新型核壳结构催化剂的制备及其对甲酸氧化的催化作用

发布时间：2018-08-22 10:11

【摘要】：本文通过采用脉冲电沉积技术在氮化物纳米粒子表面沉积原子层厚度的铂,成功地制得了以碳纳米管负载氮化物纳米粒子为核的新型核壳结构催化剂TiN@Pt/NCNTs,并考察了催化剂对于甲酸氧化的催化活性和稳定性.在相同铂负载量情况下,TiN@Pt/NCNTs催化剂的甲酸氧化质量活性可达商业Pt/C催化剂的3.3倍,并表现出良好的抗CO中毒能力和电化学稳定性.研究发现,在TiN中添加少量Cu制得的TiCuN@Pt/NCNTs比TiN@Pt/NCNTs表现出更高的催化活性,其Pt的质量活性可达商品Pt/C催化剂的4.5倍.扫描透射电镜(STEM)及能谱图谱(EDS mapping)清楚地揭示了催化剂的核壳结构.独特的核壳结构使得Pt原子得到了良好的分散是催化剂表现出良好活性的重要原因,同时Cu元素在氮化钛中的掺杂可使得Pt的d电子能级进一步降低,使得催化剂的活性得到了进一步的提升.
[Abstract]:In this paper, the thickness of atomic layer on the surface of nitride nanoparticles was deposited by pulsed electrodeposition. A novel core-shell structure catalyst, TiNbr / NCNTs, with carbon nanotube supported nitride nanoparticles as the core, was successfully prepared. The catalytic activity and stability of the catalyst for formic acid oxidation were investigated. Under the same platinum loading, the formic acid oxidation mass activity of TiNr Pt / NCNTs catalyst is 3.3 times higher than that of commercial Pt/C catalyst, and it shows good resistance to CO poisoning and electrochemical stability. It was found that the TiCuN@Pt/NCNTs prepared by adding a small amount of Cu to TiN exhibited higher catalytic activity than TiN@Pt/NCNTs, and the Pt activity was 4.5 times higher than that of commercial Pt/C catalysts. The core-shell structure of the catalyst was clearly revealed by scanning transmission electron microscopy (SEM) (STEM) and energy dispersive spectroscopy (EDS mapping). The excellent dispersion of Pt atoms due to the unique core-shell structure is an important reason for the good activity of the catalyst, and the doping of Cu in titanium nitride can further decrease the d electron level of Pt. The activity of the catalyst was further improved.
【作者单位】：华南理工大学化学与化工学院;
【基金】：国家自然科学基金(编号:21476088,U1301245)资助项目
【分类号】：O643.36;TM911.4

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