5 years ago

Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release

Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release
Didier Astruc, Roberto Ciganda, Chen Zhang, Zhao Wang, Jaime Ruiz, Lionel Salmon, Changlong Wang, Sergio Moya, Jimena Tuninetti
Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate dispersion, which in turn severely limits their catalytic functions. Here, using zeolitic imidazolate framework (ZIF-8) as MOF template, catalytically remarkably efficient ligand-free first-row late transition-metal nanoparticles are prepared and compared. Upon scrutiny of the catalytic principles in the hydrolysis of ammonia-borane, the highest total turnover frequency among these first-row late transition metals is achieved for the templated Ni nanoparticles with 85.7 molH2 molcat–1 min–1 at room temperature, which overtakes performances of previous non-noble metal nanoparticles systems, and is even better than some noble metal nanoparticles systems. Mechanistic studies especially using kinetic isotope effects show that cleavage by oxidative addition of an O–H bond in H2O is the rate-determining step in this reaction. Inspired by these mechanistic studies, an attractive and effective “on–off” control of hydrogen production is further proposed.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b06859

DOI: 10.1021/jacs.7b06859

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