A Flexible Photoactive Titanium Metal-Organic Framework Based on a [Ti3IV(μ3-O)(O)2(COO)6] Cluster

被引：95
|
作者：
Bueken, Bart [1 ]
Vermoortele, Frederik [1 ]
Vanpoucke, Danny E. P. [2 ]
Reinsch, Helge [1 ]
Tsou, Chih-Chin [3 ]
Valvekens, Pieterjan [1 ]
De Baerdemaeker, Trees [1 ]
Ameloot, Rob [1 ]
Kirschhock, Christine E. A. [1 ]
Van Speybroeck, Veronique [2 ]
Mayer, James M. [3 ]
De Vos, Dirk [1 ]
机构：
[1] Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, B-3001 Louvain, Belgium
[2] Univ Ghent, Ctr Mol Modeling, B-9052 Zwijnaarde, Belgium
[3] Yale Univ, Dept Chem, New Haven, CT 06511 USA
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2015年 / 54卷 / 47期
基金：
美国国家科学基金会;
关键词：
metallocenes; metal-organic frameworks; molecular modeling; photochemistry; titanium; EXTENDING HIRSHFELD-I; UNEXPECTED FORMATION; SORPTION PROPERTIES; OXO CLUSTERS; HYDROLYSIS; TRINUCLEAR; COMPLEXES; CHEMISTRY; CATALYSTS; TOPOLOGY;
D O I：
10.1002/anie.201505512
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
The synthesis of titanium-carboxylate metal-organic frameworks (MOFs) is hampered by the high reactivity of the commonly employed alkoxide precursors. Herein, we present an innovative approach to titanium-based MOFs by the use of titanocene dichloride to synthesize COK-69, the first breathing Ti MOF, which is built up from trans-1,4-cyclo-hexanedicarboxylate linkers and an unprecedented [Ti-3(IV)(mu(3)-O)(O)(2)(COO)(6)] cluster. The photoactive properties of COK-69 were investigated in depth by proton-coupled electron-transfer experiments, which revealed that up to one Ti-IV center per cluster can be photoreduced to Ti-III while preserving the structural integrity of the framework. The electronic structure of COK-69 was determined by molecular modeling, and a band gap of 3.77 eV was found.
引用
收藏
页码：13912 / 13917
页数：6
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