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Title: Shifts in oxidation states of cerium oxide nanoparticles detected inside intact hydrated cells and organelles

Abstract

Cerium oxide nanoparticles (CNPs) have been shown to induce diverse biological effects, ranging from toxic to beneficial. The beneficial effects have been attributed to the potential antioxidant activity of CNPs via certain redox reactions, depending on their oxidation state or Ce3+/Ce4+ ratio. However, this ratio is strongly dependent on the environment and age of the nanoparticles and it is unclear whether and how the complex intracellular environment impacts this ratio and the possible redox reactions of CNPs. To identify any changes in the oxidation state of CNPs in the intracellular environment and better understand their intracellular reactions, we directly quantified the oxidation states of CNPs outside and inside intact hydrated cells and organelles using correlated scanning transmission x-ray and super resolution fluorescence microscopies. By analyzing hundreds of small CNP aggregates, we detected a shift to a higher Ce3+/Ce4+ ratio in CNPs inside versus outside the cells, indicating a net reduction of CNPs in the intracellular environment. We further found a similar ratio in the cytoplasm and in the lysosomes, indicating that the net reduction occurs earlier in the internalization pathway. Together with oxidative stress and toxicity measurements, our observations identify a net reduction of CNPs in the intracellular environment, whichmore » is consistent with their involvement in potentially beneficial oxidation reactions, but also point to interactions that can negatively impact the health of cells.« less

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1203896
Report Number(s):
PNNL-SA-110620
11696; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Biomaterials, 62:147-154
Additional Journal Information:
Journal Name: Biomaterials, 62:147-154
Country of Publication:
United States
Language:
English
Subject:
STXM; structured illumination microscopy; cerium oxide nanoparticles; oxidation state; Environmental Molecular Sciences Laboratory

Citation Formats

Szymanski, Craig J., Munusamy, Prabhakaran, Mihai, Cosmin, Xie, Yumei, Hu, Dehong, Gilles, Marry K., Tyliszczak, T., Thevuthasan, Suntharampillai, Baer, Donald R., and Orr, Galya. Shifts in oxidation states of cerium oxide nanoparticles detected inside intact hydrated cells and organelles. United States: N. p., 2015. Web. doi:10.1016/j.biomaterials.2015.05.042.
Szymanski, Craig J., Munusamy, Prabhakaran, Mihai, Cosmin, Xie, Yumei, Hu, Dehong, Gilles, Marry K., Tyliszczak, T., Thevuthasan, Suntharampillai, Baer, Donald R., & Orr, Galya. Shifts in oxidation states of cerium oxide nanoparticles detected inside intact hydrated cells and organelles. United States. https://doi.org/10.1016/j.biomaterials.2015.05.042
Szymanski, Craig J., Munusamy, Prabhakaran, Mihai, Cosmin, Xie, Yumei, Hu, Dehong, Gilles, Marry K., Tyliszczak, T., Thevuthasan, Suntharampillai, Baer, Donald R., and Orr, Galya. 2015. "Shifts in oxidation states of cerium oxide nanoparticles detected inside intact hydrated cells and organelles". United States. https://doi.org/10.1016/j.biomaterials.2015.05.042.
@article{osti_1203896,
title = {Shifts in oxidation states of cerium oxide nanoparticles detected inside intact hydrated cells and organelles},
author = {Szymanski, Craig J. and Munusamy, Prabhakaran and Mihai, Cosmin and Xie, Yumei and Hu, Dehong and Gilles, Marry K. and Tyliszczak, T. and Thevuthasan, Suntharampillai and Baer, Donald R. and Orr, Galya},
abstractNote = {Cerium oxide nanoparticles (CNPs) have been shown to induce diverse biological effects, ranging from toxic to beneficial. The beneficial effects have been attributed to the potential antioxidant activity of CNPs via certain redox reactions, depending on their oxidation state or Ce3+/Ce4+ ratio. However, this ratio is strongly dependent on the environment and age of the nanoparticles and it is unclear whether and how the complex intracellular environment impacts this ratio and the possible redox reactions of CNPs. To identify any changes in the oxidation state of CNPs in the intracellular environment and better understand their intracellular reactions, we directly quantified the oxidation states of CNPs outside and inside intact hydrated cells and organelles using correlated scanning transmission x-ray and super resolution fluorescence microscopies. By analyzing hundreds of small CNP aggregates, we detected a shift to a higher Ce3+/Ce4+ ratio in CNPs inside versus outside the cells, indicating a net reduction of CNPs in the intracellular environment. We further found a similar ratio in the cytoplasm and in the lysosomes, indicating that the net reduction occurs earlier in the internalization pathway. Together with oxidative stress and toxicity measurements, our observations identify a net reduction of CNPs in the intracellular environment, which is consistent with their involvement in potentially beneficial oxidation reactions, but also point to interactions that can negatively impact the health of cells.},
doi = {10.1016/j.biomaterials.2015.05.042},
url = {https://www.osti.gov/biblio/1203896}, journal = {Biomaterials, 62:147-154},
number = ,
volume = ,
place = {United States},
year = {Tue Sep 01 00:00:00 EDT 2015},
month = {Tue Sep 01 00:00:00 EDT 2015}
}