新型核壳结构催化剂的制备及其对甲酸氧化的催化作用  

Preparation of nitride nanoparticles based core-shell structured catalyst and its catalysis towards formic acid oxidation

作　　者：田新龙[1] 汤海波[1] 余锦南 杜丽[1] 曾建皇[1] 廖世军[1] Xinlong Tian Haibo Tang Jinnan Yu Li Du Jianhuang Zeng Shijun Liao(School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510006, China)

机构地区：[1]华南理工大学化学与化工学院,广州510006

出　　处：《中国科学：化学》2017年第5期641-646,共6页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(编号:21476088;U1301245)资助项目

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.Nitride nanoparticles based core-shell structured catalysts, TiN@Pt/NCNTs and TiCuN@Pt/NCNTs, were prepared successfully by depositing a ultra thin Pt layer on the surface of nitride nanoparticles with a pulse deposition method. It is found that the catalysts exhibited excellent activity and stability towards the anode oxidation of formic acid. The mass activity of TiN@Pt/NCNTs and TiCuN@Pt/NCNTs could be 3.3 and 4.5 times higher than that of the commercial Pt/C catalyst with the same Pt loadings, and they also exhibited outstanding anti-CO poisoning ability and stability. The addition of Cu in nitride nanoparticles could further enhance the performance of the catalyst significantly. The HAADF/STEM images and EDS mapping measurements revealed the core-shell structure of the catalysts. The enhanced activity of TiCuN@Pt/NCNTs should be attributed to the high dispersion of the Pt atoms and the synergistic effect between the Pt shell and nitride core.

关 键 词：脉冲电沉积 氮化物 核壳结构 甲酸氧化 燃料电池 

分 类 号：O643.36[理学—物理化学]