A Flexible Photoactive Titanium Metal-Organic Framework Based on a [TiIV3(μ3-O)(O)2(COO)6] Cluster
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...
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| Veröffentlicht in: | Angewandte Chemie International Edition Jg. 54; H. 47; S. 13912 - 13917 |
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Weinheim
WILEY-VCH Verlag
16.11.2015
WILEY‐VCH Verlag Wiley Subscription Services, Inc |
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| Abstract | 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‐cyclohexanedicarboxylate linkers and an unprecedented [TiIV3(μ3‐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 TiIV center per cluster can be photoreduced to TiIII 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.
A breath of fresh air: Titanocene dichloride was used as the metal source in an innovative synthetic approach to titanium‐based metal–organic frameworks (MOFs). In this way, a breathing Ti MOF (designated COK‐69) featuring a photoactive trinuclear cluster was built up from trans‐1,4‐cyclohexanedicarboxylate and an unprecedented, photoactive [TiIV3(μ3‐O)(COO)6] inorganic building unit (see picture). |
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| AbstractList | 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‐cyclohexanedicarboxylate linkers and an unprecedented [TiIV3(μ3‐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 TiIV center per cluster can be photoreduced to TiIII 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.
A breath of fresh air: Titanocene dichloride was used as the metal source in an innovative synthetic approach to titanium‐based metal–organic frameworks (MOFs). In this way, a breathing Ti MOF (designated COK‐69) featuring a photoactive trinuclear cluster was built up from trans‐1,4‐cyclohexanedicarboxylate and an unprecedented, photoactive [TiIV3(μ3‐O)(COO)6] inorganic building unit (see picture). 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-cyclohexanedicarboxylate linkers and an unprecedented [Ti(IV)3(μ3-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. 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 TiMOF, which is built up from trans-1,4-cyclohexanedicarboxylate linkers and an unprecedented [TiIV3(µ3-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 TiIV center per cluster can be photoreduced to TiIII while preserving the structural integrity of the framework. The electronic structure of COK-69 was determined by molecular modeling, and a band gap of 3.77eV was found. 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‐cyclohexanedicarboxylate linkers and an unprecedented [Ti IV 3 (μ 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. |
| Author | Vermoortele, Frederik Bueken, Bart Valvekens, Pieterjan Ameloot, Rob Reinsch, Helge Kirschhock, Christine E. A. Mayer, James M. De Vos, Dirk Tsou, Chih-Chin Van Speybroeck, Veronique De Baerdemaeker, Trees Vanpoucke, Danny E. P. |
| Author_xml | – sequence: 1 givenname: Bart surname: Bueken fullname: Bueken, Bart organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 2 givenname: Frederik surname: Vermoortele fullname: Vermoortele, Frederik organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 3 givenname: Danny E. P. surname: Vanpoucke fullname: Vanpoucke, Danny E. P. organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium) – sequence: 4 givenname: Helge surname: Reinsch fullname: Reinsch, Helge organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 5 givenname: Chih-Chin surname: Tsou fullname: Tsou, Chih-Chin organization: Department of Chemistry, Yale University, 225 Prospect Street, p.o. box 208107, New Haven, CT 06511 (USA) – sequence: 6 givenname: Pieterjan surname: Valvekens fullname: Valvekens, Pieterjan organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 7 givenname: Trees surname: De Baerdemaeker fullname: De Baerdemaeker, Trees organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 8 givenname: Rob surname: Ameloot fullname: Ameloot, Rob organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 9 givenname: Christine E. A. surname: Kirschhock fullname: Kirschhock, Christine E. A. organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) – sequence: 10 givenname: Veronique surname: Van Speybroeck fullname: Van Speybroeck, Veronique organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium) – sequence: 11 givenname: James M. surname: Mayer fullname: Mayer, James M. organization: Department of Chemistry, Yale University, 225 Prospect Street, p.o. box 208107, New Haven, CT 06511 (USA) – sequence: 12 givenname: Dirk surname: De Vos fullname: De Vos, Dirk email: dirk.devos@biw.kuleuven.be organization: Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, p.o. box 2461, 3001 Leuven (Belgium) |
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| Copyright | 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim |
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| Keywords | molecular modeling photochemistry titanium metal-organic frameworks metallocenes |
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| SubjectTerms | metal-organic frameworks metallocenes molecular modeling photochemistry Titanium |
| Title | A Flexible Photoactive Titanium Metal-Organic Framework Based on a [TiIV3(μ3-O)(O)2(COO)6] Cluster |
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