Investigation of Rh-titanate (ATiO3) interactions on high-surface-area perovskite thin films prepared by atomic layer deposition

Chao Lin; Alexandre C. Foucher; Yichen Ji; Eric A. Stach; Raymond J. Gorte

doi:10.1039/d0ta05981a

Investigation of Rh-titanate (ATiO₃) interactions on high-surface-area perovskite thin films prepared by atomic layer deposition

Chao Lin, Alexandre C. Foucher, Yichen Ji, Eric A. Stach, Raymond J. Gorte

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Abstract

Thin, ∼1 nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and studied as catalyst supports for Rh. Scanning Transmission Electron Microcopy (STEM) and X-Ray Diffraction (XRD) demonstrated that the films had the perovskite structure and formed uniform coatings stable up to 1073 K. Rh, added by ALD, interacted strongly with CaTiO3 and somewhat less strongly with SrTiO3, while Rh on BaTiO3 was similar to Rh on unmodified MgAl2O4. STEM measurements of Rh on CaTiO3 films showed Rh remained well dispersed after repeated oxidations and reductions at 1073 K; however, the Rh was inactive for CO-oxidation. Rh formed small particles on SrTiO3 films and was active for CO oxidation after reduction at 1073 K. The reducibility and catalytic activity of Rh/BaTiO3/MgAl2O4 were similar to that of Rh/MgAl2O4. Evidence from CO-TPR, FTIR, and XPS all indicated that the degree of interaction between Rh and the three perovskite films can be ranked in the following order: Rh/CaTiO3/MgAl2O4 > Rh/SrTiO3/MgAl2O4 > Rh/BaTiO3/MgAl2O4. Bulk ex-solution catalysts, synthesized by reduction of ATi0.98Rh0.02O3 (A = Ca, Sr, and Ba), were also examined for comparison.

Original language	English
Pages (from-to)	16973-16984
Number of pages	12
Journal	Journal of Materials Chemistry A
Volume	8
Issue number	33
DOIs	https://doi.org/10.1039/d0ta05981a
State	Published - Sep 7 2020
Externally published	Yes

Funding

Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, grant no. DE-FG02-13ER16380. C. L. and R. J. G. are grateful to the Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, Grant No. DE-FG02-13ER16380 for support of this work. A. C. F. and E. A. S. acknowledge support from the Vagelos Institute for Energy Science and Technology through a graduate fellowship to A. C. F. Electron microscopy was carried out at the Singh Center for Nanotechnology at the University of Pennsylvania which is supported by the National Science Foundation (NSF) National Nanotechnology Coordinated Infrastructure Program grant NNCI-1542153, with additional support from the University of Pennsylvania Materials Research Science and Engineering Center (MRSEC) grant supported by the National Science Foundation (DMR-1720530).

Funders	Funder number
University of Pennsylvania Materials Research Science and Engineering Center
Vagelos Institute for Energy Science and Technology
National Science Foundation	NNCI-1542153
U.S. Department of Energy
Basic Energy Sciences
Materials Research Science and Engineering Center, Harvard University	DMR-1720530
Chemical Sciences, Geosciences, and Biosciences Division	DE-FG02-13ER16380

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10.1039/d0ta05981a

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title = "Investigation of Rh-titanate (ATiO3) interactions on high-surface-area perovskite thin films prepared by atomic layer deposition",

abstract = "Thin, ∼1 nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and studied as catalyst supports for Rh. Scanning Transmission Electron Microcopy (STEM) and X-Ray Diffraction (XRD) demonstrated that the films had the perovskite structure and formed uniform coatings stable up to 1073 K. Rh, added by ALD, interacted strongly with CaTiO3 and somewhat less strongly with SrTiO3, while Rh on BaTiO3 was similar to Rh on unmodified MgAl2O4. STEM measurements of Rh on CaTiO3 films showed Rh remained well dispersed after repeated oxidations and reductions at 1073 K; however, the Rh was inactive for CO-oxidation. Rh formed small particles on SrTiO3 films and was active for CO oxidation after reduction at 1073 K. The reducibility and catalytic activity of Rh/BaTiO3/MgAl2O4 were similar to that of Rh/MgAl2O4. Evidence from CO-TPR, FTIR, and XPS all indicated that the degree of interaction between Rh and the three perovskite films can be ranked in the following order: Rh/CaTiO3/MgAl2O4 > Rh/SrTiO3/MgAl2O4 > Rh/BaTiO3/MgAl2O4. Bulk ex-solution catalysts, synthesized by reduction of ATi0.98Rh0.02O3 (A = Ca, Sr, and Ba), were also examined for comparison.",

author = "Chao Lin and Foucher, {Alexandre C.} and Yichen Ji and Stach, {Eric A.} and Gorte, {Raymond J.}",

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AU - Lin, Chao

AU - Foucher, Alexandre C.

AU - Ji, Yichen

AU - Stach, Eric A.

AU - Gorte, Raymond J.

PY - 2020/9/7

Y1 - 2020/9/7

N2 - Thin, ∼1 nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and studied as catalyst supports for Rh. Scanning Transmission Electron Microcopy (STEM) and X-Ray Diffraction (XRD) demonstrated that the films had the perovskite structure and formed uniform coatings stable up to 1073 K. Rh, added by ALD, interacted strongly with CaTiO3 and somewhat less strongly with SrTiO3, while Rh on BaTiO3 was similar to Rh on unmodified MgAl2O4. STEM measurements of Rh on CaTiO3 films showed Rh remained well dispersed after repeated oxidations and reductions at 1073 K; however, the Rh was inactive for CO-oxidation. Rh formed small particles on SrTiO3 films and was active for CO oxidation after reduction at 1073 K. The reducibility and catalytic activity of Rh/BaTiO3/MgAl2O4 were similar to that of Rh/MgAl2O4. Evidence from CO-TPR, FTIR, and XPS all indicated that the degree of interaction between Rh and the three perovskite films can be ranked in the following order: Rh/CaTiO3/MgAl2O4 > Rh/SrTiO3/MgAl2O4 > Rh/BaTiO3/MgAl2O4. Bulk ex-solution catalysts, synthesized by reduction of ATi0.98Rh0.02O3 (A = Ca, Sr, and Ba), were also examined for comparison.

AB - Thin, ∼1 nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and studied as catalyst supports for Rh. Scanning Transmission Electron Microcopy (STEM) and X-Ray Diffraction (XRD) demonstrated that the films had the perovskite structure and formed uniform coatings stable up to 1073 K. Rh, added by ALD, interacted strongly with CaTiO3 and somewhat less strongly with SrTiO3, while Rh on BaTiO3 was similar to Rh on unmodified MgAl2O4. STEM measurements of Rh on CaTiO3 films showed Rh remained well dispersed after repeated oxidations and reductions at 1073 K; however, the Rh was inactive for CO-oxidation. Rh formed small particles on SrTiO3 films and was active for CO oxidation after reduction at 1073 K. The reducibility and catalytic activity of Rh/BaTiO3/MgAl2O4 were similar to that of Rh/MgAl2O4. Evidence from CO-TPR, FTIR, and XPS all indicated that the degree of interaction between Rh and the three perovskite films can be ranked in the following order: Rh/CaTiO3/MgAl2O4 > Rh/SrTiO3/MgAl2O4 > Rh/BaTiO3/MgAl2O4. Bulk ex-solution catalysts, synthesized by reduction of ATi0.98Rh0.02O3 (A = Ca, Sr, and Ba), were also examined for comparison.

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Investigation of Rh-titanate (ATiO₃) interactions on high-surface-area perovskite thin films prepared by atomic layer deposition

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