemistry, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan, and Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishigyo-ku, Kyoto 615-8510, Japan
  • 20140303

書誌事項

公開日
2006-11-22
DOI
  • 10.1021/ja064152r
公開者
American Chemical Society (ACS)

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説明

Three new coordination polymers, [CoCl2(4-pmna)2]n (1), {[Co(NCS)2(4-pmna)2].2Me2CO}n (2 superset 2Me2CO), and {[Co(4-pmna)2(H2O)2](NO3)2.2CH3OH}n (3 superset 2H2O.2MeOH) (4-pmna = N-(pyridin-4-ylmethyl)nicotinamide), have been synthesized and characterized using single-crystal X-ray diffraction. The cobalt(II) atoms are bridged by 4-pmna ligands in all three compounds to form double-stranded one-dimensional "repeated rhomboid-type" chains with rectangular-shaped cavities. In 1, each chain slips and obstructs the neighboring cavities so that there are no guest-incorporated pores. Both 2 superset 2Me2CO and 3 superset 2H2O.2MeOH do not have such a staggered arrangement and have pores that can be filled with a guest molecule. Compound 3 superset 2H2O.2MeOH traps guest molecules with multiple hydrogen bonds and shows a reversible structural rearrangement during adsorption and desorption. The new crystalline compound, 3, is stabilized by forming hydrogen bonds with the amide moieties of the 4-pmna ligands and was characterized using infrared spectroscopy. The clathration enthalpy of the reaction 3 + 2H2O(l) + 2MeOH(l) <==> 3 superset 2H2O.2MeOH (approximately 35 kJ/mol) was estimated from differential scanning calorimetry data by considering the vaporization enthalpies of H2O and MeOH. The desorption process of 3 superset 2H2O.2MeOH --> 3 follows a single zero-order reaction mechanism under isothermal conditions. The activation energy of ca. 100 kJ/mol was obtained by plotting the logarithm of the reaction time for the same reacted fraction versus the reciprocal of the temperature. Moreover, the distribution of the one-dimensional channels in 3 superset 2H2O.2MeOH was estimated using the observation that the reaction rate is directly proportional to the total sectional area.

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