Well-Dispersed High-Loading Pt Nanoparticles Supported by Shell−Core Nanostructured Carbon for Methanol Electrooxidation

Shell−core nanostructured carbon materials with a nitrogen-doped graphitic layer as a shell and pristine carbon black particle as a core were synthesized by carbonizing the hybrid materials containing in situ polymerized aniline onto carbon black. In an N-doped carbon layer, the nitrogen atoms subst...

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Bibliographic Details
Published in:Langmuir 2008-04, Vol.24 (7), p.3566-3575
Main Authors: Wu, Gang, Li, Deyu, Dai, Changsong, Wang, Dianlong, Li, Ning
Format: Article
Language:English
Subjects:
Applied sciences
Catalysis
Chemistry
Colloidal state and disperse state
Energy
Energy. Thermal use of fuels
Equipments for energy generation and conversion: thermal, electrical, mechanical energy, etc
Exact sciences and technology
Fuel cells
General and physical chemistry
Physical and chemical studies. Granulometry. Electrokinetic phenomena
Surface physical chemistry
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
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Summary:Shell−core nanostructured carbon materials with a nitrogen-doped graphitic layer as a shell and pristine carbon black particle as a core were synthesized by carbonizing the hybrid materials containing in situ polymerized aniline onto carbon black. In an N-doped carbon layer, the nitrogen atoms substitute carbon atoms at the edge and interior of the graphene structure to form pyridinic N and quaternary N structures, respectively. As a result, the carbon structure becomes more compact, showing curvatures and disorder in the graphene stacking. In comparison with nondoped carbon, the N-doped one was proved to be a suitable supporting material to synthesize high-loading Pt catalysts (up to 60 wt %) with a more uniform size distribution and stronger metal−support interactions due to its high electrochemically accessible surface area, richness of disorder and defects, and high electron density. Moreover, the more rapid charge-transfer rates over the N-doped carbon material are evidenced by the high crystallinity of the graphitic shell layer with nitrogen doping as well as the low charge-transfer resistance at the electrolyte/electrode interface. Beneficial roles of nitrogen doping can be found to enhance the CO tolerance of Pt catalysts. Accordingly, an improved performance in methanol oxidation was achieved on a high-loading Pt catalyst supported by N-doped carbon. The enhanced catalytic properties were extensively discussed based on mass activity (Pt utilization) and intrinsic activity (charge-transfer rate). Therefore, N-doped carbon layers present many advantages over nondoped ones and would emerge as an interesting supporting carbon material for fuel cell electrocatalysts.
ISSN:0743-7463
1520-5827
DOI:10.1021/la7029278