Fuel purification, Lewis acid and aerobic oxidation catalysis performed by a microporous Co-BTT (BTT3-=1,3,5-benzenetristetrazolate) framework having coordinatively unsaturated sites

被引:74
作者
Biswas, Shyam [1 ]
Maes, Michael [2 ]
Dhakshinamoorthy, Amarajothi [3 ,4 ]
Feyand, Mark [1 ]
De Vos, Dirk E. [2 ]
Garcia, Hermenegildo [3 ,4 ]
Stock, Norbert [1 ]
机构
[1] Univ Kiel, Inst Anorgan Chem, D-24118 Kiel, Germany
[2] Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, B-3001 Louvain, Belgium
[3] Inst Univ Tecnol Quim CSIC UPV, Valencia 46022, Spain
[4] Univ Politecn Valencia, Dept Quim, Valencia 46022, Spain
关键词
METAL-ORGANIC FRAMEWORK; HETEROGENEOUS ASYMMETRIC HYDROGENATION; GAS-ADSORPTION; CARBON-DIOXIDE; SORPTION PROPERTIES; PERMANENT POROSITY; THERMAL-STABILITY; POROUS SOLIDS; HYBRID SOLIDS; LIQUID-PHASE;
D O I
10.1039/c2jm15592c
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Two isostructural microporous metal-organic frameworks [Co(DMA)(6)](3)[(Co4Cl)(3-)(BTT)(8)(H2O)(12)](2)center dot 12H2O (BTT3- = 1,3,5-benzenetristetrazolate; DMA N,N'-dimethylacetamide) (1) and [Cd(DMF)(6)](3)[(Cd4Cl)(3)(BTT)(8)(H2O)(12)](2)center dot 14H(2)O center dot 4DMF (DMF = N,N'-dimethylformamide) (2) were synthesized under solvothermal conditions. The structures of both compounds were determined by single-crystal X-ray diffraction data. Each compound adopts a porous three-dimensional framework consisting of square-planar [M4Cl](7+) (M2+ = Co, 1; Cd, 2) units interconnected by triangular tritopic BTT3- bridging ligands to give an anionic (3,8)-connected "Moravia" net. Phase purity of the compounds was confirmed by X-ray powder diffraction (XRPD), IR spectroscopy, thermogravimetric (TG) and elemental analysis. TGA and temperature-dependent XRPD (TDXRPD) experiments indicate a moderate thermal stability up to 350 and 300 degrees C, respectively. Guest exchange followed by heating led to microporous solids with coordinatively unsaturated metal sites. These unsaturated metal sites create opportunities in adsorptive and catalytic applications. These have been probed by the selective removal of sulfur compounds from fuel feeds as well as the catalytic ring opening of styrene oxide and the oxidation of several cycloalkanes and benzyl compounds.
引用
收藏
页码:10200 / 10209
页数:10
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