Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 33, Pages 11610-11615Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b06859
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Funding
- China Scholarship Council (CSC) of the People's Republic of China
- University of Toulouse 3
- University of Bordeaux
- Centre National de la Recherche Scientifique (CNRS)
- CIC biomaGUNE (FP7-PEOPLE-IRSES- HIGRAPHEN Project) [612704]
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Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate,dispersion, which in ttirn 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 mol(H2) mol(cat)(-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 kitietic 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.
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