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Mesostructured thin films as electrocatalysts with tunable composition and surface morphology

Nature Materials volume 11, pages 10511058 (2012) | Download Citation

Abstract

Among the most challenging issues in technologies for electrochemical energy conversion are the insufficient activity of the catalysts for the oxygen reduction reaction, catalyst degradation and carbon-support corrosion. In an effort to address these barriers, we aimed towards carbon-free multi/bimetallic materials in the form of mesostructured thin films with tailored physical properties. We present here a new class of metallic materials with tunable near-surface composition, morphology and structure that have led to greatly improved affinity for the electrochemical reduction of oxygen. The level of activity for the oxygen reduction reaction established on mesostructured thin-film catalysts exceeds the highest value reported for bulk polycrystalline Pt bimetallic alloys, and is 20-fold more active than the present state-of-the-art Pt/C nanoscale catalyst.

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Acknowledgements

The research was conducted at Argonne National Laboratory, which is a US Department of Energy Office of Science Laboratory operated by UChicago Argonne, LLC under contract no. DE-AC02-06CH11357. The portion of work related to extended single-crystalline and thin-film surfaces was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. The portion of work exploring practical thin-film-based electrocatalysts was supported by the Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Program. The authors thank Hitachi High Technologies America for the access to high-resolution electron microscopy facilities and J. Pearson and A. P. Paulikas for supporting thin film deposition experiments. V.R.S. is grateful to S. D. Bader and G.W. Crabtree for productive discussions.

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Author notes

    • Dennis F. van der Vliet
    •  & Chao Wang

    These authors contributed equally to this work

Affiliations

  1. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA

    • Dennis F. van der Vliet
    • , Chao Wang
    • , Dusan Tripkovic
    • , Dusan Strmcnik
    • , Nenad M. Markovic
    •  & Vojislav R. Stamenkovic
  2. Hitachi High Technologies America, Pleasanton, California 94588, USA

    • Xiao Feng Zhang
  3. Fuel Cell Components Program, 3M, St Paul, Minnesota 55144, USA

    • Mark K. Debe
    •  & Radoslav T. Atanasoski

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Contributions

D.F.V., C.W. and V.R.S. designed the experiments. C.W., D.F.V., D.T., D.S., X.F.Z., R.T.A., M.K.D. and V.R.S. carried out the experimental work. D.F.V., C.W., M.K.D., N.M.M. and V.R.S. discussed the results and V.R.S. wrote the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to Dennis F. van der Vliet or Chao Wang or Vojislav R. Stamenkovic.

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DOI

https://doi.org/10.1038/nmat3457

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