Authors

S. Stolbov;M. A. Ortigoza

Comments

Authors: contact us about adding a copy of your work at [email protected]

Abbreviated Journal Title

J. Chem. Phys.

Keywords

PLATINUM-MONOLAYER ELECTROCATALYSTS; HYDROGEN FUEL-CELLS; CARBON-MONOXIDE; SURFACE ALLOYS; METAL-SURFACES; NANOPARTICLES; PERFORMANCE; DISSOLUTION; CATALYSTS; HYBRIDS; Physics, Atomic, Molecular & Chemical

Abstract

In addressing the growing need of renewable and sustainable energy resources, hydrogen-fuel-cells stand as one of the most promising routes to transform the current energy paradigm into one that integrally fulfills environmental sustainability. Nevertheless, accomplishing this technology at a large scale demands to surpass the efficiency and enhance the cost-effectiveness of platinum-based cathodes, which catalyze the oxygen reduction reaction (ORR). In this work, our first-principles calculations show that Au atoms incorporated into graphene di-vacancies form a highly stable and cost-effective electrocatalyst that is, at the same time, as or more (dependently of the dopant concentration) active toward ORR than the best-known Pt-based electrocatalysts. We reveal that partial passivation of defected-graphene by gold atoms reduces the reactivity of C dangling bonds and increases that of Au, thus optimizing them for catalyzing the ORR and yielding a system of high thermodynamic and electrochemical stabilities. We also demonstrate that the linear relation among the binding energies of the reaction intermediates assumed in computational high-throughput material screening does not hold, at least for this non-purely transition-metal material. We expect Au-doped graphene to finally overcome the cathode-related challenge hindering the realization of hydrogen-fuel cells as the leading means of powering transportation and portable devices.

Journal Title

Journal of Chemical Physics

Volume

142

Issue/Number

15

Publication Date

1-1-2015

Document Type

Article

Language

English

First Page

9

WOS Identifier

WOS:000353307700043

ISSN

0021-9606

Download

Share

COinS
 

Accessibility Statement

This item was created or digitized prior to April 24, 2027, or is a reproduction of legacy media created before that date. It is preserved in its original, unmodified state specifically for research, reference, or historical recordkeeping. In accordance with the ADA Title II Final Rule, the University Libraries provides accessible versions of archival materials upon request. To request an accommodation for this item, please submit an accessibility request form.