Density Functional Theory Study of Pt3M Alloy Surface Segregation with Adsorbed O/OH and Pt3Os as Catalysts for Oxygen Reduction Reaction

• DOI: 10.1021/jp507103c
• Publication Date: 2014-10-22T19:23:36Z
• Authors: Ho-Cheng Tsai; Ted H. Yu; Yao Sha; Boris V. Merinov; Pu-Wei Wu; San-Yuan Chen; William A. Goddard
• Keywords: 540; 530; 01 natural sciences; 0104 chemical sciences

Using quantum mechanics calculations, we have studied the segregation energy with adsorbed O and OH for 28 Pt3M alloys, where M is a transition metal. The calculations found surface to become energetically unfavorable Pt3Co Pt3Ni, as well most other Pt binary in presence of OH. However, Pt3Os Pt3Ir remain segregated show best preference among alloys both species on surface. Binding energies various oxygen reduction reaction (ORR) intermediates Pt(111) Pt3Os(111) surfaces were calculated analyzed. Energy barriers different ORR steps computed catalysts, rate-determining (RDS) identified. It turns out that RDS barrier alloy catalyst lower than corresponding pure Pt. This result allows us predict better performance compared