In this work, copper-based metal organic frameworks Cu3(BTC)2 (BTC = 1,3,5-benzenetricarboxylatle), were applied in the conversion of toxic oxynitride into nitrogen at low temperature. Scanning electron microscope (SEM), thermal gravimetric analysis (TGA), X-ray photoelectron spectroscopy (XRD) and other characterization methods were employed to fully understand the properties of the catalysts. We introduced acetic acid into the synthesis process as the modulator of the crystal structure and morphology. The catalytic assessment indicated that compared with the prototype, modified Cu-MOFs materials obtain enhanced catalytic activity for the SCR reaction. Besides, several thermolysis experiments were conducted to explain structure–function relationship.