Hostname: page-component-8448b6f56d-sxzjt Total loading time: 0 Render date: 2024-04-24T00:48:23.285Z Has data issue: false hasContentIssue false
  • English
  • Français

In situ small-angle x-ray scattering analysis of improved catalyst—support interactions through nitrogen modification

Published online by Cambridge University Press:  09 July 2012

Kevin N. Wood ,
Steven T. Christensen ,
Svitlana Pylypenko ,
Tim S. Olson ,
Arrelaine A. Dameron ,
Katherine E. Hurst ,
Huyen N. Dinh ,
Thomas Gennett  and
Ryan O'Hayre
Kevin N. Wood
Affiliation:
Department of Metallurgical & Materials Engineering, Colorado School of Mines, Golden, Colorado 80401
Steven T. Christensen
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Svitlana Pylypenko
Affiliation:
Department of Metallurgical & Materials Engineering, Colorado School of Mines, Golden, Colorado 80401
Tim S. Olson
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Arrelaine A. Dameron
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Katherine E. Hurst
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Huyen N. Dinh
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Thomas Gennett
Affiliation:
National Renewable Energy Laboratory, Golden, Colorado 80401
Ryan O'Hayre*
Affiliation:
Department of Metallurgical & Materials Engineering, Colorado School of Mines, Golden, Colorado 80401
*
Address all correspondence to Ryan O'Hayre atrohayre@mines.edu
Get access

Abstract

In situ small-angle x-ray scattering (SAXS) is used to investigate the electrochemical durability of Pt-Metal (Pt-M) catalysts sputtered onto nitrogen-modified high surface area carbon powder. The results demonstrate that nitrogen modification promotes catalyst durability through reduction of nanoparticle dissolution and coarsening. Although particle sizes of Pt-M on high surface area carbon supports can be difficult to determine with transmission electron microscopy (TEM), a novel SAXS method has been employed to calculate particle size. SAXS analysis shows that the Pt-M nanoparticle size distribution remained stable for 3000 electrochemical cycles after nitrogen modification, whereas the unmodified support material leads to Pt-M nanoparticle instabilities. These results for industrial-relevant catalyst/support architectures underscore the potential of nitrogen-modified carbon support structures for enhanced Pt-M catalyst durability.

Type
Research Letters
Information
MRS Communications , Volume 2 , Issue 3 , September 2012 , pp. 85 - 89
Copyright
Copyright © Materials Research Society 2012

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

1.Xu, X. and Ye, S.: High-temperature fuel cell membranes based on mechanically stable para-ordered polybenzimidazole prepared by direct casting. J. Power Sources 172, 145 (2007).Google Scholar
2.Shyam, B., Arruda, T.M., Murkjee, S., and Ramaker, D.E.: Effect of RuOxHy island size on PtRu particle aging in methanol. J. Phys. Chem. C 113, 19713 (2009).Google Scholar
3.Avasarala, B., Moore, R., and Haldar, P.: Surface oxidation of carbon supports due to potential cycling under PEM fuel cell conditions. Electrochim. Acta 55, 4765 (2010).Google Scholar
4.Choo, H.S., Kinumoto, T., Leong, S.K., Iriyama, Y., Abe, T., and Ogumi, Z.: Mechanism for electrochemical oxidation of highly oriented pyrolytic graphite in sulfuric acid solution. J. Electrochem. Soc. 154, B1017, (2007).Google Scholar
5.Borup, R., Meyers, J., Pivovar, B., Kim, Y.S., Mukundan, R., Garland, N., Myers, D., Wilson, M., Garzon, F., Wood, D., Zelenay, P., More, K., Stroh, K., Zawodzinski, T., Boncella, J., McGrath, J.E., Inaba, M., Miyatake, K., Hori, M., Ota, K., Ogumi, Z., Miyata, S., Nishikata, A., Siroma, Z., Uchimoto, Y., Yasuda, K., Kimijima, K.I., and Iwashita, N.: Scientific aspects of polymer electrolyte fuel cell durability and degradation. Chemical Reviews. 107, 3904 (2007).Google Scholar
6.Ye, S., Vijh, A.K., and Dao, L.H.: A new fuel cell electrocatalyst based on highly porous carbonized polyacrylonitrile foam with very low platinum loading. J. Electrochem. Soc. 143, L7 (1996).Google Scholar
7.Roy, S.C., Christensen, P.A., Hamnett, A., Thomas, K.M., and Trapp, V.: Direct methanol fuel cell cathodes with sulfur and nitrogen-based carbon functionality. J. Electrochem. Soc. 143, 3073 (1996).Google Scholar
8.Zhou, Y.K., Pasquarelli, R., Holme, T., Berry, J., Ginley, D., and O'Hayre, R.: Improving PEM fuel cell catalyst activity and durability using nitrogen-doped carbon supports: observations from model Pt/HOPG systems. J. Mater. Chem. 19, 7830 (2009).CrossRefGoogle Scholar
9.Chen, Y.G., Wang, J.J., Liu, H., Li, R.Y., Sun, X.L., Ye, S., and Knights, S.: Enhanced stability of Pt electrocatalysts by nitrogen doping in CNTs for PEM fuel cells. Electrochem. Commun. 11, 2071 (2009).Google Scholar
10.Maldonado, S. and Stevenson, K.J.: Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes. J. Phys. Chem. B 109, 4707 (2005).Google Scholar
11.Ye, S., Vijh, K.A., and Dao, L.H.: A new fuel cell electrocatalyst based on carbonized polyacrylonitrile foam. J. Electrochem. Soc. 144, 90 (1997).CrossRefGoogle Scholar
12.Maiyalagan, T., Viswanathan, B., and Varadaraju, U.V.: Nitrogen containing carbon nanotubes as supports for Pt – Alternate anodes for fuel cell applications. Electrochem. Comm. 7, 905 (2005).CrossRefGoogle Scholar
13.Holme, T., Zhou, Y.K., Pasquarelli, R., and O'Hayre, R.: First principles study of doped carbon supports for enhanced platinum catalysts. Phys. Chem. Chem. Phys. 12, 9461 (2010).Google Scholar
14.Groves, M.N., Chan, A.S.W., Malardier-Jugroot, C., and Jugroot, M.: Improving platinum catalyst binding energy to graphene through nitrogen doping. Chem. Phys. Lett. 481, 214 (2009).Google Scholar
15.Pylypenko, S., Queen, A., Olson, T.S., Dameron, A., O'Neill, K., Neyerlin, K.C., Pivovar, B., Dinh, H.N., Ginley, D.S., Gennett, T., and O'Hayre, R.: Tuning carbon-based fuel cell catalyst support structures via nitrogen functionalization. I. Investigation of structural and compositional modification of highly oriented pyrolytic graphite model catalyst supports as a function of nitrogen implantation dose. J. Phys. Chem. C 115, 13667 (2011).Google Scholar
16.Pylypenko, S., Queen, A., Olson, T.S., Dameron, A., O'Neill, K., Neyerlin, K.C., Pivovar, B., Dinh, H.N., Ginley, D.S., Gennett, T., and O'Hayre, R.: Tuning carbon-based fuel cell catalyst support structures via nitrogen functionalization. II. Investigation of durability of Pt–Ru nanoparticles supported on highly oriented pyrolytic graphite model catalyst supports as a function of nitrogen implantation dose. J. Phys. Chem. C 115, 13676 (2011).Google Scholar
17.Dameron, A., Olson, T.S., Christensen, S.T., Leisch, J.E., Hurst, K.E., Pylypenko, S., Bult, J.B., Ginley, D.S., O'Hayre, R., Dinh, H.N., and Gennett, T.: Pt–Ru alloyed fuel cell catalysts sputtered from a single alloyed target. ACS Catal. 1, 1307 (2011).Google Scholar
18.Yu, C., Koh, S., Leisch, J., Toney, M., and Strasser, P.: Size and composition distribution dynamics of alloy nanoparticle electrocatalysts probed by anomalous small angle x-ray scattering (ASAXS). Faraday Discuss. 140, 283 (2008).Google ScholarPubMed
19.Yu, C.: Structural dynamics of Pt and Pt alloy nanoparticle probed by x-ray scattering techniques. Ph.D. Thesis, University of Houston, August 2010.Google Scholar
20.Ilavsky, J. and Jemian, P.R.: Irena: tool suite for modeling and analysis of small-angle scattering. J. Appl. Crystallogr. 42, 347 (2009).Google Scholar
21.Allen, A.J., Krueger, S., Skandan, G., Long, G.G., Hahn, H., Kerch, H.M., Parker, J.C., and Ali, M.N.: Microstructural evolution during the sintering of nanostructured ceramic oxides. J. Am. Ceram. Soc. 79, 1201 (1996).CrossRefGoogle Scholar
22.Gontard, L.C., Dunin-Borkowski, R.E., Ozkaya, D., Hyde, T., Midgley, P.A., and Ash, P.: Crystal size and shape analysis of Pt nanoparticles in two and three dimensions. J. Phys. Conf. Ser. 26, 367 (2006).Google Scholar
23.Hyde, T.: Crystallite size analysis of supported platinum catalysts by XRD. Platinum Met. Rev. 52, 129 (2008).Google Scholar
24.Zhou, Y., Neyerlin, K., Olson, T.S., Pylypenko, S., Bult, J., Dinh, H.N., Gennett, T., Shao, Z., and O'Hayre, R.: Enhancement of Pt and Pt-alloy fuel cell catalyst activity and durability via nitrogen-modified carbon supports. Energy Environ. Sci. 3, 1437 (2010).Google Scholar
Supplementary material: File

Wood et al. supplementary material

Supplementary data

Download Wood et al. supplementary material(File)
File 283.6 KB