Oxygen Reduction Catalyzed by Platinum Nanoparticles Supported on Graphene Quantum Dots

被引:184
作者
He, Guoqiang [1 ]
Song, Yang [1 ]
Liu, Ke [1 ]
Walter, Andrew [1 ]
Chen, Sophie [1 ]
Chen, Shaowei [1 ]
机构
[1] Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA
来源
ACS CATALYSIS | 2013年 / 3卷 / 05期
基金
美国国家科学基金会;
关键词
graphen quantum dot; platinum nanoparticle; oxygen reduction; defect; X-ray diffraction; XPS; Tafel plot; FUEL-CELL APPLICATIONS; ELECTROCATALYTIC ACTIVITY; CARBON; FUNCTIONALIZATION; STABILITY; XPS; 1ST-PRINCIPLES; SPECTROSCOPY; ENHANCEMENT; COMPOSITE;
D O I
10.1021/cs400114s
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
Nanosized graphene quantum dots were prepared by acid etching of carbon fibers and used as effective substrate supports for platinum nanoparticles which were synthesized by thermolytic reduction of platinum(II) chloride in ethylene glycol. Transmission electron microscopic measurements showed that the resulting nanocomposite (Pt/G) particles exhibited in average diameter of 2.79 +/- 0.38 nm, with clearly defined lattice fringes. of 0.23 nm that might be assigned to the interlayer spacing of the (111) Crystal planes of fcc Pt. In addition, the Pt nanoparticles were found to be wrapped with a low-contrast halo that likely arose from the Poorly:, crystalline:graphene Quantum dots. X-ray diffraction studies confirmed the composite nature of the Pt/G nanoparticles, and the average size of the crystal doinains of the Pt/G nanoparticles was found to be close to the nanoparticle physical dimensions,, whereas for. commercial Pt/C nano, particles the size. :of the crystal domains was only half that of the nanoparticle diameter. XPS measurements showed the formation of metallic platinum along with sp(2) and oxygenated carbons in the nanocomposite nanoparticles. Significantly, in comparison with commercial Pt/C catalysts, the Pt/G nanocomposites showed markedly enhanced catalytic activity in oxygen reduction reactions, with an onset potential of +1.05 V that was 70 mV more positive than that of Pt/C, and a specific activity that was almost nine times higher. These results were ascribed to the abundant structural defects of the nanosized graphene quantum dots that manipulated that dissociative adsorption of oxygen and the binding of reaction intermediates O* and HO* on platinum surfaces.
引用
收藏
页码:831 / 838
页数:8
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