期刊
DALTON TRANSACTIONS
卷 41, 期 13, 页码 3832-3842出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2dt12187e
关键词
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资金
- Fundacion Seneca [08670/PI/08]
- Universidad de Murcia
- DST
- UGC
The synthesis of mono- and dinuclear cyclometallated palladium(II) complexes with deprotonated saccharinate ligands displaying different coordination modes is described. The new compounds were prepared by direct reaction between saccharine and the corresponding hydroxo-complexes [{Pd(mu-OH) (C boolean AND N)}(2)] (C boolean AND N = 2-(2-pyridyl)phenyl (Phpy) I; = 7,8-benzoquinolyl (Bzq) II), showing a general formula [{Pd(mu-sac)(C boolean AND N)}(2)] with saccharinate 1 displaying a bridging -NCO-coordination mode. Bridge splitting with neutral ligands (L = pyridine (py) 2, quinoline (quinol) 3 or acridine (acrid) 4) yielded new mononuclear derivatives with saccharinate acting as an N-monodentated ligand. Structural characterization by X-ray diffraction of complexes I1, I2 and II2 confirmed the proposed formulae. All complexes emit in the solution and solid state at room temperature. Emission features between 640-680 nm in the solid state for complexes I1 and II1 are significantly red-shifted if compared to the emission in solution. These broad emissions are consistent with the simultaneous presence of 3 pp* and (MMLCT)-M-3 transitions indicating the existence of a strong intramolecular Pd-Pd ground state interaction. The dimeric complexes have also shown to catalyze Suzuki-Miyaura cross-coupling of coumaryl tosylate and aryl boronic acids under phosphine-free conditions. Initial studies suggest the involvement of palladium nanoparticles, which has been further investigated using mercury-drop test and poisoning experiments.
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