In this study, a new magnetically recoverable NNN-pincer catalyst, Fe3O4@SiO2-NH-CC-AMT-Cu(II), and a novel remarkably efficient and reusable metal-organic framework catalyst, Cu-TSTA MOF, have been developed for the synthesis of propargylamine compounds through one-pot A3 coupling reaction between aromatic aldehydes, morpholine or piperidine, and phenylacetylene via C-H bond activation by utilizing toluene as efficient solvent (Figure A). The target propargylamines were achieved in excellent yields. The catalysts can be reused five times without significant loss of their catalytic activity. The as-synthesized solid heterogeneous catalysts have the interests of attractive yields, low amount of catalyst, and the catalyst recoverability and reusability. Furthermore, a new heterogeneous catalyst was also prepared by immobilizing a mixed-addenda heteropoly acid, H5PMo10V2O40, into an amine-functionalized metal-organic framework, HPMoV@UiO-66-NH2 MOF through post-synthetic modification method and utilized for the selective oxidation of alcohols to corresponding carbonyl compounds by hydrogen peroxide as a green oxidant (Figure B). The influences of reaction time, temperature, amount of H2O2, catalyst loading, and recyclability of the catalyst have also been studied to optimize reaction conditions. The catalyst was re-examined 6 times and no noteworthy reduction in activity was observed. All the produced catalysts were characterized using usual spectroscopic methods, like FT-IR, EDX, FE-SEM, MAP images, TGA, XRD, and ICP-OES.