Wet to Dry Controls Lanthanide Scandate Synthesis

Emily P. Greenstein; Kenneth R. Poeppelmeier; Laurence D. Marks

doi:10.1021/acs.inorgchem.2c04107

Wet to Dry Controls Lanthanide Scandate Synthesis

Emily P. Greenstein^*, Kenneth R. Poeppelmeier, Laurence D. Marks

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

The choice of temperature and gas conditions used in a water pressure-controlled reactor is guided by density functional theory (DFT) to synthesize nearly phase-pure lanthanide scandate nanoparticles (LnScO₃, Ln = La, Nd, Sm, Gd). In this synthetic method, low water-vapor partial pressures, well below water’s gas liquidus, inhibit particle growth, while an excess of water vapor results in undesired rare-earth hydroxide and oxyhydroxide secondary phases. The optimal humidity for high-purity LnScO₃ particle synthesis is shown to vary with the lanthanide; DFT is used to calculate the thermodynamics of secondary phase formation for each lanthanide tested such that the role of water vapor may be quantified and used to maintain phase purity (greater than 96 mol %) across the series. The combination of thermodynamic calculation and experimental confirmation with this pressure-controlled reactor provides an opportunity to explore analogous syntheses of other inorganic perovskite nanoparticles.

Original language	English (US)
Pages (from-to)	4853-4860
Number of pages	8
Journal	Inorganic chemistry
Volume	62
Issue number	12
DOIs	https://doi.org/10.1021/acs.inorgchem.2c04107
State	Published - Mar 27 2023

Funding

This work was supported by the Northwestern University Institute for Catalysis in Energy Processes (ICEP) under grant no. DOE DE-FG02-03ER15457. ICEP is funded by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Science, U.S. Department of Energy. The authors acknowledge Dr. Robert Kennedy and Dr. Fenghua Ding for their help to design and construct the hydrosauna reactor, and Dr. Ryan Paull for his discussions about and fundamental contributions to development of the hydrosauna method.

ASJC Scopus subject areas

Inorganic Chemistry
Physical and Theoretical Chemistry

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10.1021/acs.inorgchem.2c04107

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title = "Wet to Dry Controls Lanthanide Scandate Synthesis",

abstract = "The choice of temperature and gas conditions used in a water pressure-controlled reactor is guided by density functional theory (DFT) to synthesize nearly phase-pure lanthanide scandate nanoparticles (LnScO3, Ln = La, Nd, Sm, Gd). In this synthetic method, low water-vapor partial pressures, well below water{\textquoteright}s gas liquidus, inhibit particle growth, while an excess of water vapor results in undesired rare-earth hydroxide and oxyhydroxide secondary phases. The optimal humidity for high-purity LnScO3 particle synthesis is shown to vary with the lanthanide; DFT is used to calculate the thermodynamics of secondary phase formation for each lanthanide tested such that the role of water vapor may be quantified and used to maintain phase purity (greater than 96 mol %) across the series. The combination of thermodynamic calculation and experimental confirmation with this pressure-controlled reactor provides an opportunity to explore analogous syntheses of other inorganic perovskite nanoparticles.",

author = "Greenstein, {Emily P.} and Poeppelmeier, {Kenneth R.} and Marks, {Laurence D.}",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

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doi = "10.1021/acs.inorgchem.2c04107",

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T1 - Wet to Dry Controls Lanthanide Scandate Synthesis

AU - Greenstein, Emily P.

AU - Poeppelmeier, Kenneth R.

AU - Marks, Laurence D.

PY - 2023/3/27

Y1 - 2023/3/27

N2 - The choice of temperature and gas conditions used in a water pressure-controlled reactor is guided by density functional theory (DFT) to synthesize nearly phase-pure lanthanide scandate nanoparticles (LnScO3, Ln = La, Nd, Sm, Gd). In this synthetic method, low water-vapor partial pressures, well below water’s gas liquidus, inhibit particle growth, while an excess of water vapor results in undesired rare-earth hydroxide and oxyhydroxide secondary phases. The optimal humidity for high-purity LnScO3 particle synthesis is shown to vary with the lanthanide; DFT is used to calculate the thermodynamics of secondary phase formation for each lanthanide tested such that the role of water vapor may be quantified and used to maintain phase purity (greater than 96 mol %) across the series. The combination of thermodynamic calculation and experimental confirmation with this pressure-controlled reactor provides an opportunity to explore analogous syntheses of other inorganic perovskite nanoparticles.

AB - The choice of temperature and gas conditions used in a water pressure-controlled reactor is guided by density functional theory (DFT) to synthesize nearly phase-pure lanthanide scandate nanoparticles (LnScO3, Ln = La, Nd, Sm, Gd). In this synthetic method, low water-vapor partial pressures, well below water’s gas liquidus, inhibit particle growth, while an excess of water vapor results in undesired rare-earth hydroxide and oxyhydroxide secondary phases. The optimal humidity for high-purity LnScO3 particle synthesis is shown to vary with the lanthanide; DFT is used to calculate the thermodynamics of secondary phase formation for each lanthanide tested such that the role of water vapor may be quantified and used to maintain phase purity (greater than 96 mol %) across the series. The combination of thermodynamic calculation and experimental confirmation with this pressure-controlled reactor provides an opportunity to explore analogous syntheses of other inorganic perovskite nanoparticles.

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JO - Inorganic chemistry

JF - Inorganic chemistry

IS - 12

ER -

Wet to Dry Controls Lanthanide Scandate Synthesis

Abstract

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