Hostname: page-component-cd9895bd7-p9bg8 Total loading time: 0 Render date: 2024-12-23T12:27:54.440Z Has data issue: false hasContentIssue false

Optical Fluorescence Microscopy for Spatially Characterizing Electron Transfer across a Solid-Liquid Interface on Heterogeneous Electrodes

Published online by Cambridge University Press:  28 April 2016

Eric Choudhary*
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
Jeyavel Velmurugan
Affiliation:
Maryland NanoCenter, University of Maryland, College Park, MD 20742, U.S.A.
James M. Marr
Affiliation:
Maryland NanoCenter, University of Maryland, College Park, MD 20742, U.S.A.
James A. Liddle
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
Veronika Szalai
Affiliation:
Center for Nanoscale Science and Technology, National Institute of Standards and Technology 100 Bureau Dr, Gaithersburg, MD 20899, U.S.A.
*
Get access

Abstract

Heterogeneous catalytic materials and electrodes are used for (electro)chemical transformations, including those important for energy storage and utilization.1, 2 Due to the heterogeneous nature of these materials, activity measurements with sufficient spatial resolution are needed to obtain structure/activity correlations across the different surface features (exposed facets, step edges, lattice defects, grain boundaries, etc.). These measurements will help lead to an understanding of the underlying reaction mechanisms and enable engineering of more active materials. Because (electro)catalytic surfaces restructure with changing environments,1 it is important to perform measurements in operando. Sub-diffraction fluorescence microscopy is well suited for these requirements because it can operate in solution with resolution down to a few nm. We have applied sub-diffraction fluorescence microscopy to a thin cell containing an electrocatalyst and a solution containing the redox sensitive dye p-aminophenyl fluorescein to characterize reaction at the solid-liquid interface. Our chosen dye switches between a nonfluorescent reduced state and a one-electron oxidized bright state, a process that occurs at the electrode surface. This scheme is used to investigate the activity differences on the surface of polycrystalline Pt, in particular to differentiate reactivity at grain faces and grain boundaries. Ultimately, this method will be extended to study other dye systems and electrode materials.

Type
Articles
Copyright
Copyright © Materials Research Society 2016 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

Marković, N. M. and Ross, P. N. Jr, Surface, Science Reports 45 (4–6), 117229 (2002).Google Scholar
Bard, A. J., Journal of the American Chemical Society 132 (22), 75597567 (2010).Google Scholar
Ronge, J., Bosserez, T., Martel, D., Nervi, C., Boarino, L., Taulelle, F., Decher, G., Bordiga, S. and Martens, J. A., Chemical Society Reviews 43 (23), 79637981 (2014).Google Scholar
Taylor, H. S., Proceedings of the Royal Society of London A: Mathematical, Physical and Engineering Sciences 108 (745), 105111 (1925).Google Scholar
Lee, S. W., Chen, S., Suntivich, J., Sasaki, K., Adzic, R. R. and Shao-Horn, Y., The Journal of Physical Chemistry Letters 1 (9), 13161320 (2010).Google Scholar
Lee, I., Morales, R., Albiter, M. A. and Zaera, F., Proceedings of the National Academy of Sciences of the United States of America 105 (40), 1524115246 (2008).Google Scholar
Joyner, R. W., in Catalysis: Volume 5, edited by Bond, G. C. and Webb, G. (The Royal Society of Chemistry, 1982), Vol. 5, pp. 147.Google Scholar
Mostafa, S., Behafarid, F., Croy, J. R., Ono, L. K., Li, L., Yang, J. C., Frenkel, A. I. and Cuenya, B. R., Journal of the American Chemical Society 132 (44), 1571415719 (2010).CrossRefGoogle Scholar
Vaarkamp, M., Miller, J. T., Modica, F. S. and Koningsberger, D. C., Journal of Catalysis 163 (2), 294305 (1996).Google Scholar
Sambur, J. B. and Chen, P., Annual Review of Physical Chemistry 65, 395422 (2014).Google Scholar
Sambur, J. B., Chen, T.-Y., Choudhary, E., Chen, G., Nissen, E. J., Thomas, E. M., Zou, N. and Chen, P., Nature 530 (7588), 77-80 (2016).Google Scholar
Pastrana, E., Nat Meth 8 (1), 4646 (2011).Google Scholar
Sutter, E. A. and Sutter, P. W., Journal of the American Chemical Society 136 (48), 1686516870 (2014).CrossRefGoogle Scholar
de Jonge, N and Ross, F. M., Nat Nano 6 (11), 695704 (2011).CrossRefGoogle Scholar
Landau, M. V., Vidruk, R., Vingurt, D., Fuks, D. and Herskowitz, M., Reviews in Chemical Engineering 30 (4) (2014).Google Scholar
Thompson, R. E., Larson, D. R. and Webb, W. W., Biophysical Journal 82 (5), 27752783 (2002).CrossRefGoogle Scholar
Chen, P., Zhou, X., Andoy, N. M., Han, K.-S., Choudhary, E., Zou, N., Chen, G. and Shen, H., Chemistry Society Reviews 43, 1107 (2014).Google Scholar
Nørskov, J. K., Rossmeisl, J., Logadottir, A., Lindqvist, L., Kitchin, J. R., Bligaard, T. and Jónsson, H., The Journal of Physical Chemistry B 108 (46), 1788617892 (2004).Google Scholar
Hod, I., Bury, W., Gardner, D. M., Deria, P., Roznyatovskiy, V., Wasielewski, M. R., Farha, O. K. and Hupp, J. T., The Journal of Physical Chemistry Letters 6 (4), 586591 (2015).CrossRefGoogle Scholar