To satisfy global energy demands and maintain sustainable levels of atmospheric greenhouse gases, alternative energy sources are required. H₂ generation from hydrolysis of NaBH₄ represents as a safe and convenient method for storing and releasing H₂. The free amine groups (NH₂) and the big pores in the NH₂-UiO-66 metal-organic framework were exploited to encapsulate ultrasmall bimetallic Ru-Co alloy nanoclusters and monometallic Ru and Co nanoclusters with an average particle size of 1.5 nm via direct anionic exchange technique. To prove the role of the NH₂ groups and the MOF’s pores in the creation of a well and uniform-dispersed ruthenium and cobalt nanoclusters, the NH₂-UiO-66 was calcined at 600 °C for 3 h in the air to prepare N-doped carbonaceous ZrO₂ (ZrO₂N @ C) nanocomposite. Hydrazine hydrate (HH) was used as a reducing agent in the presence of microwave irradiation