One-step pyrolysis method for the synthesis of highly efficient 3D hollow carbon nanostructure supported metallic catalysts

被引:14
作者
Ding, Ya [1 ,2 ]
Jin, Bo [1 ]
Gu, Gang [1 ]
Xia, Xing-Hua [1 ]
机构
[1] Nanjing Univ, Sch Chem & Chem Engn, Key Lab Analyt Chem Life Sci, Nanjing 210093, Peoples R China
[2] China Pharmaceut Univ, Coll Pharm, Nanjing 210009, Peoples R China
基金
中国国家自然科学基金;
关键词
METHANOL FUEL-CELLS; ORDERED MESOPOROUS CARBON; ELECTROCATALYST SUPPORT; PLATINUM NANOPARTICLES; CO TOLERANCE; ELECTROOXIDATION; OXIDATION; NANOTUBE; PTRU; NANOSPHERES;
D O I
10.1039/b913767j
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
By using a one-step pyrolysis method, porous hollow carbon nanosphere supported PtRu catalysts are synthesized from the metallic salt-adsorbed hollow polymer (i.e. chitosan) nanosphere complex. The hollow polymer structure acts as both the template and the carbon precursor for the hollow structure fabrication, provides sites for dispersing metallic precursors and subsequent nucleation centers for catalyst deposition in the pyrolysis process. TEM, XRD, and XPS measurements show that formation of metallic nanoparticles and carbon support occurs simultaneously in the pyrolysis process, the resultant carbon nanospheres have porous hollow core-shell structure, and the loaded catalyst has high PtRu alloying degree. In addition, the present approach allows us to finely adjust the loading and bulk composition of PtRu particles by changing the concentration and atomic ratio of the metallic solutions for salt adsorption, and the particle size of PtRu can be well controlled to less than 10 nm. Electrochemical results show that the prepared catalyst (with 18.5% wt Pt and the atomic ratio of Pt/Ru 1: 1) shows high electrochemical activity and stability toward the oxidation of methanol, even outperforming the commercial PtRu/XC-72 (JM) catalyst. This excellent performance could be due to the unique structure of carbon nanostructure and the pyrolysis-method-induced high stability and alloying degree of the loaded metallic catalysts.
引用
收藏
页码:9141 / 9146
页数:6
相关论文
共 49 条
[1]   Size-selected synthesis of PtRu nano-catalysts: Reaction and size control mechanism [J].
Bock, C ;
Paquet, C ;
Couillard, M ;
Botton, GA ;
MacDougall, BR .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (25) :8028-8037
[2]   Alternative supports for the preparation of catalysts for low-temperature fuel cells: the use of carbon nanotubes [J].
Carmo, M ;
Paganin, VA ;
Rosolen, JM ;
Gonzalez, ER .
JOURNAL OF POWER SOURCES, 2005, 142 (1-2) :169-176
[3]   Synthesis of ordered, uniform, macroporous carbons with mesoporous walls templated by aggregates of polystyrene spheres and silica particles for use as catalyst supports in direct methanol fuel cells [J].
Chai, GS ;
Shin, IS ;
Yu, JS .
ADVANCED MATERIALS, 2004, 16 (22) :2057-+
[4]   Spherical carbon capsules with hollow macroporous core and mesoporous shell structures as a highly efficient catalyst support in the direct methanol fuel cell [J].
Chai, GS ;
Yoon, SB ;
Kim, JH ;
Yu, JS .
CHEMICAL COMMUNICATIONS, 2004, (23) :2766-2767
[5]   Sintering of passivated gold nanoparticles under the electron beam [J].
Chen, Y ;
Palmer, RE ;
Wilcoxon, JP .
LANGMUIR, 2006, 22 (06) :2851-2855
[6]   PREPARATION OF PLATINUM SUPPORTED ON PREGRAPHITIZED CARBON-BLACKS [J].
COLOMA, F ;
SEPULVEDAESCRIBANO, A ;
FIERRO, JLG ;
RODRIGUEZREINOSO, F .
LANGMUIR, 1994, 10 (03) :750-755
[7]   Effect of Ru surface composition on the CO tolerance of Ru modified carbon supported Pt catalysts [J].
Crabb, EM ;
Ravikumar, MK ;
Thompsett, D ;
Hurford, M ;
Rose, A ;
Russell, AE .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2004, 6 (08) :1792-1798
[8]  
Cullity B. D., 1956, ELEMENTS XRAY DIFFRA, P150
[9]   VEGARD LAW [J].
DENTON, AR ;
ASHCROFT, NW .
PHYSICAL REVIEW A, 1991, 43 (06) :3161-3164
[10]   Facile synthesis of hollow carbon nanospheres from hollow chitosan nanospheres [J].
Ding, Y ;
Xia, XH .
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY, 2006, 6 (04) :1101-1106