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Density Functional Theory Study of Pt_3M Alloy Surface Segregation with Adsorbed O/OH and Pt_3Os as Catalysts for Oxygen Reduction Reaction

Tsai, Ho-Cheng and Yu, Ted H. and Sha, Yao and Merinov, Boris V. and Wu, Pu-Wei and Chen, San-Yuan and Goddard, William A., III (2014) Density Functional Theory Study of Pt_3M Alloy Surface Segregation with Adsorbed O/OH and Pt_3Os as Catalysts for Oxygen Reduction Reaction. Journal of Physical Chemistry C, 118 (46). pp. 26703-26712. ISSN 1932-7447. https://resolver.caltech.edu/CaltechAUTHORS:20141110-134852748

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Abstract

Using quantum mechanics calculations, we have studied the segregation energy with adsorbed O and OH for 28 Pt_3M alloys, where M is a transition metal. The calculations found surface segregation to become energetically unfavorable for Pt_3Co and Pt_3Ni, as well as for the most other Pt binary alloys, in the presence of adsorbed O and OH. However, Pt_3Os and Pt_3Ir remain surface segregated and show the best energy preference among the alloys studied for both adsorbed species on the surface. Binding energies of various oxygen reduction reaction (ORR) intermediates on the Pt(111) and Pt_3Os(111) surfaces were calculated and analyzed. Energy barriers for different ORR steps were computed for Pt and Pt_3Os catalysts, and the rate-determining steps (RDS) were identified. It turns out that the RDS barrier for the Pt_3Os alloy catalyst is lower than the corresponding barrier for pure Pt. This result allows us to predict a better ORR performance of Pt_3Os compared to that of pure Pt.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://pubs.acs.org/doi/abs/10.1021/jp507103cPublisherArticle
http://dx.doi.org/10.1021/jp507103cDOIArticle
http://pubs.acs.org/doi/suppl/10.1021/jp507103cRelated ItemSupporting Information
ORCID:
AuthorORCID
Yu, Ted H.0000-0003-3202-0981
Merinov, Boris V.0000-0002-2783-4262
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Density Functional Theory Study of Pt3M Alloy Surface Segregation with Adsorbed O/OH and Pt3Os as Catalysts for Oxygen Reduction Reaction
Additional Information:© 2014 American Chemical Society. Received: July 16, 2014; Revised: October 15, 2014; Published: October 22, 2014. This work was supported by the National Science Foundation (Grant CBET-1067848, Caltech) and the Caltech and Taiwan Energy Exchange (CTEE) collaborative program funded by the National Science Council of Taiwan (Grant NSC 103-3113-P-008-001). The facilities of the Materials and Process Simulation Center used in this study were established with grants from DURIP-ONR, DURIP-ARO and NSF-CSEM.
Funders:
Funding AgencyGrant Number
NSFCBET-1067848
National Science Council (Taipei)NSC 101-3113-P-008-001
Office of Naval Research (ONR)UNSPECIFIED
Army Research Office (ARO)UNSPECIFIED
Issue or Number:46
Record Number:CaltechAUTHORS:20141110-134852748
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20141110-134852748
Official Citation:Density Functional Theory Study of Pt3M Alloy Surface Segregation with Adsorbed O/OH and Pt3Os as Catalysts for Oxygen Reduction Reaction Ho-Cheng Tsai, Ted H. Yu, Yao Sha, Boris V. Merinov, Pu-Wei Wu, San-Yuan Chen, and William A. Goddard, III The Journal of Physical Chemistry C 2014 118 (46), 26703-26712
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:51526
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:11 Nov 2014 00:33
Last Modified:03 Oct 2019 07:33

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