Abstract： 

High performance heterogeneous catalysts are strongly dependent on the availability of interfaces. However, the formation of these interfaces is often compromised by harsh synthetic conditions, low structural controllability, and limited active sites. Here, we report that a facile in-situ growth of copper nanoparticles (NPs) in a cobalt metal-organic framework (Cu NPs-Co MOF), via solvothermal and moderate activation process, leads to catalysts with abundant dual sites at their interface. The optimized Cu-0.5@Co-0.5-MOF/5 composite exhibits outstanding performances with a turnover frequency of 129.8 min(-1), stability of over 10 cycles and low activation energy of 26.5 kJ.mol(-1) for ammonia borane hydrolysis. Such a prominent activity is achieved by the intimate synergy of Cu degrees-Co2+ atomic ensembles at the interface, which substantially boost the reaction rate by catalyzing ammonia borane and water in a synchronized manner. This research opens up a new pathway for the rational design of non-noble metal heterogeneous catalysts by fabricating metal NPs-MOFs interfaces at nanoscale.