Platinum Nanoparticle Functionalized CNTs as Nanoscaffolds and Catalysts To Enhance the Dehydrogenation of Ammonia-Borane

Platinum Nanoparticle Functionalized CNTs as Nanoscaffolds and Catalysts To Enhance the Dehydrogenation of Ammonia-Borane
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DOI:
10.1021/jp1091152
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发表时间:
2010-12-16
影响因子:
3.7
通讯作者:
Yu, X. B.
Yu, X. B.
中科院分区:
化学3区
文献类型:
--
作者:
Li, S. F.;Guo, Y. H.;Yu, X. B.

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本文报道了通过新的“氨潮解”方法制备的铂纳米颗粒功能化碳纳米管(CNTs)(Pt@CNTs)改性的氨硼烷(AB,NH3BH3)的脱氢性能。已经证明,碳纳米管和铂纳米颗粒的协同催化作用以及碳纳米管中AB的纳米限制是增强AB脱氢的两个关键因素。碳纳米管和铂纳米粒子对AB的热解表现出良好的催化活性,不仅抑制了有毒副产物环硼氮烷的排放,而且防止了分解过程中严重的材料发泡和膨胀。同时,通过“氨潮解”方法对AB进行纳米限制,增强了脱氢动力学,在70℃下5小时内释放出第一当量的氢气,而在相同条件下原始AB中没有释放氢气。通过阿伦尼乌斯方法计算出改性AB的活化能为106.2 kJ mol(-1),与原始AB的活化能(137.8 kJ mol(-1))相比大大降低。这些结果表明,“氨潮解”方法与 Pt@CNTs 作为催化剂相结合是改变 AB 性能并有利脱氢的有效方法。
In this paper, the dehydrogenation properties of ammonia-borane (AB, NH3BH3) modified with platinum nanoparticle functionalized carbon nanotubes (CNTs) (Pt@CNTs) that were prepared through a new "ammonia-deliquescence" method are reported. It has been demonstrated that the synergetic catalysis of CNTs and platinum nanoparticles, and the nanoconfinement of AB incorporated into the CNTs are two crucial factors in enhancing the dehydrogenation of AB. Both CNTs and platinum nanoparticles showed favorable catalytic activities toward the thermolysis of AB, which not only depressed the emission of the poisonous byproduct borazine, but also prevented severe material foaming and expansion during the decomposition. Meanwhile, the nanoconfinement of AB through the "ammonia-deliquescence" method led to enhanced dehydrogenation kinetics, releasing the first equivalent of hydrogen at 70 degrees C within 5 h, while no hydrogen was released from pristine AB under the same conditions. By the Arrhenius method, the activation energy of the modified AB was calculated to be 106.2 kJ mol(-1), which is reduced considerably compared to the activation energy for the pristine AB (137.8 kJ mol(-1)). These results indicate that the "ammonia-deliquescence" method combined with the utilization of Pt@CNTs as catalyst is an effective approach in modifying the properties of AB with favorable dehydrogenation.