DFT Study of Oxygen Reduction Reaction on Pt-Zr Catalysts

Wednesday, 8 October 2014: 11:20
Expo Center, 1st Floor, Universal 14 (Moon Palace Resort)
B. V. Merinov, H. C. Tsai (California Institute of Technology), T. H. Yu (California State University, Long Beach), and W. A. Goddard III (California Institute of Technology)
The sluggish oxygen reduction reaction (ORR) kinetics at cathode and expensive Pt electrocatalysts are two main issues that retard fuel cell technology commercialization.1-3 To overcome these problems, alloying Pt with transition metals, core-shell structures, and non-Pt catalysts are applied to improve the catalytic activity and reduce the catalyst cost.4-8 It was found that Pt3Ni, Pt3Co, and Pt3Fe have better activity than pure Pt.9-11 However, stability of these alloys needs to be improved. Pt3Zr, Pt3Y, Pt3Sc show greater stability and high catalytic activity,9,10,12but these materials need further experimental and theoretical investigations.

We used DFT calculations to study the origins of the better ORR performance and greater stability of Pt-Zr catalysts. To accurately evaluate the activity of Pt-Zr catalysts, we examined binding energies of ORR intermediates and reaction energy barriers for ORR steps both in gas phase and solution. Based on the results obtained, ORR mechanisms on Pt-Zr catalysts will be considered and compared to pure Pt and Pt alloys. Some related experimental results will be discussed as well.

 Acknowledgement. This work is financially supported by the National Science Foundation (grant CBET-1067848).


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