Monodisperse palladium nanoparticles assembled on graphene oxide with the high catalytic activity and reusability in the dehydrogenation of dimethylamine-borane
Monodisperse palladium nanoparticles assembled on graphene oxide with the high catalytic activity and reusability in the dehydrogenation of dimethylamine-borane
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DOI：
10.1016/j.ijhydene.2018.03.175
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发表时间：
2018-11-01
影响因子：
7.2
通讯作者：
Sen, Fatih
中科院分区：
文献类型：
--
作者：
Sen, Betul;Aygun, Aysenur;Sen, Fatih
合成了高效稳定的氧化石墨烯负载钯纳米粒子（PdNPs），并对其进行了表征和应用于二甲胺硼烷（DMAB）的脱氢反应。以油胺和GO为载体，采用超声还原法在室温下合成了单分散钯纳米粒子。通过过滤反应混合物，以可再现的方式分离出尺寸为3.89 nm的几乎均匀分布的Pd（0）纳米颗粒。采用TEM、HRTEM、XRD、拉曼和XPS等手段对样品进行了表征。发现Pd@GO NP是稳定的，并且是DMAB脱氢中最具活性的催化剂之一。该催化剂的转化频率为38.02h（-1），是文献中制备的DMAB脱氢催化剂中最好的催化剂之一。计算了催化脱氢反应的活化焓（Δ H-#）、活化熵（Δ S-#）和表观活化能（Ea），分别为16.5 kJ mol（-1）、-179 Jmol（-1）K（-1）和18.6 kJ mol（-1）。(C)2018年氢能出版有限责任公司。由爱思唯尔有限公司出版。保留所有权利。
Highly effective and stable palladium nanoparticles (Pd NPs) supported on graphene oxide (GO) were synthesized, characterized and applied for dehydrogenation of dimethylamine-borane (DMAB). Monodisperse Pd NPs were synthesized with the ultrasonic reduction method in the presence of oleylamine and GO as support matrices at room temperature. Almost uniformly distributed Pd (0) nanoparticles in size of 3.89 nm were isolated in a reproducible manner by filtering through the reaction mixture. They were characterized by TEM, HRTEM, XRD, Raman, and XPS. It was found that Pd@GO NPs are stable and one of the most active catalysts in the dehydrogenation of DMAB. This catalyst with its turnover frequency of 38.02 h(-1) exhibits one of the good results among all the catalysts prepared in the literature for dehydrogeneration of DMAB. Significant activation parameters of the catalytic dehydrogenation reaction were also calculated, and the activation enthalpy (Delta H-#), activation entropy (Delta S-#) and the apparent activation energy (Ea) were found 16.5 kJ mol(-1), -179 J mol(-1) K-1, and 18.6 kJ mol(-1), respectively. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.