Superior activity of Pd nanoparticles confined in carbon nanotubes for hydrogen production from formic acid decomposition at ambient temperature
Superior activity of Pd nanoparticles confined in carbon nanotubes for hydrogen production from formic acid decomposition at ambient temperature
复制标题
限制在碳纳米管中的钯纳米粒子在环境温度下通过甲酸分解产生氢气的优异活性
DOI：
10.1016/j.jcis.2018.12.017
复制
发表时间：
2019-03-07
影响因子：
9.9
通讯作者：
Yang, Yao-Yue
中科院分区：
文献类型：
--
作者：
Ding, Tian-Yi;Zhao, Zhi-Gang;Yang, Yao-Yue
设计高效、低成本的催化剂是实现常温下甲酸分解制氢（FAD）实际应用的关键。在此，我们报告的混合材料的Pd纳米粒子封装在碳纳米管（CNT）（Pd-CNTs-in）的合成。透射电子显微镜图像显示，大多数Pd纳米粒子（平均直径4.2 +/- 0.8 nm）位于纳米管内部。H-2的程序升温还原研究表明，吸附在CNT内壁上的Pd（II）物种的平均还原温度比吸附在CNT外壁上的Pd（II）物种的平均还原温度低12 ℃。此外，所制备的Pd-CNTs-in催化剂在室温下显示出极高的FAD活性和耐久性。在最初的10 min内，翻转频率（TOF）值高达1135 h（-1），并且在连续3次再循环研究期间没有显著衰减。X射线光电子能谱（XPS）、表面增强红外光谱（SEIRAS）和气相色谱（GC）的研究表明，碳纳米管的限制作用导致了Pd的电子结构调制，这可能是Pd-CNTs-in表面FAD催化活性增强的主要原因。该研究为制备高性能、低成本的甲酸脱氢钯基催化剂提供了新的思路。(C)2018爱思唯尔公司All rights reserved.
Designing highly efficient and low-cost catalysts is essential toward realizing the practical application of hydrogen generation by formic acid decomposition (FAD) under ambient conditions. Herein, we report the synthesis of a hybrid material of Pd nanoparticles encapsulated within carbon nanotubes (CNTs) (Pd-CNTs-in). Transmission electron microscopy images show that most Pd nanoparticles (mean diameter 4.2 +/- 0.8 nm) are located inside the nanotubes. Temperature-programmed reduction studies of H-2 reveal that the average reduction temperature of the Pd(II) species adsorbed on the interior wall of the CNTs is 12 degrees C lower than those adsorbed on the outer walls of the CNT. Moreover, the as-prepared Pd-CNTs-in catalysts show extremely high FAD activity and durability at ambient temperature. The turn over frequency (TOF) value is as high as 1135 h(-1) for the initial 10 min and does not decay significantly during the consecutive 3-time recycling studies. X-Ray photoelectron spectroscopy (XPS), surface enhanced infrared spectroscopy (SEIRAS), and gas chromatography (GC) studies indicate that CNT confinement induced electronic structure modulation of Pd could be the major reason for the enhancement of FAD catalysis on the Pd-CNTs-in surface. This work could provide promising strategies for the fabrication of cost-effective and high-active Pd-based catalysts for formic acid dehydrogenation. (C) 2018 Elsevier Inc. All rights reserved.