Multiscale Computational Design of Core/Shell Nanoparticles for Oxygen Reduction Reaction

被引:28
作者
Chen, Zhengzheng [1 ]
Zhang, Xu [1 ]
Lu, Gang [1 ]
机构
[1] Calif State Univ Northridge, Dept Phys & Astron, Northridge, CA 91330 USA
关键词
CORE-SHELL NANOPARTICLES; INITIO MOLECULAR-DYNAMICS; HETEROGENEOUS CATALYSIS; ALLOY NANOPARTICLES; STRAIN; PLATINUM; ELECTROCATALYSTS; NANOCRYSTALS; TRANSITION; HYDROGEN;
D O I
10.1021/acs.jpcc.6b11337
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 propose a multiscale computational framework to design core/shell nanoparticles (NPs) for oxygen reduction reaction (ORR). Essential to the framework are linear scaling relations between oxygen adsorption energy and surface strain, which can be determined for NP facets and edges from first-principles and multiscale QM/MM calculations, respectively. Based on the linear scaling relations and a microkinetic model, we can estimate ORR rates as a function of surface strain on core/shell NPs. Employing the multiscale framework, we have systematically examined the ORR activity on Pd-based core/shell NPs as a function of their shape, size, shell thickness, and alloy composition of the core. Three NP shapes-icosahedron, octahedron, and truncated octahedron-are explored, and the truncated octahedron is found to be the most active and the icosahedron is the least active. NixPd1-x@Pd NPs with high Ni concentrations and thin shells could exhibit higher ORR rates than the pure Pt(111) surface and/or Pt NPs. AgxPd1-x@Pd in the truncated octahedron shape and high Ag concentrations are predicted to be even more active than NixPd1-x@Pd NPs under the same conditions. The highly active AgxPd1-x@Pd and NixPd1-x@Pd NPs are thermodynamically stable.
引用
收藏
页码:1964 / 1973
页数:10
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