The catalytic dehydrogenation of hydrazine borane (NHBH) and hydrous hydrazine (NH·HO) for H evolution is considered as two of the pivotal reactions for the implementation of the hydrogen-based economy. A reduction rate controlled strategy is successfully applied for the encapsulating of uniform tiny NiPt alloy nanoclusters within the opening porous channels of MOFs in this work. The resultant NiPt/MOF core-shell composite with a low Pt content exerted exceedingly high activity and durability for complete H evolution (100% hydrogen selectivity) from alkaline NHBH and NH·HO solution. The features of small NiPt alloy NPs, strong synergistic effect between NiPt alloy NPs and the MOF, and open pore structure for freely mass transfer made NiPt/MIL-101 an excellent catalyst for highly efficient H evolution from NHBH or NH·HO.
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