Fabrication of Gold and Silver Nanoparticles Supported on Zinc Imidazolate Metal-Organic Frameworks as Active Catalysts for Hydrogen Release from Ammonia Borane

制备负载于锌咪唑金属有机框架上的金银纳米粒子作为氨硼烷释放氢气的活性催化剂

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Abstract

Well-dispersed Au and Ag nanoparticles (NPs) have been immobilized on a zinc imidazolate metal-organic framework, Zn(mim), using the "one-pot" method and tested as catalysts in ammonia borane hydrolysis. The AuNPs@Zn(mim) and AgNPs@Zn(mim) materials were characterized by FTIR, XRD, ICP-OES, TGA, BET, SEM, and TEM. The AgNPs@Zn(mim) catalyst showed a high yield (98.5%) and high hydrogen generation rate (3352.71 mL min(-1) g(Ag) (-1)) in NH(3)BH(3) dehydrogenation. The determined activation energies (19.6 kJ mol(-1) for AuNPs@Zn(mim) and 38.13 kJ mol(-1) for AgNPs@Zn(mim)) are lower than those for most reported catalysts containing Au/Ag-MOF used in the hydrolysis of NH(3)BH(3). Moreover, the catalysts tested here revealed good stability and reusability, preserving 71.42% (AuNPs@Zn(mim)) and 88.23% (AgNPs@Zn(mim)) of their initial catalytic activities after five consecutive cycles. In the case of AgNPs@Zn(mim), the combination of the simple and green synthesis method, low active metal content, relatively low cost, and moderate dehydrogenation conditions makes the material an excellent candidate to produce hydrogen from ammonia borane.

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