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Combinatorial Synthesis and Reactivity Screening of Electro-Oxidation Catalyst Gradients

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Abstract

Combinatorial methods represent an appealing experimental method for the discovery of heterogeneous catalysts. One can efficiently identify candidate materials or sample vast regions of composition space using a combination of dense catalyst libraries and high-throughput reactivity screening techniques. This is particularly appealing for the discovery of novel catalysts for low temperature fuel cells where multi-component systems have shown improved performance. For example, the poison tolerance of typical anode catalysts can be improved by the addition of oxophilic components such as ruthenium, molybdenum, tin or osmium. Consequently, a vast composition space must be sampled in order to identify catalyst compositions or regions of composition space with greater activity. Combinatorial methods represent a practical means to speed-up the catalyst discovery process. In this manuscript, we demonstrate a novel method for combinatorial catalyst discovery based upon the synthesis and reactivity mapping of catalyst composition gradients. Samples consisting of uniform variations in surface composition of metals catalysts (Pt-M1 and Pt-M1-M2, where M1 M2 = Ru, Mo, Sn or Os) are fabricated using a gel-transfer technique. A concentration gradient of source metal ions is produced in a swollen polymer gel and then transferred onto a surface by electrodeposition to create a continuous composition gradient. An in situ reactivity-mapping tool based on the scanning electrochemical microscope is used to interrogate these catalyst gradients for the hydrogen oxidation reaction in the presence of adsorbed carbon monoxide.

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Acknowledgements

The authors thank the Office of Naval Research for a Young Investigator Award, the National Science Foundation for a CAREER Award, the Camille and Henry Dreyfus Foundation for a New Faculty Award, and the Donors of The Petroleum Research Fund as administered by the American Chemical Society, for partial support of this research.

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Authors and Affiliations

  1. Department of Chemical Engineering, Department of Chemistry, Institute of Combinatorial Discovery, Iowa State University, Ames, IA, 50011, USA

    Shrisudersan Jayaraman & Andrew C. Hillier

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  1. Shrisudersan Jayaraman
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  2. Andrew C. Hillier
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Jayaraman, S., Hillier, A.C. Combinatorial Synthesis and Reactivity Screening of Electro-Oxidation Catalyst Gradients. MRS Online Proceedings Library 804, 239–247 (2003). https://doi.org/10.1557/PROC-804-JJ8.11

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