Binding of CO and O on Low-Symmetry Pt Clusters Supported on Amorphous Silica

被引：5

作者：

Li, Lin ^{[1
]}

Ewing, Christopher S. ^{[1
]}

Abdelgaid, Mona ^{[1
]}

Banerjee, Sudesna ^{[1
]}

Garza, Richard B. ^{[1
]}

Hacku, Robert ^{[1
]}

Hess, Nathan D. ^{[1
]}

Hong, Sungil ^{[1
]}

Islamov, Meiirbek ^{[1
]}

Luciani, Lauren L. ^{[1
]}

Papadopoulos, Stefanos ^{[1
]}

Parker, Christopher ^{[1
]}

Patel, Riddhesh A. ^{[1
]}

Pawar, Ritesh ^{[1
]}

Poklar, Miranda H. ^{[1
]}

Salem, Maya ^{[1
]}

Shabnam, Fathima ^{[1
]}

Shukla, Priyanka B. ^{[1
]}

Vena, Sai K. ^{[1
]}

Wang, Huiran ^{[1
]}

Wang, Rui ^{[1
]}

Wei, Xin ^{[1
]}

Yang, Fan ^{[1
]}

Johnson, J. Karl ^{[1
]}

机构：

[1] Univ Pittsburgh, Dept Chem & Petr Engn, Pittsburgh, PA 15261 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2021年 / 125卷 / 25期

基金：

美国国家科学基金会;

关键词：

DENSITY-FUNCTIONAL THEORY; METAL NANOPARTICLES; SURFACE-CHEMISTRY; CATALYST; HYDROGENATION; OXIDATION; MODELS; TRENDS; SIZE;

D O I：

10.1021/acs.jpcc.1c01452

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We quantified the impact of support interactions on the binding and interaction energies of CO and O adsorbed on Pt-13 nanoclusters supported on amorphous silica surfaces through the use of density functional theory calculations. We used an accurate model for amorphous silica having two different surface silanol concentrations, corresponding to low (200 degrees C) and high (715 degrees C) surface pretreatment temperatures. We compared CO and O adsorbed on supported and freestanding Pt-13 clusters. We found that Pt-13 is highly susceptible to both support- and adsorbate-induced reconstruction, depending on the relaxed structure of the Pt-13 cluster on the surface. Structure relaxation effects dominate over electronic effects of the support. We considered an ensemble of 50 different systems by varying the placement of the Pt-13 cluster on the surfaces and by exploring a range of different binding sites for CO and O on the Pt-13 cluster. In select cases, binding energy differences between supported and freestanding Pt-13 are as large as 2 eV. However, the mean absolute error between supported and freestanding clusters over all systems we studied is only a few tenths of an eV. Coverage effects on coadsorption of CO and O are significantly different on supported clusters compared with the Pt(111) surface. Our results can be used for predicting when support interactions may be important for any reaction catalyzed by small metal nanoclusters.

引用

页码：13780 / 13787

页数：8

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