Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 18, Issue 24, Pages 7443-7451Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201103011
Keywords
density functional calculations; electrochemistry; graphene; nanostructures; platinum
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Funding
- National Natural Science Foundation of China [21031001, 20971040, U1034003, 21001112, 91122018, 21101061]
- Ministry of Education of China [708029]
- Natural Science Foundation of Heilongjiang Province [B201003]
- Education Department of Heilongjiang Province, China [12511388]
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The synergistic effect between Pt and WC is beneficial for methanol electro-oxidation, and makes PtWC catalyst a promising anode candidate for the direct methanol fuel cell. This paper reports on the design and synthesis of small-sized and contacting PtWC nanostructures on graphene that bring the synergistic effect into full play. Firstly, DFT calculations show the existence of a strong covalent interaction between WC and graphene, which suggests great potential for anchoring WC on graphene with formation of small-sized, well-dispersed WC particles. The calculations also reveal that, when Pt attaches to the pre-existing WC/graphene hybrid, Pt particles preferentially grow on WC rather than graphene. Our experiments confirmed that highly disperse WC nanoparticles (ca. 5 nm) can indeed be anchored on graphene. Also, Pt particles 23 nm in size are well dispersed on WC/graphene hybrid and preferentially grow on WC grains, forming contacting PtWC nanostructures. These results are consistent with the theoretical findings. X-ray absorption fine structure spectroscopy further confirms the intimate contact between Pt and WC, and demonstrates that the presence of WC can facilitate the crystallinity of Pt particles. This new PtWC/graphene catalyst exhibits a high catalytic efficiency toward methanol oxidation, with a mass activity 1.98 and 4.52 times those of commercial PtRu/C and Pt/C catalysts, respectively.
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