TY - JOUR
T1 - Surface compositions of Pt–Pd=Pd(111) alloys in the presence of O and OH during oxygen reduction reaction
T2 - A first-principles study
AU - Chantaramolee, Bhume
AU - Aspera, Susan Meñez
AU - Arevalo, Ryan Lacdao
AU - Arguelles, Elvis Flaviano
AU - Kishida, Ryo
AU - Padama, Allan Abraham Bustria
AU - Kasai, Hideaki
AU - Nakanishi, Hiroshi
N1 - Funding Information:
Acknowledgments This work is supported in part by Tanaka Kikinzoku Kogyo K.K., JST ACCEL grant number JPMJAC1501 “Creation of the Functional Materials on the Basis of the Inter-Element-Fusion Strategy and their Innovative Applications”, MEXT Grant-in-Aid for Scientific Research (16K04876), JST CREST Innovative Catalysts and Creation Technologies for the Utilization of Diverse Natural Carbon Resources: In-situ atomic characterization of catalytic reactions for the development of InnovativeCatalysts (No. 17942262), the GREEN POWER PROGRAM of the Commission on Higher Education-Philippine California Advanced Research Institutes (CHED-PCARI) (IIID-2015-09) and the University of the Philippines Emerging Interdisciplinary Research (EIDR) Program (C08-003). Susan Meñez Aspera would like to acknowledge Kansai Research Foundation for their support. Some of the numerical calculations presented here were done using the computer facilities at the following institutes: High Energy Accelerator Research Organization (KEK), Institute for Solid State Physics (ISSP, University of Tokyo), Yukawa Institute for Theoretical Physics (YITP, Kyoto University), and the National Institute for Fusion Science (NIFS).
Publisher Copyright:
©2019 The Physical Society of Japan
PY - 2019
Y1 - 2019
N2 - The surface stability and compositions of catalysts under varied conditions play an important role in its activity and selectivity toward various reactions. In this paper, density functional theory based first principles calculations were used to investigate the stability and compositions of the first two layers of Pt–Pd alloys on Pd substrate under the electrode-potential dependent oxygen reduction conditions. The adsorption of O and OH have different preference surface compositions of Pt: Pd 50: 50 and Pt: Pd 0: 100, respectively. However, at high electrode potential, it is found that O should be dominant adsorbate on the surface. Therefore, the surface composition should favor the Pt: Pd 50: 50. Moreover, this oxygen covered surface is characterized by weakened surface Pt–Pt bonds, which is attributed to the increase in the population of the Pt–Pt antibonding state. These findings support the experimentally observed Pd segregation from the as-prepared Pt=Pd(111) to the composition of Pt: Pd ¼ 60: 40 during ORR.
AB - The surface stability and compositions of catalysts under varied conditions play an important role in its activity and selectivity toward various reactions. In this paper, density functional theory based first principles calculations were used to investigate the stability and compositions of the first two layers of Pt–Pd alloys on Pd substrate under the electrode-potential dependent oxygen reduction conditions. The adsorption of O and OH have different preference surface compositions of Pt: Pd 50: 50 and Pt: Pd 0: 100, respectively. However, at high electrode potential, it is found that O should be dominant adsorbate on the surface. Therefore, the surface composition should favor the Pt: Pd 50: 50. Moreover, this oxygen covered surface is characterized by weakened surface Pt–Pt bonds, which is attributed to the increase in the population of the Pt–Pt antibonding state. These findings support the experimentally observed Pd segregation from the as-prepared Pt=Pd(111) to the composition of Pt: Pd ¼ 60: 40 during ORR.
UR - http://www.scopus.com/inward/record.url?scp=85067255857&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85067255857&partnerID=8YFLogxK
U2 - 10.7566/JPSJ.88.044802
DO - 10.7566/JPSJ.88.044802
M3 - Article
AN - SCOPUS:85067255857
SN - 0031-9015
VL - 88
JO - journal of the physical society of japan
JF - journal of the physical society of japan
IS - 4
M1 - 044802
ER -