The utilization of formic acid (FA) as efficient H 2 medium through the conversion between FA and CO 2 has received the great attention recently. In this research, the mesoporous material layered double hydroxide grafted with different types of amine groups (primary, secondary, and tertiary amine) have been synthesized via traditional impregnation method. The primary amine becomes the significant parameter to synthesis of ultrafine Pd nano-particles with high initial TOF of 1250 h −1 at room temperature in FA dehydrogenation. Meanwhile, the de...