Adsorbate-driven reactive interfacial Pt-NiO(1-x) nanostructure formation on the Pt(3)Ni(111) alloy surface.
Adsorbate-driven reactive interfacial Pt-NiO(1-x) nanostructure formation on the Pt(3)Ni(111) alloy surface.
复制标题
DOI：
10.1126/sciadv.aat3151
复制
发表时间：
2018-07
期刊：
影响因子：
13.6
通讯作者：
Park JY
中科院分区：
文献类型：
--
作者：
Kim J;Park WH;Doh WH;Lee SW;Noh MC;Gallet JJ;Bournel F;Kondoh H;Mase K;Jung Y;Mun BS;Park JY
Formation of catalytically reactive metal oxide interfaces on the Pt3Ni(111) surface is revealed using operando surface analysis. 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 NiO1−x clusters under oxygen gas, and (iii) the coexistence of NiO1−x clusters on the Pt-skin during the CO oxidation reaction. The formation of interfacial Pt-NiO1−x 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 NiO1−x cluster has a low surface energy barrier of 0.37 eV, compared with 0.86 eV for the Pt(111) surface.
登录
查看更多内容
影响因子：
56.9
作者：
Chen, Chen;Kang, Yijin;Stamenkovic, Vojislav R.
通讯作者：
Stamenkovic, Vojislav R.
影响因子：
3.7
作者：
KUHLENBECK, H;ODORFER, G;NEUMANN, M
通讯作者：
NEUMANN, M
影响因子：
3.6
作者：
Naitabdi, Ahmed;Fagiewicz, Robert;Rochet, Francois
通讯作者：
Rochet, Francois
影响因子：
15
作者：
Mu, Rentao;Fu, Qiang;Bao, Xinhe
通讯作者：
Bao, Xinhe
影响因子：
3.7
作者：
Hammer, B;Hansen, LB;Norskov, JK
通讯作者：
Norskov, JK