A Multi-electrode Electrochemical and Scanning Differential Electrochemical Mass Spectrometry Study of Methanol Oxidation on Electrodeposited PtxRuy

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Jambunathan, K.
Jayaraman, S.
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Hillier, Andrew
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Chemical and Biological Engineering

The function of the Department of Chemical and Biological Engineering has been to prepare students for the study and application of chemistry in industry. This focus has included preparation for employment in various industries as well as the development, design, and operation of equipment and processes within industry.Through the CBE Department, Iowa State University is nationally recognized for its initiatives in bioinformatics, biomaterials, bioproducts, metabolic/tissue engineering, multiphase computational fluid dynamics, advanced polymeric materials and nanostructured materials.

The Department of Chemical Engineering was founded in 1913 under the Department of Physics and Illuminating Engineering. From 1915 to 1931 it was jointly administered by the Divisions of Industrial Science and Engineering, and from 1931 onward it has been under the Division/College of Engineering. In 1928 it merged with Mining Engineering, and from 1973–1979 it merged with Nuclear Engineering. It became Chemical and Biological Engineering in 2005.

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  • Department of Chemical Engineering (1913–1928)
  • Department of Chemical and Mining Engineering (1928–1957)
  • Department of Chemical Engineering (1957–1973, 1979–2005)
    • Department of Chemical and Biological Engineering (2005–present)

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Methanol electro-oxidation was studied on a series of electrodeposited PtxRuy catalysts constructed as multielement band electrodes. A combination of electrochemical and scanning differential electrochemical mass spectrometry measurements were performed to evaluate the composition-dependence of methanol oxidation, methanol decomposition, CO2 current efficiency, and the product distribution at 25 and 50 °C. At 25 °C, cyclic voltammetry revealed that the presence of Ru led to enhanced methanol oxidation rates over that of pure Pt. Methanol decomposition showed a similar composition-dependence. Mass spectrometry measurements revealed the evolution of HCOOH and CO2 during methanol oxidation and allowed indirect determination of H2CO produced. Notably, these products were not observed during methanol decomposition. The most active electrode compositions and the highest instantaneous current efficiencies for the formation of CO2 were found to depend on several factors. At 25 °C, the maximum activity was 10% Ru, while at 50 °C the most active composition increased to 25% Ru. Pure Pt had the highest instantaneous current efficiency for CO2 at both temperatures. The product distribution reflected high CO2 evolution for Pt, with an increasing fraction of the product emerging as H2CO at higher Ru content. Increasing the temperature improved the CO2 current efficiency for all electrode compositions. These results confirm that methanol oxidation occurs though a parallel reaction pathway on PtxRuy electrodes. In addition, the balance between the different reaction pathways depends on several factors, including Ru composition and temperature.


This article is from Langmuir20 (2004): 1856-1863, doi: 10.1021/la035567i. Posted with permission.

Thu Jan 01 00:00:00 UTC 2004