Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 13, Issue 15, Pages 6883-6891Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c0cp02495c
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Funding
- academic research fund AcRF [MOE2009-T2-2-024]
- Ministry of Education, Singapore [2009 NRF-CRP 001-032]
- National Research Foundation, Singapore
- Agency for Science, Technology and Research (A*Star), Singapore [072 134 0054]
- Curtin Research Fellowship
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Pt and Au nanoparticles with controlled Pt : Au molar ratios and PtAu nanoparticle loadings were successfully self-assembled onto poly(diallyldimethylammonium chloride) (PDDA)-functionalized graphene (PDDA-G) as highly effective electrocatalysts for formic acid oxidation in direct formic acid fuel cells (DFAFCs). The simultaneously assembled Pt and Au nanoparticles on PDDA-G showed superb electrocatalytic activity for HCOOH oxidation, and the current density associated with the preferred dehydrogenation pathway for the direct formation of CO2 through HCOOH oxidation on a Pt1Au8/PDDA-G (i.e., a Pt : Au ratio of 1 : 8) is 32 times higher than on monometallic Pt/PDDA-G. The main function of the Au in the mixed Pt and Au nanoparticles on PDDA-G is to facilitate the first electron transfer from HCOOH to HCOOads and the effective spillover of HCOOads from Au to Pt nanoparticles, where HCOOads is further oxidized to CO2. The Pt : Au molar ratio and PtAu nanoparticle loading on PDDA-G supports are the two critical factors to achieve excellent electrocatalytic activity of PtAu/PDDA-G catalysts for the HCOOH oxidation reactions.
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