Emergence of Rapid Oxygen Surface Exchange Kinetics during in Situ Crystallization of Mixed Conducting Thin Film Oxides
- Ting ChenTing ChenDepartment of Hydrogen Energy Systems and International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, JapanMore by Ting Chen
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- George F. HarringtonGeorge F. HarringtonInternational Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Next-Generation Fuel Cell Research Center (NEXT-FC) and Center for Co-Evolutional Social Systems, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, JapanDepartment of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United StatesMore by George F. Harrington
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- Juveria MasoodJuveria MasoodDepartment of Materials Science and Engineering, Northwestern University, 2220 Campus Drive, Evanston, Illinois 60208, United StatesMore by Juveria Masood
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- Kazunari SasakiKazunari SasakiDepartment of Hydrogen Energy Systems, International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Next-Generation Fuel Cell Research Center (NEXT-FC) and Center for Co-Evolutional Social Systems, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, JapanMore by Kazunari Sasaki
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- Nicola H. Perry*Nicola H. Perry*E-mail: [email protected]International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, JapanDepartment of Materials Science and Engineering, University of Illinois at Urbana-Champaign, 1304 West Green Street, Urbana, Illinois 61801, United StatesMore by Nicola H. Perry
Abstract
The oxygen surface exchange kinetics of mixed ionic and electronic conducting oxides (MIECs) play a critical role in the efficiency of intermediate-to-high-temperature electrochemical devices. Although there is increasing interest in low-temperature preparation of MIEC thin films, the impact of the resultant varied degrees of crystallinity on the surface exchange kinetics has not been widely investigated. Here, we probe the effect of crystallization on oxygen surface exchange kinetics in situ, by applying an optical transmission relaxation (OTR) approach during annealing of amorphous films. OTR enables contact-free, in situ, and continuous quantification of the oxygen surface exchange coefficient (kchem); we previously applied it to PrxCe1–xO2−δ and SrTi1–xFexO3−δ thin films. In this work, the OTR approach was successfully extended to other mixed conducting thin film compositions for the first time (i.e., perovskite SrTi0.65Co0.35O3−δ and Ruddlesden–Popper Sr2Ti0.65Fe0.35O4±δ), as well as to Pr0.1Ce0.9O2−δ, enabling quantification of the kchem of their native surfaces and comparison of the behavior of films with different final crystal structures. All thin films were prepared by pulsed laser deposition at 25 or 700–800 °C and subject to subsequent thermal treatments with simultaneous OTR monitoring of kchem. The surface roughness, grain size, and crystallinity were evaluated by scanning probe microscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Fluorite Pr0.1Ce0.9O2−δ films grown at 25 °C did not exhibit an increase in kchem after annealing, as they were already crystalline as grown at 25 °C. For all other compositions, OTR enabled in situ observation of both the crystallization process and the emergence of rapid surface exchange kinetics immediately upon crystallization. Perovskite SrTi0.65Co0.35O3-δ and Ruddlesden–Popper Sr2Ti0.65Fe0.35O4±δ thin films grown at 25 °C exhibited at least 1–2 orders of magnitude enhanced kchem after annealing compared with highly crystalline thin films grown at 800 °C, indicating the benefits of in situ crystallization.
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