Solubility of Nanocrystalline Cerium Dioxide: Experimental Data and Thermodynamic Modeling
Abstract
For this study, ultrafine 5 nm ceria isotropic nanoparticles were prepared using the rapid chemical precipitation approach from cerium(III) nitrate and ammonium hydroxide aqueous solutions. The as-prepared nanoparticles were shown to contain predominantly Ce(IV) species. The solubility of nanocrystalline CeO2 at several pH values was determined using ICP-MS and radioactive tracer methods. Phase composition of the ceria samples remained unchanged upon partial dissolution, while the shape of the particles changed dramatically, yielding nanorods under neutral pH conditions. According to X-ray absorption spectroscopy investigation of the supernatant, Ce(III) was the main cerium species in solution at pH < 4. Based on the results obtained, a reductive dissolution model was used for data interpretation. According to this model, the solubility product for ceria nanoparticles was determined to be log Ksp = -59.3 ± 0.3 in 0.01 M NaClO4. Taken together, our results show that the pH dependence of ceria anti- and pro-oxidant activity can be related to the dissolution of CeO2 in aqueous media.
- Authors:
-
- Lomonosov Moscow State Univ. (Russian Federation)
- National Research Centre (NRC), Moscow (Russian Federation). Kurchatov Inst. (NRCKI)
- CEA/DEN/MAR/DRCP, Bagnols sur Ceze (France). Nuclear Energy Division and Radiochemistry and Process Dept.
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS) and Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Lomonosov Moscow State Univ. (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation). Frumkin Inst. of Physical Chemistry and Electrochemistry
- Lomonosov Moscow State Univ. (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation). Kurnakov Inst. for General and Inorganic Chemistry; Tomsk State Univ. (Russian Federation). National Research
- Lomonosov Moscow State Univ. (Russian Federation); National Research Centre (NRC), Moscow (Russian Federation). Kurchatov Inst. (NRCKI)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Russian Foundation for Basic Research (RFBR); Lomonosov Moscow State Univ. (Russian Federation)
- OSTI Identifier:
- 1436138
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 120; Journal Issue: 39; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Plakhova, Tatiana V., Romanchuk, Anna Yu., Yakunin, Sergey N., Dumas, Thomas, Demir, Selvan, Wang, Shuao, Minasian, Stefan G., Shuh, David K., Tyliszczak, Tolek, Shiryaev, Andrey A., Egorov, Alexander V., Ivanov, Vladimir K., and Kalmykov, Stepan N. Solubility of Nanocrystalline Cerium Dioxide: Experimental Data and Thermodynamic Modeling. United States: N. p., 2016.
Web. doi:10.1021/acs.jpcc.6b05650.
Plakhova, Tatiana V., Romanchuk, Anna Yu., Yakunin, Sergey N., Dumas, Thomas, Demir, Selvan, Wang, Shuao, Minasian, Stefan G., Shuh, David K., Tyliszczak, Tolek, Shiryaev, Andrey A., Egorov, Alexander V., Ivanov, Vladimir K., & Kalmykov, Stepan N. Solubility of Nanocrystalline Cerium Dioxide: Experimental Data and Thermodynamic Modeling. United States. https://doi.org/10.1021/acs.jpcc.6b05650
Plakhova, Tatiana V., Romanchuk, Anna Yu., Yakunin, Sergey N., Dumas, Thomas, Demir, Selvan, Wang, Shuao, Minasian, Stefan G., Shuh, David K., Tyliszczak, Tolek, Shiryaev, Andrey A., Egorov, Alexander V., Ivanov, Vladimir K., and Kalmykov, Stepan N. Mon .
"Solubility of Nanocrystalline Cerium Dioxide: Experimental Data and Thermodynamic Modeling". United States. https://doi.org/10.1021/acs.jpcc.6b05650. https://www.osti.gov/servlets/purl/1436138.
@article{osti_1436138,
title = {Solubility of Nanocrystalline Cerium Dioxide: Experimental Data and Thermodynamic Modeling},
author = {Plakhova, Tatiana V. and Romanchuk, Anna Yu. and Yakunin, Sergey N. and Dumas, Thomas and Demir, Selvan and Wang, Shuao and Minasian, Stefan G. and Shuh, David K. and Tyliszczak, Tolek and Shiryaev, Andrey A. and Egorov, Alexander V. and Ivanov, Vladimir K. and Kalmykov, Stepan N.},
abstractNote = {For this study, ultrafine 5 nm ceria isotropic nanoparticles were prepared using the rapid chemical precipitation approach from cerium(III) nitrate and ammonium hydroxide aqueous solutions. The as-prepared nanoparticles were shown to contain predominantly Ce(IV) species. The solubility of nanocrystalline CeO2 at several pH values was determined using ICP-MS and radioactive tracer methods. Phase composition of the ceria samples remained unchanged upon partial dissolution, while the shape of the particles changed dramatically, yielding nanorods under neutral pH conditions. According to X-ray absorption spectroscopy investigation of the supernatant, Ce(III) was the main cerium species in solution at pH < 4. Based on the results obtained, a reductive dissolution model was used for data interpretation. According to this model, the solubility product for ceria nanoparticles was determined to be log Ksp = -59.3 ± 0.3 in 0.01 M NaClO4. Taken together, our results show that the pH dependence of ceria anti- and pro-oxidant activity can be related to the dissolution of CeO2 in aqueous media.},
doi = {10.1021/acs.jpcc.6b05650},
journal = {Journal of Physical Chemistry. C},
number = 39,
volume = 120,
place = {United States},
year = {Mon Sep 12 00:00:00 EDT 2016},
month = {Mon Sep 12 00:00:00 EDT 2016}
}
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Figures / Tables:
Figure 1: Characterization of as-prepared CeO2 nanoparticles: a) XRD data; b), c) HRTEM data; d) CeO2 NPs size distribution according to HRTEM and SAXS data.
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