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A series of copper(II) with 2-aminobenzonitrile and 3-(2-oxo-pyrrolidin-yl)-propionitrile were first synthesized and characterized, and the reaction of these nitriles with Cu(OAc)·HO or CuCl·2HO in ethanol resulted in the production of three novel copper complexes, I, II, and III. In addition, we obtained the manganese (II) oxygen complex ( IV) in the process of synthesis of the manganese (II) nitrogen complex, in which o-phenylenediamine was used as the ligands to react with MnCl·4HO. The structure of each complex was determined by X-ray diffraction analysis. Each complex was also characterized using elemental analysis, H NMR and IR. The complexes were then all used to catalyze the Henry reaction, and moderate catalytic results were achieved. Graphical Abstract: A series of copper(II) with 2-aminobenzonitrile and 3-(2-oxo-pyrrolidin-yl)-propionitrile were first synthesized and characterized, and the reaction of these nitriles with Cu(OAc)·HO or CuCl·2HO in ethanol resulted in the production of three novel copper complexes, I, II, and III. In addition, we obtained the manganese (II) oxygen complex ( IV) in the process of synthesis of the manganese (II) nitrogen complex, in which o-phenylenediamine was used as the ligands to react with MnCl·4HO. The structure of each complex was determined by X-ray diffraction analysis. Each complex was also characterized using elemental analysis, H NMR and IR. The complexes were then all used to catalyze the Henry reaction, and moderate catalytic results were achieved. [Figure not available: see fulltext.] [ABSTRACT FROM AUTHOR]