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Synthesis of Platinum-nickel Nanowires and Optimization for Oxygen Reduction Performance
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First principles based mean field model for oxygen reduction reaction.

Ryosuke Jinnouchi1, Kensaku Kodama, Tatsuya Hatanaka

  • 1Toyota Central R&D Labs., Inc., 41-1 Yokomichi Nagakute, Aichi, 480-1192, Japan. e1262@mosk.tytlabs.co.jp

Physical Chemistry Chemical Physics : PCCP
|November 9, 2011
PubMed
Summary

A new model explains the oxygen reduction reaction (ORR) on platinum catalysts. It reveals how catalyst structure and oxygen levels affect reaction pathways and activity, crucial for fuel cell performance.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Computational Chemistry

Background:

  • The oxygen reduction reaction (ORR) is critical for fuel cell efficiency.
  • Understanding ORR mechanisms on platinum-based catalysts is essential for catalyst design.
  • Previous models often simplified the complex surface interactions involved in ORR.

Purpose of the Study:

  • To develop a first-principles-based mean field model for the ORR.
  • To investigate the influence of surface coverage and material properties on ORR kinetics.
  • To simulate ORR on various platinum (Pt) catalyst surfaces.

Main Methods:

  • Developed a mean field model incorporating coverage- and material-dependent reversible potentials.
  • Applied the model to simulate single crystal surfaces of Pt, Pt alloys, and Pt core-shell catalysts.
  • Validated model predictions against existing experimental and theoretical ORR data.

Main Results:

  • Model results align with experimental data for surface coverages, current-voltage curves on Pt(111), and material-dependent activity.
  • Identified the oxygen associative pathway with HO(2)(ads) formation as dominant on Pt(111).
  • Determined the O(ads) removal step as the rate-determining step (RDS) on Pt(111), which is accelerated in alloys and core-shell structures.

Conclusions:

  • The model elucidates the interrelation between ORR pathway, RDS, surface coverages, Tafel slope, reaction order, and material activity.
  • Catalyst modifications in alloys and core-shell structures accelerate the RDS, reducing reaction intermediates.
  • Increased oxygen partial pressure leads to higher surface coverages, reducing the apparent reaction order to below unity.