Ln-substituted polytungstates as efficient hetergeneous catalysts for Knoevenagel condensation reaction

Three isomorphic polytungstates,CsgK_(18)H_(10){[Sm_(2)(H_(2)O)_(4)W_(4)O_(10)(AsW_(9)0_(33))3]_(2)(N(CH_(2)PO_(3))_(2))}:46.5H_(2)O(1),CS_(10)K_(9)H_(18){[Eu_(2)(H_(2)O)_(4)W_(4)O_(10)(AsW_(9)0_(33))_(3)]_(2)(N(CH_(2)PO_(3))_(2))}.41.5H_(2)O(2),Cs_(10)K_(9)H_(18){[Gd_(2)(H_(2)O)_(4)W_(4)O_(10)(AsW_(9)O_(33))_(3)]_(2)(N(CH_(2)PO_(3))_(2))}:46H_(2)O(_(3)),have been successfully synthesized and characterized by routine methods,and demonstrated excellent catalytic activities in Knoevenagel condensation reaction as heterogeneous catalysts.Notably,catalyst 1 achieved higher reaction activity than catalysts 2 and 3,where a satisfactory reaction yield(95%)and high TON value(6380)could be obtained at moderate reaction condition.In addition,in the scale-up experiment,with the help of catalyst 1,7.8g benzaldehyde and 5.7g ethyl cyanoacetate could transform into corresponding condensation product with a satisfactory yield(83%)and impressive TON value(13.883).

Synthesis,Structures,Luminescence and Catalytic Activity in the Knoevenagel Condensation Reaction of Two Cd(Ⅱ)Coordination Polymers Based on a Biphenyl-dicarboxylic Acid

Two cadmium(II)coordination polymers,namely[Cd(μ-dda)(H2 biim)]n(1)and[Cd(μ4-dda)(py)]n(2)have been constructed hydrothermally using H2 dda(H2 dda=4,4?-dihydroxybiphenyl-3,3?-dicarboxylic acid),H_(2)biim(H_(2)biim=2,2?-biimidazole),py(py=pyridine),and cadmium chloride at 160°C.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses(TGA),and single-crystal X-ray diffraction analyses.Single-crystal X-ray diffraction analyses revealed that both compounds crystallize in the monoclinic system,space group C2/c.Compound 1 discloses a 1 D chain structure.Compound 2 features a 3 D framework.The luminescent properties of compounds 1 and 2 were evaluated.Besides,the catalytic activities in the Knoevenagel condensation reaction of two compounds were investigated.Compound 1 exhibits an excellent catalytic activity in the Knoevenagel condensation reaction at room temperature.

Syntheses,crystal structures,and catalytic properties of three zinc(Ⅱ),cobalt(Ⅱ)and nickel(Ⅱ)coordination polymers constructed from 5⁃(4⁃carboxyphenoxy)nicotinic acid

Three zinc(Ⅱ),cobalt(Ⅱ),and nickel(Ⅱ)coordination polymers,namely[Zn(μ^(3-)cpna)(μ-dpea)_(0.5)]_(n)(1),[Co(μ^(3-)cpna)(μ-dpey)_(0.5)]_(n)(2),and[Ni(μ^(3-)cpna)(μ-dpey)_(0.5)(H_(2)O)]_(n)(3),have been constructed hydrothermally using H_(2)cpna(5-(4-carboxyphenoxy)nicotinic acid),dpea(1,2-di(4-pyridyl)ethane),dpey(1,2-di(4-pyridyl)ethylene),and zinc,cobalt,and nickel chlorides at 160℃.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses,and single-crystal X-ray diffraction analyses.Single-crystal X-ray diffraction analyses revealed that three compounds crystallize in the triclinic system,space group P1.Compounds 1-3 show 2D layer structures.The catalytic activities in the Knoevenagel condensation reaction of these compounds were investigated.Compounds 1 and 2 exhibit effective catalytic activities in the Knoevenagel condensa-tion reaction at room temperature.For this reaction,various parameters were optimized,followed by the investiga-tion of the substrate scope.CCDC:2335676,1;2335677,2;2335678,3.

Synthesis and structures of malonate derivative-calix [4] arene conjugates

A series of malonate derivatives-calix[4]arene conjugates were synthesized through Knoevenagel condensation reaction between formyl-tetrapropoxycalix[4]arene and malonate derivatives. The structures of the resulting malonate derivative functionalized calix[4]arenes were characterized by NMR spectroscopy, mass spectrometry and even single crystal X-ray diffraction analysis.

Sulfamic acid as a green,reusable catalyst for stepwise,tandem&one-pot solvent-free synthesis of pyrazole derivatives

Sulfamic acid（SA） is a bi-functional, cost-effective and reusable green catalyst for the synthesis of 4-（pyrazol-4-yl）methylenepyrazol-5（4H）-one derivatives by one-pot, three-component condensation of pyrazol-4-carbaxaldehydes, b-ketoesters and phenyl hydrazine（Route-I）. In addition to this method,another simple condensation of pyrazol-4-carbaxaldehydes with pyrazolone in the presence of SA under the solvent-free condition in good yield is reported. The merits of these protocols are mild conditions,non-aqueous workup, high yields, easy availability of the catalyst, no chromatographic separation and inexpensive solid acid catalyst. Furthermore, SA could be recycled and reused for five times without losing its catalytic activity.