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

被引:91
作者
Chen, Hongtai [1 ]
Fan, Liming [1 ]
Zhang, Xiutang [1 ]
Ma, Lufang [2 ]
机构
[1] North Univ China, Coll Sci, Dept Chem, Taiyuan 030051, Peoples R China
[2] Luoyang Normal Univ, Coll Chem & Chem Engn, Luoyang 471934, Peoples R China
关键词
3p-4f heterometallic cluster; nanocage; iodine sorption; carbon dioxide; epoxide; METAL-ORGANIC FRAMEWORKS; CONJUGATED MICROPOROUS POLYMERS; REVERSIBLE IODINE CAPTURE; CARBON-DIOXIDE CAPTURE; STRECKER REACTION; VOLATILE IODINE; MOF PLATFORM; ADSORPTION; SEPARATION; CONVERSION;
D O I
10.1021/acsami.0c07061
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
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.
引用
收藏
页码:27803 / 27811
页数:9
相关论文
共 70 条
[31]   Zirconium-Based Metal-Organic Frameworks for the Catalytic Hydrolysis of Organophosphorus Nerve Agents [J].
Kirlikovali, Kent O. ;
Chen, Zhijie ;
Islamoglu, Timur ;
Hupp, Joseph T. ;
Farha, Omar K. .
ACS APPLIED MATERIALS & INTERFACES, 2020, 12 (13) :14702-14720
[32]   Visualization of Iodine Chemisorption Facilitated by Aryl C-H Bond Activation [J].
Lee, Byeongchan ;
Chen, Ying-Pin ;
Park, Jinkyu ;
Park, Jinhee .
ACS APPLIED MATERIALS & INTERFACES, 2019, 11 (29) :25817-25823
[33]   Design of a Multifunctional Indium-Organic Framework: Fluorescent Sensing of Nitro Compounds, Physical Adsorption, and Photocatalytic Degradation of Organic Dyes [J].
Li, Hai-Peng ;
Dou, Zhaodi ;
Chen, Shuang-Qiu ;
Hu, Mancheng ;
Li, Shuni ;
Sun, Hua-Ming ;
Jiang, Yucheng ;
Zhai, Quan-Guo .
INORGANIC CHEMISTRY, 2019, 58 (16) :11220-11230
[34]   A Discrete Tetrahedral Indium Cage as an Efficient Heterogeneous Catalyst for the Fixation of CO2 and the Strecker Reaction of Ketones [J].
Liang, Guang-Ming ;
Xiong, Peng ;
Azam, Khan ;
Ni, Qing-Ling ;
Zeng, Jian-Qiang ;
Gui, Liu-Cheng ;
Wang, Xiu-Jian .
INORGANIC CHEMISTRY, 2020, 59 (03) :1653-1659
[35]   Nitrogen-Rich Conjugated Microporous Polymers: Facile Synthesis, Efficient Gas Storage, and Heterogeneous Catalysis [J].
Liao, Yaozu ;
Cheng, Zhonghua ;
Zuo, Weiwei ;
Thomas, Arne ;
Faul, Charl F. J. .
ACS APPLIED MATERIALS & INTERFACES, 2017, 9 (44) :38390-38400
[36]   Highly Efficient and Reversible Iodine Capture in Hexaphenylbenzene-Based Conjugated Microporous Polymers [J].
Liao, Yaozu ;
Weber, Jens ;
Mills, Benjamin M. ;
Ren, Zihao ;
Faul, Charl F. J. .
MACROMOLECULES, 2016, 49 (17) :6322-6333
[37]   Redox-Responsive Polymeric Nanocomplex for Delivery of Cytotoxic Protein and Chemotherapeutics [J].
Lim, Wei Qi ;
Phua, Soo Zeng Fiona ;
Zhao, Yanli .
ACS APPLIED MATERIALS & INTERFACES, 2019, 11 (35) :31638-31648
[38]   An Elastic Hydrogen-Bonded Cross-Linked. Organic Framework for Effective Iodine Capture in Water [J].
Lin, Yunxiao ;
Jiang, Xuanfeng ;
Kim, Samuel T. ;
Alahakoon, Sampath B. ;
Hou, Xisen ;
Zhang, Zhiyun ;
Thompson, Christina M. ;
Smaldone, Ronald A. ;
Ke, Chenfeng .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (21) :7172-7175
[39]   Trace Carbon Dioxide Capture by Metal-Organic Frameworks [J].
Liu, Jia ;
Wei, Yajuan ;
Zhao, Yanli .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2019, 7 (01) :82-93
[40]   Exceptionally Robust In-Based Metal-Organic Framework for Highly Efficient Carbon Dioxide Capture and Conversion [J].
Liu, Lin ;
Wang, Shi-Ming ;
Han, Zheng-Bo ;
Ding, Meili ;
Yuan, Da-Qiang ;
Jiang, Hai-Long .
INORGANIC CHEMISTRY, 2016, 55 (07) :3558-3565