石墨烯负载Co-CeOx纳米复合物的制备及其对氨硼烷水解产氢的催化性能

Preparation of graphene-supported Co-CeOx nanocomposites as a catalyst for the hydrolytic dehydrogenation of ammonia borane

  • 摘要: 高效、低成本催化剂是实现以氨硼烷(NH3BH3, AB)为化学储氢材料水解产氢的关键。本文采用简单的浸渍还原法,制备了石墨烯负载的Co-CeOx 纳米复合物(Co-CeOx /graphene)催化剂,对其氨硼烷水解产氢的催化性能进行了研究。结果表明,Co与CeOx 之间存在强的协同电子效应,同时高分散的纳米Co-CeOx 粒子与石墨烯之间存在强的金属--载体相互作用,因而所制备的Co-CeOx /graphene催化剂对氨硼烷水解具有良好的催化活性和循环稳定性。Co-CeOx /graphene催化剂上氨硼烷水解的活化能( Ea )为39.5 kJ/mol,反应转化频率(TOF)为45.1 min−1,分别为纯Co及Co/graphene催化剂上的12倍与9倍之多,高于大多数已报道的非贵金属催化剂。

     

    Abstract: Low-cost and high-performance catalyst is crucial for hydrogen generation via the hydrolysis of ammonia borane (NH3BH3, AB) as a chemical hydrogen storage material. In this work, Co-CeOx nanocomposites supported on graphene (Co-CeOx/graphene) were prepared through a facile impregnation and chemical reduction method and used as a catalyst in the hydrolytic dehydrogenation of ammonia borane. The results indicate that the as-prepared Co-CeOx/graphene nanocomposite exhibits superior catalytic activity and recycling stability in the hydrolysis of ammonia borane, owing to the ultra-fine size of Co-CeOx particles, the strong synergistic electronic effect between Co and CeOx, as well as the strong metal-support interaction between Co-CeOx and graphene. For the hydrolysis of ammonia borane over the optimized Co-CeOx/graphene catalyst, the turnover frequency (TOF) reaches 45.1 min−1, with the activation energy (Ea) of 39.5 kJ/mol; such a TOF value is 12 times and 9 times higher than those over Co and Co/graphene, respectively, also much higher than those reported for most noble-metal-free catalysts.

     

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