4.8 Article

Nanocage-Based In III{TbIII}2-Organic Framework Featuring Lotus-Shaped Channels for Highly Efficient CO2 Fixation and I2 Capture

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 24, 页码 27803-27811

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c07061

关键词

3p-4f heterometallic cluster; nanocage; iodine sorption; carbon dioxide; epoxide

资金

  1. Natural Science Foundation of China [21101097, 21801230]
  2. Opening Foundation of Key Laboratory of Laser and Infrared System (Shandong University) from Ministry of Education
  3. Project of Central Plains Science and Technology Innovation Leading Talents of Henan Province [204200510001]
  4. North University of China

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The exquisite combination of independent 3p [In(CO2)(4)] units and 4f [Tb-2(CO2)(8)] clusters in the presence of the designed hexatopic 2,4,6-tri(2,4-dicarboxyphenyl)pyridine ligand engenders one peculiar nanocaged In(III){Tb(III)}(2)-organic framework: ({(Me2NH2)[InTb2(HTDP)(2)].3DMF.3H(2)O}(n), designated as NUC-5), which features dual types of lotus-shaped channels along the [100] and [110] axes with related node windows of 5.3 x 6.8 and 12.1 x 9.2 angstrom(2), respectively. To the best of our knowledge, except several coexisted 3p-4f In/Ln dusters of {In(3)Ln}- and {In(3)Ln(2)}-based metal-organic frameworks (MOFs), NUC-5 is one novel type of In/Ln heterometallic framework In addition, its topology was an unprecedented 3D TAYZIC net with a Schlifli symbol of {4.(4)6(2)}{4.(5)6(5)}(2){4.(6)6.(8)8}. Moreover, activated NUC-5 is proved to be one efficient adsorbent for CO2 and one recycled cydoaddition catalyst for the transformation of epoxides into related carbonates with high yields under mild conditions. Furthermore, the excellent reversible sorption performance for I-2 in the volatilization phase or in cyclohexane solution with a maximum adsorption capacity of 609.1 mg/g (3.75 iodine molecules per unit cell) makes NUC-5 a promising adsorbent for radioactive products of I-129 and I-131 in the field of nuclear industry. This study provides one synthetic strategy that the original nature of MOFs could be enhanced by introducing some specific function-prompted inorganic subunits with the aid of predesigned supporting ligands.

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