Characterizing the interaction of Pt and PtRu clusters with boron-doped, nitrogen-doped, and activated carbon: Density functional theory calculations and parameterization

被引:62
作者
Acharya, Chethan K. [1 ]
Sullivan, Daniel I. [1 ]
Turner, C. Heath [1 ]
机构
[1] Univ Alabama, Dept Chem & Biol Engn, Tuscaloosa, AL 35487 USA
关键词
D O I
10.1021/jp8034488
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
Previous density functional theory calculations of Pt and PtRu clusters on carbon supports have shown that the adsorption energies of these metal clusters increase substantially with substitutional boron defects in the carbon lattice. Here, the stability of metal clusters is further probed with substitutional nitrogen defects and surface functional groups. Also, the dynamics of Pt and Ru atoms on pure and boron-doped carbon are studied as a function of temperature using ab initio molecular dynamics (AIMD) simulations. Although the time scale accessible is limited, the AIMD simulations show reduced mobility on the boron-doped surface. In order to calculate additional dynamic properties of the systems, such as diffusion coefficients, the motion of the metal clusters should be studied for much longer periods of time, which can be accomplished by performing classical molecular dynamics (MD) simulations. Thus, we have parametrized our electronic structure calculations to an analytical Lennard-Jones (U) potential function, which will enable much longer time and length scales to be simulated in future investigations.
引用
收藏
页码:13607 / 13622
页数:16
相关论文
共 71 条
[21]   A view from the inside: Complexity in the atomic scale ordering of supported metal nanoparticles [J].
Frenkel, AI ;
Hills, CW ;
Nuzzo, RG .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (51) :12689-12703
[22]  
Hammer B, 2000, ADV CATAL, V45, P71
[23]   Control of the growth of ordered C60 films by chemical modification of Pt(111) surfaces [J].
He, H ;
Swami, N ;
Koel, BE .
THIN SOLID FILMS, 1999, 348 (1-2) :30-37
[24]   A fast and robust algorithm for Bader decomposition of charge density [J].
Henkelman, Graeme ;
Arnaldsson, Andri ;
Jonsson, Hannes .
COMPUTATIONAL MATERIALS SCIENCE, 2006, 36 (03) :354-360
[25]   Carbon support effects on bimetallic Pt-Ru nanoparticles formed from molecular precursors [J].
Hills, CW ;
Nashner, MS ;
Frenkel, AI ;
Shapley, JR ;
Nuzzo, RG .
LANGMUIR, 1999, 15 (03) :690-700
[26]   The size-dependent structural phase behaviors of supported bimetallic (Pt-Ru) nanoparticles [J].
Hills, CW ;
Mack, NH ;
Nuzzo, RG .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (12) :2626-2636
[27]   Platinum nanoclusters on graphite substrates: a molecular dynamics study [J].
Huang, SP ;
Balbuena, PB .
MOLECULAR PHYSICS, 2002, 100 (13) :2165-2174
[28]   Effects of electronic structure modifications on the adsorption of oxygen reduction reaction intermediates on model Pt(111)-alloy surfaces [J].
Hyman, Matthew P. ;
Medlin, J. Will .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (45) :17052-17060
[29]   Particle growth behavior of carbon-supported Pt, Ru, PtRu catalysts prepared by an impregnation reductive-pyrolysis method for direct methanol fuel cell anodes [J].
Kawaguchi, T ;
Sugimoto, W ;
Murakami, Y ;
Takasu, Y .
JOURNAL OF CATALYSIS, 2005, 229 (01) :176-184
[30]   Cation doping and oxygen diffusion in zirconia: a combined atomistic simulation and molecular dynamics study [J].
Khan, MS ;
Islam, MS ;
Bates, DR .
JOURNAL OF MATERIALS CHEMISTRY, 1998, 8 (10) :2299-2307