title: Gold atomic clusters extracting the valence electrons to shield the carbon monoxide passivation on near-monolayer core-shell nanocatalysts in methanol oxidation reactions.
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.
authors.affiliation: Department of Engineering and System Science, National Tsing Hua University, Hsinchu 30013, Taiwan. chencaeser@gmail.com.
authors.forename: Tsan-Yao
authors.initials: TY
authors.lastname: Chen
authors.forename: Hong Dao
authors.initials: HD
authors.lastname: Li
authors.forename: Guo-Wei
authors.initials: GW
authors.lastname: Lee
authors.forename: Po-Chun
authors.initials: PC
authors.lastname: Huang
authors.forename: Po-Wei
authors.initials: PW
authors.lastname: Yang
authors.forename: Yu-Ting
authors.initials: YT
authors.lastname: Liu
authors.forename: Yen-Fa
authors.initials: YF
authors.lastname: Liao
authors.forename: Horng-Tay
authors.initials: HT
authors.lastname: Jeng
authors.forename: Deng-Sung
authors.initials: DS
authors.lastname: Lin
authors.forename: Tsang-Lang
authors.initials: TL
authors.lastname: Lin