Gold atomic clusters extracting the valence electrons to shield the carbon monoxide passivation on near-monolayer core–shell nanocatalysts in methanol oxidation reactions

Literature Information

Publication Date 2015-05-07
DOI 10.1039/C5CP01103E
Impact Factor 3.676
Authors

Hong Dao Li, Guo-Wei Lee, Po-Chun Huang, Po-Wei Yang, Yu-Ting Liu, Yen-Fa Liao, Horng-Tay Jeng, Deng-Sung Lin, Tsang-Lang Lin


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Abstract

Atomic-scale gold clusters were intercalated at the inter-facet corner sites of Pt-shell Ru-core nanocatalysts with near-monolayer shell thickness. We demonstrated that these unique clusters could serve as a drain of valence electrons in the kink region of the core–shell heterojunction. As jointly revealed by density functional theory calculations and valence band spectra, these Au clusters extract core-level electrons to the valence band. They prevent corrosion due to protonation and enhance the tolerance of CO by increasing the electronegativity at the outermost surface of the NCs during the methanol oxidation reaction (MOR). In these circumstances, the retained current density of Pt-shell Ru-core NCs is doubled in a long-term (2 hours) MOR at a fixed voltage (0.5 V vs. SCE) by intercalating these sub-nanometer gold clusters. Such novel structural confinement provides a possible strategy for developing direct-methanol fuel cell (DMFC) modules with high power and stability.

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