Nanoceria supported palladium(0) nanoparticles: Superb catalyst in dehydrogenation of formic acid at room temperature
Nanoceria supported palladium(0) nanoparticles: Superb catalyst in dehydrogenation of formic acid at room temperature
复制标题
DOI：
10.1016/j.apcatb.2017.01.063
复制
发表时间：
2017-06-05
影响因子：
22.1
通讯作者：
Ozkar, Saim
中科院分区：
文献类型：
--
作者：
Akbayrak, Serdar;Tonbul, Yalcin;Ozkar, Saim
以纳米氧化铈负载的纳米钯(Pd-0/CeO2)为催化剂，实现了甲酸(FA)的常温高效脱氢。采用Pd(II)离子在CeO2表面浸渍，然后在水溶液中用硼氢化钠还原的方法在室温下制备了Pd-0/CeO2。通过离心法从反应液中分离出Pd(0)/CeO2，并结合先进的分析技术对其进行了表征。考察了Pd负载量在1.0~5.0%wt范围内的Pd-0/CeO2催化剂对甲酸/甲酸钠(FA/SF=1/9)脱氢反应的催化活性。Pd负载量为2.27%wt的Pd-0/CeO2催化剂在25.0+-0.1℃时的转化率为1400h(-1)。Pd-0/CeO2催化剂的优异催化活性归因于甲醛分解过程中CeO2的还原性质；CO2+H-2)。通过测量纯H-2气体的体积得到的动力学数据，可以通过考虑甲酸盐离子和甲酸之间的平衡(HCO2H可逆箭头HCOO-+H3O+)来换算成FA的浓度变化。黄腐酸浓度与时间的关系符合一级动力学规律。(C)2017爱思唯尔B.V.保留所有权利。
Highly efficient dehydrogenation of formic acid (FA) at room temperature was achieved using palladium(0) nanoparticles supported on nanoceria (Pd-0/CeO2) as catalysts. Pd-0/CeO2 was prepared by impregnation of palladium(II) ions on the surface of ceria followed by their reduction with sodium borohydride in aqueous solution at room temperature. Pd((0)/CeO2 was isolated from the reaction solution by centrifugation and characterized by a combination of advanced analytical techniques. The catalytic activity of Pd-0/CeO2 samples with various Pd loading in the range 1.0-5.0% wt was tested in dehydrogenation of formic acid plus sodium formate with a molar ratio of FA/SF = 1/9. Pd-0/CeO2 with Pd loading of 2.27% wt shows superb catalytic activity in dehydrogenation of FA with a turnover frequency (TOF) value of 1400 h(-1) at 25.0 +/- 0.1 degrees C. The superb catalytic activity of Pd-0/CeO2 is ascribed to the reducible nature of ceria during the decomposition of FA (HCO2H -> CO2+H-2). The kinetic data, obtained by measuring the volume of pure H-2 gas, could be converted to the change in concentration of FA by considering the equilibrium between the formate ion and formic acid (HCO2H reversible arrow HCOO- + H3O+). The FA concentration versus time data fit to the first order kinetics with respect to the FA concentration. (C) 2017 Elsevier B.V. All rights reserved.