In Situ Ambient Pressure X-ray Photoelectron Spectroscopy of Cobalt Perovskite Surfaces under Cathodic Polarization at High Temperatures
AuthorsCrumlin, Ethan J.
Hong, Wesley T.
Biegalski, Michael D.
Christen, Hans M.
Online Publication Date2013-07-29
Print Publication Date2013-08-08
Permanent link to this recordhttp://hdl.handle.net/10754/598590
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AbstractHeterostructured oxide interfaces have demonstrated enhanced oxygen reduction reaction rates at elevated temperatures (∼500-800 C); however, the physical origin underlying this enhancement is not well understood. By using synchrotron-based in situ ambient pressure X-ray photoelectron spectroscopy (APXPS), we focus on understanding the surface electronic structure, elemental composition, and chemical nature of epitaxial La0.8Sr 0.2CoO3-δ (LSC113), (La 0.5Sr0.5)2CoO4±δ (LSC214), and LSC214-decorated LSC113 (LSC 113/214) thin films as a function of applied electrical potentials (0 to -800 mV) at 520 C and p(O2) of 1 × 10-3 atm. Shifts in the top of the valence band binding energy and changes in the Sr 3d and O 1s spectral components under applied bias reveal key differences among the film chemistries, most notably in the degree of Sr segregation to the surface and quantity of active oxygen sites in the perovskite termination layer. These differences help to identify important factors governing the enhanced activity of oxygen electrocatalysis observed for the LSC113/214 heterostructured surface. © 2013 American Chemical Society.
CitationCrumlin EJ, Mutoro E, Hong WT, Biegalski MD, Christen HM, et al. (2013) In Situ Ambient Pressure X-ray Photoelectron Spectroscopy of Cobalt Perovskite Surfaces under Cathodic Polarization at High Temperatures. The Journal of Physical Chemistry C 117: 16087–16094. Available: http://dx.doi.org/10.1021/jp4051963.
SponsorsThis work was supported in part by DOE (SISGR DE- SC0002633) and King Abdullah University of Science and Technology. E.M. is grateful for financial support from the German Research Foundation (DFG research scholarship). We would like to thank the King Fahd University of Petroleum and Minerals in Dharam, Saudi Arabia, for funding the research reported in this article through the Center for Clean Water and Clean Energy at MIT and KFUPM. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. The PLD preparation performed was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy.
PublisherAmerican Chemical Society (ACS)