Gold-doped graphene as a cost-effective, highly stable and active electrocatalyst for the oxygen reduction reaction: prediction from first principles

One of the main obstacles hindering large scale practical application of hydrogen fuel cells is a prohibited cost of the Pt (or Pt-based) catalysts for the oxygen reduction reaction (ORR) on the fuel cell cathode. In this work, we consider Au-doped graphene as an alternative to Pt for facilitating ORR. Our first-principles calculations show that Au atoms incorporated into graphene di-vacancies form a thermodynamically and electrochemically stable structure. Furthermore, calculation of the binding energies of the ORR intermediates reveals that Au-C bonding makes the C atoms neighboring to Au optimally reactive for ORR. The calculated ORR free energy diagrams suggest that the Au-graphene structures have an ORR onset potential as high as that of Pt. We also demonstrate that the linear relation among the binding energy of the reaction intermediates assumed in a number of works on computational high-throughput material screening does not hold, at least for this none purely transition-metal material.