Adsorbate-driven reactive interfacial Pt-NiO1−x nanostructure formation on the Pt3Ni(111) alloy surface

Jeongjin Kim, Woong Hyeon Park, Won Hui Doh, Si Woo Lee, Myung Cheol Noh, Jean Jacques Gallet, Fabrice Bournel, Hiroshi Kondoh, Kazuhiko Mase, Yousung Jung, Bongjin Simon Mun, Jeong Young Park

Research output: Contribution to journalArticlepeer-review

77 Citations (Scopus)


The origin of the synergistic catalytic effect between metal catalysts and reducible oxides has been debated for decades. Clarification of this effect, namely, the strong metal-support interaction (SMSI), requires an understanding of the geometric and electronic structures of metal-metal oxide interfaces under operando conditions. We show that the inherent lattice mismatch of bimetallic materials selectively creates surface segregation of subsurface metal atoms. Interfacial metal-metal oxide nanostructures are then formed under chemical reaction environments at ambient pressure, which thus increases the catalytic activity for the CO oxidation reaction. Our in situ surface characterizations using ambient-pressure scanning tunneling microscopy and ambient-pressure x-ray photoelectron spectroscopy exhibit (i) a Pt-skin layer on the Pt-Ni alloyed surface under ultrahigh vacuum, (ii) selective Ni segregation followed by the formation of NiO1x clusters under oxygen gas, and (iii) the coexistence of NiO1x clusters on the Pt-skin during the CO oxidation reaction. The formation of interfacial Pt-NiO1x nanostructures is responsible for a highly efficient step in the CO oxidation reaction. Density functional theory calculations of the Pt3Ni(111) surface demonstrate that a CO molecule adsorbed on an exposed Pt atom with an interfacial oxygen from a segregated NiO1x cluster has a low surface energy barrier of 0.37 eV, compared with 0.86 eV for the Pt(111) surface.

Original languageEnglish
Article numbereaat3151
JournalScience Advances
Issue number7
Publication statusPublished - 2018 Jul 13

ASJC Scopus subject areas

  • General


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