Physical and chemical transformations of zirconium doped ceria nanoparticles in the presence of phosphate: increasing realism in environmental fate and behaviour experiments

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@article{347bc1b4999345f489073a71da9f42d6,
title = "Physical and chemical transformations of zirconium doped ceria nanoparticles in the presence of phosphate: increasing realism in environmental fate and behaviour experiments",
abstract = "During their lifecycle, many engineered nanoparticles (ENPs) undergo significant transformations that may modify their toxicity, behaviour, and fate in the environment. Therefore, understanding the possible environmentally relevant transformations that ENPs may undergo as a result of their surroundings is becoming increasingly important. This work considers industrially produced ceria (CeO2) and focuses on a particle library consisting of seven zirconium-doped variants (Ce1-xZrxO2) where the Zr doping range is x = 0–1. The study assesses their potential transformation in the presence of environmentally relevant concentrations of phosphate. These ENPs have an important role in the operation of automotive catalysts and therefore may end up in the environment where transformations can take place. Samples were exposed to pH adjusted (c. 5.5) solutions made up of either 1 mM or 5 mM each of KH2PO4, citric acid and ascorbic acid and the transformed particles were characterised by means of DLS – size and zeta potential, UV/VIS, TEM, FT-IR, EDX and XRD. Exposure to the phosphate solutions resulted in chemical and physical changes in all ceria-containing samples to cerium phosphate (with the monazite structure). The transformations were dependent on time, ceria concentration in the particles (Ce:Zr ratio) and phosphate to ceria ratio. The presence of Zr within the doped samples did not inhibit these transformations, yet the pure end member ZrO2 ENPs showed no conversion to phosphate. The quite dramatic changes in size, structure and composition observed raise important questions regarding the relevant form of the materials to investigate in ecotoxicity tests, and for regulations based on one or more dimensions in the nanoscale.",
keywords = "Cerium, Zirconium doped ceria, Cerium phosphate, Nanoparticles, Transformation, Environmental realism, Regulation",
author = "Briffa, {Sophie Marie} and Iseult Lynch and Dimitri Hapiuk and Eva Valsami-Jones",
year = "2019",
month = sep,
day = "1",
doi = "10.1016/j.envpol.2019.06.014",
language = "English",
volume = "252",
pages = "974--981",
journal = "Environmental Pollution",
issn = "0269-7491",
publisher = "Elsevier",
number = "Part B",

}

RIS

TY - JOUR

T1 - Physical and chemical transformations of zirconium doped ceria nanoparticles in the presence of phosphate

T2 - increasing realism in environmental fate and behaviour experiments

AU - Briffa, Sophie Marie

AU - Lynch, Iseult

AU - Hapiuk, Dimitri

AU - Valsami-Jones, Eva

PY - 2019/9/1

Y1 - 2019/9/1

N2 - During their lifecycle, many engineered nanoparticles (ENPs) undergo significant transformations that may modify their toxicity, behaviour, and fate in the environment. Therefore, understanding the possible environmentally relevant transformations that ENPs may undergo as a result of their surroundings is becoming increasingly important. This work considers industrially produced ceria (CeO2) and focuses on a particle library consisting of seven zirconium-doped variants (Ce1-xZrxO2) where the Zr doping range is x = 0–1. The study assesses their potential transformation in the presence of environmentally relevant concentrations of phosphate. These ENPs have an important role in the operation of automotive catalysts and therefore may end up in the environment where transformations can take place. Samples were exposed to pH adjusted (c. 5.5) solutions made up of either 1 mM or 5 mM each of KH2PO4, citric acid and ascorbic acid and the transformed particles were characterised by means of DLS – size and zeta potential, UV/VIS, TEM, FT-IR, EDX and XRD. Exposure to the phosphate solutions resulted in chemical and physical changes in all ceria-containing samples to cerium phosphate (with the monazite structure). The transformations were dependent on time, ceria concentration in the particles (Ce:Zr ratio) and phosphate to ceria ratio. The presence of Zr within the doped samples did not inhibit these transformations, yet the pure end member ZrO2 ENPs showed no conversion to phosphate. The quite dramatic changes in size, structure and composition observed raise important questions regarding the relevant form of the materials to investigate in ecotoxicity tests, and for regulations based on one or more dimensions in the nanoscale.

AB - During their lifecycle, many engineered nanoparticles (ENPs) undergo significant transformations that may modify their toxicity, behaviour, and fate in the environment. Therefore, understanding the possible environmentally relevant transformations that ENPs may undergo as a result of their surroundings is becoming increasingly important. This work considers industrially produced ceria (CeO2) and focuses on a particle library consisting of seven zirconium-doped variants (Ce1-xZrxO2) where the Zr doping range is x = 0–1. The study assesses their potential transformation in the presence of environmentally relevant concentrations of phosphate. These ENPs have an important role in the operation of automotive catalysts and therefore may end up in the environment where transformations can take place. Samples were exposed to pH adjusted (c. 5.5) solutions made up of either 1 mM or 5 mM each of KH2PO4, citric acid and ascorbic acid and the transformed particles were characterised by means of DLS – size and zeta potential, UV/VIS, TEM, FT-IR, EDX and XRD. Exposure to the phosphate solutions resulted in chemical and physical changes in all ceria-containing samples to cerium phosphate (with the monazite structure). The transformations were dependent on time, ceria concentration in the particles (Ce:Zr ratio) and phosphate to ceria ratio. The presence of Zr within the doped samples did not inhibit these transformations, yet the pure end member ZrO2 ENPs showed no conversion to phosphate. The quite dramatic changes in size, structure and composition observed raise important questions regarding the relevant form of the materials to investigate in ecotoxicity tests, and for regulations based on one or more dimensions in the nanoscale.

KW - Cerium

KW - Zirconium doped ceria

KW - Cerium phosphate

KW - Nanoparticles

KW - Transformation

KW - Environmental realism

KW - Regulation

U2 - 10.1016/j.envpol.2019.06.014

DO - 10.1016/j.envpol.2019.06.014

M3 - Article

VL - 252

SP - 974

EP - 981

JO - Environmental Pollution

JF - Environmental Pollution

SN - 0269-7491

IS - Part B

ER -