Copper-organic frameworks assembled from in situ generated 5-(4-pyridyl)tetrazole building blocks: synthesis, structural features, topological analysis and catalytic oxidation of alcohols

被引:74
作者
Nasani, Rajendar [1 ]
Saha, Manideepa [1 ]
Mobin, Shaikh M. [1 ]
Martins, Luisa M. D. R. S. [2 ,3 ]
Pombeiro, Armando J. L. [3 ]
Kirillov, Alexander M. [3 ]
Mukhopadhyay, Suman [1 ]
机构
[1] Indian Inst Technol Indore, Sch Basic Sci, Dept Chem, Indore 452017, India
[2] ISEL, Dept Chem Engn, P-1959007 Lisbon, Portugal
[3] Univ Lisbon, Inst Super Tecn, Ctr Quim Estrutural, P-1049001 Lisbon, Portugal
关键词
STATE COORDINATION CHEMISTRY; BIS-TETRAZOLATO COMPLEXES; AEROBIC OXIDATION; TRANSITION-METAL; 1,3-DIPOLAR CYCLOADDITION; 5-SUBSTITUTED TETRAZOLES; MICROWAVE SYNTHESIS; SELECTIVE OXIDATION; BENZYLIC ALCOHOLS; ALLYLIC OXIDATION;
D O I
10.1039/c4dt00531g
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Two new metal- organic compounds {[Cu-3(mu(3)-4-(p)tz)(4)(mu(2)-N-3)(2)(DMF)(2)](DMF)(2)}(n) (1) and {[Cu(4ptz) (2)(H2O)(2)]}(n) (2) {4-ptz = 5-(4-pyridyl)tetrazolate} with 3D and 2D coordination networks, respectively, have been synthesized while studying the effect of reaction conditions on the coordination modes of 4-pytz by employing the [2 + 3] cycloaddition as a tool for generating in situ the 5-substituted tetrazole ligands from 4-pyridinecarbonitrile and NaN3 in the presence of a copper(II) salt. The obtained compounds have been structurally characterized and the topological analysis of 1 discloses a topologically unique trinodal 3,5,6-connected 3D network which, upon further simplification, results in a uninodal 8-connected underlying net with the bcu (body centred cubic) topology driven by the [Cu-3(mu(2)-N-3)(2)] cluster nodes and mu(3)-4-ptz linkers. In contrast, the 2D metal-organic network in 2 has been classified as a uninodal 4-connected underlying net with the sql [Shubnikov tetragonal plane net] topology assembled from the Cu nodes and mu(2)-4-ptz linkers. The catalytic investigations disclosed that 1 and 2 act as active catalyst precursors towards the microwave-assisted homogeneous oxidation of secondary alcohols (1-phenylethanol, cyclohexanol, 2-hexanol, 3-hexanol, 2-octanol and 3-octanol) with tert-butylhydroperoxide, leading to the yields of the corresponding ketones up to 86% (TOF = 430 h(-1)) and 58% (TOF = 290 h(-1)) in the oxidation of 1-phenylethanol and cyclohexanol, respectively, after 1 h under low power ( 10 W) microwave irradiation, and in the absence of any added solvent or additive.
引用
收藏
页码:9944 / 9954
页数:11
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