Abstract

In despite of significant progresses have been accomplished in the programming and development of updated and efficient nana-catalysts for H2 production from a wide variety of chemical hydrogen storage materials. However, it is a practical matter of the utmost importance to develop the “on-off” control for on demand H2 release in the cause of effectively and safely producing, carrying and depositing H2 gas. Herein, we have first designed and synthesized a sequence of carbon nanosphere (CNS)-stabilized bimetallic PtNi nanoparticles (PtNi/CNS), by stabilization of nearly monodispersed PtNi bimetallic nanoparticles onto the surface of carbon nanosphere, for the highly selective and efficient on-demand H2 release upon the dehydrogenation of hydrous hydrazine. Then, the optional nanocatalyst Pt1Ni1/CNS exhibits the highest catalytic performance in hydrogen production from dehydrogenation of hydrous hydrazine, with 100 % H2 selectivity and the turnover frequency (TOF) of 3928 mol (H2)·molcat−1·h−1 at 50 °C. The detailed physical characterizations have confirmed that the superior catalytic performance of Pt1Ni1/CNS in the H2 release upon hydrous hydrazine dehydrogenation is attributed to the electronic interaction and synergistic effect between Ni and Pt. More importantly, the highly selective “on-off” control for demand-based H2 release upon the dehydrogenation of hydrous hydrazine is successfully realized by pH regulation.

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