Probing the Lewis Acidity and Catalytic Activity of the Metal-Organic Framework [Cu3(btc)2] (BTC=Benzene-1,3,5-tricarboxylate)

An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu3(btc)2] (BTC=benzene‐1,3,5‐tricarboxylate). The crystalline material was characterized by X‐ray diffraction, optical microscopy, SEM, X‐ray photoelectron spectroscopy, N2 sorption, thermograv...

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Vydáno v:	Chemistry : a European journal Ročník 12; číslo 28; s. 7353 - 7363
Hlavní autoři:	Alaerts, Luc, Séguin, Etienne, Poelman, Hilde, Thibault-Starzyk, Frédéric, Jacobs, Pierre A., De Vos, Dirk E.
Médium:	Journal Article
Jazyk:	angličtina
Vydáno:	Weinheim WILEY-VCH Verlag 25.09.2006 WILEY‐VCH Verlag Wiley Wiley-VCH Verlag
Témata:	carbon monoxide Chemical Sciences Chemistry Chemistry, Multidisciplinary heterogeneous catalysis IR spectroscopy Lewis acids metal-organic frameworks Physical Sciences Science & Technology DESIGN heterogeneous catalysis STABILITY ISOMERIZATION carbon monoxide Lewis acids IR spectroscopy metal-organic frameworks REARRANGEMENT (+)CITRONELLAL ALPHA-PINENE OXIDE SITES ZEOLITES COORDINATION POLYMERS 2-BROMOPROPIOPHENONE
ISSN:	0947-6539, 1521-3765
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Abstract	An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu3(btc)2] (BTC=benzene‐1,3,5‐tricarboxylate). The crystalline material was characterized by X‐ray diffraction, optical microscopy, SEM, X‐ray photoelectron spectroscopy, N2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number of Cu2O impurities, and particularly on the free CuII coordination sites in the framework. [Cu3(btc)2] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of α‐pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2‐bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu3(btc)2] are hard Lewis acids. Catalyst stability, re‐usability, and heterogeneity are critically assessed. A systematic study of the catalytic properties of a metal‐organic framework: [Cu3(btc)2] is a very selective catalyst for specific isomerizations of terpenes, terpene epoxides, and ketals (see scheme). Together with IR spectroscopic measurements on adsorbed probe molecules, this proves the hard Lewis acid properties of the material.
AbstractList	An optimized procedure was designed for the preparation of the microporous metal-organic framework (MOF) [Cu3(btc)2] (BTC=benzene-1,3,5-tricarboxylate). The crystalline material was characterized by X-ray diffraction, optical microscopy, SEM, X-ray photoelectron spectroscopy, N2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number of Cu2O impurities, and particularly on the free CuII coordination sites in the framework. [Cu3(btc)2] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of alpha-pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2-bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu3(btc)2] are hard Lewis acids. Catalyst stability, re-usability, and heterogeneity are critically assessed. An optimized procedure was designed for the preparation of the microporous metal-organic framework (MOF) [Cu-3(btc),] (BTC=benzene-1,3,5-tricarboxylate). The crystalline material was characterized by X-ray diffraction, optical microscopy, SEM, X-ray photoelectron spectroscopy, N-2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number Of Cu2O impurities, and particularly on the free Cu-II coordination sites in the framework. [Cu-3(btC)(2)] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of a-pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2-bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu-3(btC)(2)] are hard Lewis acids. Catalyst stability, re-usability, and heterogeneity are critically assessed. An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu3(btc)2] (BTC=benzene‐1,3,5‐tricarboxylate). The crystalline material was characterized by X‐ray diffraction, optical microscopy, SEM, X‐ray photoelectron spectroscopy, N2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number of Cu2O impurities, and particularly on the free CuII coordination sites in the framework. [Cu3(btc)2] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of α‐pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2‐bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu3(btc)2] are hard Lewis acids. Catalyst stability, re‐usability, and heterogeneity are critically assessed. A systematic study of the catalytic properties of a metal‐organic framework: [Cu3(btc)2] is a very selective catalyst for specific isomerizations of terpenes, terpene epoxides, and ketals (see scheme). Together with IR spectroscopic measurements on adsorbed probe molecules, this proves the hard Lewis acid properties of the material. An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu 3 (btc) 2 ] (BTC=benzene‐1,3,5‐tricarboxylate). The crystalline material was characterized by X‐ray diffraction, optical microscopy, SEM, X‐ray photoelectron spectroscopy, N 2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number of Cu 2 O impurities, and particularly on the free Cu II coordination sites in the framework. [Cu 3 (btc) 2 ] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of α‐pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2‐bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu 3 (btc) 2 ] are hard Lewis acids. Catalyst stability, re‐usability, and heterogeneity are critically assessed. Abstract An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu 3 (btc) 2 ] (BTC=benzene‐1,3,5‐tricarboxylate). The crystalline material was characterized by X‐ray diffraction, optical microscopy, SEM, X‐ray photoelectron spectroscopy, N 2 sorption, thermogravimetry, and IR spectroscopy of adsorbed CO. CO adsorbs on a small number of Cu 2 O impurities, and particularly on the free Cu II coordination sites in the framework. [Cu 3 (btc) 2 ] is a highly selective Lewis acid catalyst for the isomerization of terpene derivatives, such as the rearrangement of α‐pinene oxide to campholenic aldehyde and the cyclization of citronellal to isopulegol. By using the ethylene ketal of 2‐bromopropiophenone as a test substrate, it was demonstrated that the active sites in [Cu 3 (btc) 2 ] are hard Lewis acids. Catalyst stability, re‐usability, and heterogeneity are critically assessed.
Author	Séguin, Etienne Thibault-Starzyk, Frédéric Jacobs, Pierre A. Poelman, Hilde Alaerts, Luc De Vos, Dirk E.
Author_xml	– sequence: 1 givenname: Luc surname: Alaerts fullname: Alaerts, Luc organization: Centre for Surface Chemistry and Catalysis K.U.Leuven, Kasteelpark Arenberg 23, 3001 Heverlee, Belgium, Fax: (+32) 16-321-998 – sequence: 2 givenname: Etienne surname: Séguin fullname: Séguin, Etienne organization: Laboratoire Catalyse & Spectrochimie CNRS-UMR 6506, ENSICAEN, Boulevard Maréchal Juin 6 14050 Caen CEDEX, France – sequence: 3 givenname: Hilde surname: Poelman fullname: Poelman, Hilde organization: Department of Solid State Sciences Ghent University, Krijgslaan 281 S1, 9000 Gent, Belgium – sequence: 4 givenname: Frédéric surname: Thibault-Starzyk fullname: Thibault-Starzyk, Frédéric organization: Laboratoire Catalyse & Spectrochimie CNRS-UMR 6506, ENSICAEN, Boulevard Maréchal Juin 6 14050 Caen CEDEX, France – sequence: 5 givenname: Pierre A. surname: Jacobs fullname: Jacobs, Pierre A. organization: Centre for Surface Chemistry and Catalysis K.U.Leuven, Kasteelpark Arenberg 23, 3001 Heverlee, Belgium, Fax: (+32) 16-321-998 – sequence: 6 givenname: Dirk E. surname: De Vos fullname: De Vos, Dirk E. email: dirk.devos@biw.kuleuven.be organization: Centre for Surface Chemistry and Catalysis K.U.Leuven, Kasteelpark Arenberg 23, 3001 Heverlee, Belgium, Fax: (+32) 16-321-998
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/16881030$$D View this record in MEDLINE/PubMed https://hal.science/hal-05222814$$DView record in HAL
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Snippet	An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu3(btc)2] (BTC=benzene‐1,3,5‐tricarboxylate). The... An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu 3 (btc) 2 ] (BTC=benzene‐1,3,5‐tricarboxylate).... An optimized procedure was designed for the preparation of the microporous metal-organic framework (MOF) [Cu-3(btc),] (BTC=benzene-1,3,5-tricarboxylate). The... An optimized procedure was designed for the preparation of the microporous metal-organic framework (MOF) [Cu3(btc)2] (BTC=benzene-1,3,5-tricarboxylate). The... Abstract An optimized procedure was designed for the preparation of the microporous metal–organic framework (MOF) [Cu 3 (btc) 2 ]...
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StartPage	7353
SubjectTerms	carbon monoxide Chemical Sciences Chemistry Chemistry, Multidisciplinary heterogeneous catalysis IR spectroscopy Lewis acids metal-organic frameworks Physical Sciences Science & Technology
Title	Probing the Lewis Acidity and Catalytic Activity of the Metal-Organic Framework [Cu3(btc)2] (BTC=Benzene-1,3,5-tricarboxylate)
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