Controlling topotactic phase transitions in oxide thin films
EMSL Project ID
49597
Abstract
The objective of this research is to understand, predict, and control the phase transitions occurring in structurally ordered thin films to enable the rational design, synthesis, and utilization of such materials. Transition metal oxides (TMOs) with ordered vacant lattice sites enable easy electron and ion intercalation reactions and thus have been extensively investigated for energy conversion and storage applications, particularly for use as mixed electronic/ionic conductors, electrocatalysts, and electrodes in batteries and fuel cells. However, phase transitions are often observed when intercalation reactions take place, causing drastic changes in physical properties and device performance. We will use the unique toolset available at EMSL to establish well-defined structure-stability-function relationships. The combination of highly controlled synthesis by molecular beam epitaxy and in situ/in operando structural and chemical imaging by advanced transmission electron microscopies, with guidance from theoretical simulations, will allow us to reveal, verify, and eventually control the transport dynamics, intermediate states, phase transition trajectories, and reaction outcomes. This project is well aligned with EMSL's "Molecular Transformations" thrust of investigating the "dynamic transformation mechanisms and physical and chemical properties at critical interfaces in catalysts and energy materials needed to design new materials and systems for sustainable energy applications," and will lead to the discovery and design of more robust functional materials.
Project Details
Project type
Exploratory Research
Start Date
2016-10-26
End Date
2017-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Guo L., Z. Yang, K. Marcus, Z. Li, B. Luo, L. Zhou, and X. Wang, et al. 2018. "MoS2/TiO2 Heterostructures as Nonmetal Plasmonic Photocatalysts for Highly Efficient Hydrogen Evolution." Energy & Environmental Science 11, no. 1:106-114. PNNL-SA-129523. doi:10.1039/C7EE02464A
Guo L, Z Yang, K Marcus, Z Li, B Luo, L Zhou, X Wang, Y Du, and Y Yang. 2017. "MoS2/TiO2 Heterostructures as Nonmetal Plasmonic Photocatalysts for Highly Efficient Hydrogen Evolution†." Energy & Environmental Science 11:106-114.
Liang K, L Guo, K Marcus, S Zhang, Z Yang, DE Perea, L Zhou, Y Du, and Y Yang. 2017. "Overall Water Splitting with Room-Temperature Synthesized NiFe Oxyfluoride Nanoporous Films." ACS Catalysis 7(12):8406-8412. doi:10.1021/acscatal.7b02991
Li X., K. Zhang, Z. Yang, M. Wang, Y. Tang, J. Fei, and Y. Du, et al. 2018. "Fundamental Insight into Zr Modification of Li- and Mn-Rich Cathodes: Combined Transmission Eelctron Microscopy and Electrochemical Impedance Spectroscopy Study." Chemistry of Materials 30, no. 8:2566-2573. PNNL-SA-130227. doi:10.1021/acs.chemmater.7b04861
Ong P., Y. Du, and P.V. Sushko. 2017. "Low Dimensional Oxygen Vacancy Ordering and Diusion in SrCrO3-d." Journal of Physical Chemistry Letters 8, no. 8:1757-1763. PNNL-SA-123934. doi:10.1021/acs.jpclett.7b00355