摘要
Low-cost metallic nanoparticles as catalysts with good performance are highly desired for the development of hydrogen storage materials . In this work, ceria-doped CuNi nanoparticles were successfully immobilized on the surfaces of reduced graphene oxide (rGO) by a simple co-reduction approach in aqueous solution at room temperature, characterized by ICP-OES, XRD , TEM, SEM-EDS and XPS techniques. The as-synthesized CuNi-CeO 2 /rGO nanocomposites with various metal contents had been employed as heterogeneous catalysts for the hydrolytic dehydrogenation of ammonia borane (NH 3 BH 3 , AB) under mild conditions. The optimal catalyst of Cu 0.8 Ni 0.2 -CeO 2 /rGO with CeO 2 content of 13.9 mol% exhibited an excellent catalytic activity with the exceedingly high TOF value of 34.4·mol H2 ·mol catalyst −1 ·min −1 at 298 K. The apparent activation energy was calculated to be 19.1 kJ mol −1 , even lower than most of noble-metal-based catalysts for AB dehydrogenation. The detailed kinetics of AB hydrolysis catalyzed by Cu 0.8 Ni 0.2 -CeO 2 /rGO had been investigated on different concentrations of catalyst, substrate and temperatures. Moreover, the obtained in situ hydrogen from AB hydrolysis can be further applied to reduce 4-nitrophenol with a high TOF value of 8.1 min −1 at room temperature. The high catalytic activity of Cu 0.8 Ni 0.2 -CeO 2 /rGO would be contributed to the small size of CuNi-CeO 2 NPs, metal-metal synergy, and the metal-support interaction.
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