The formation of cerium(<scp>iii</scp>) hydroxide nanoparticles by a radiation mediated increase in local pH

Abellán, Patricia; Moser, Trevor; Lucas, Ivan T.; Grate, Jay W.; Evans, James E.; Browning, Nigel D.

doi:10.1039/c6ra27066b

Cited by 67 publications

(61 citation statements)

References 54 publications

(78 reference statements)

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“…We note that the net charge of the peptide is expected to be similar at neutral pH (pH 7) vs pH 5.4 (Figure S1), although the effect of binding at neutral pH was not part of this study. Additionally, we expect the Ce 3+ ion will be stable in the pH range tested, according to a recent version of the Pourbaix diagram . All solution concentrations are given as μg/mL and molar concentrations can be found in Table S1.…”

Section: Methodsmentioning

confidence: 99%

Characterization of cerium (III) ion binding to surface‐immobilized EF‐hand loop I of calmodulin

Renner

2019

Peptide Science

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Cerium has a wide range of current and emerging applications, and the binding of cerium ions to solid substrates is important for cerium recovery, or in advanced material synthesis. In this study, we investigate the affinity of a surface‐bound peptide derived from the EF‐hand loop I of calmodulin for cerium (III) ions and compare the results to a scrambled control. Results obtained via quartz crystal microbalance with dissipation are used to estimate the dissociation constant between the bound EF‐hand loop I peptide and cerium (III) ions (1.3 ± 0.1 μM), which is comparable with other dissociation constants measured for EF‐hand peptides and cerium ions in solution reported this work and in literature (0.95‐5.8 μM). Circular dichroism also suggests that the peptide binds to cerium (III) ions in solution, and undergoes a secondary structural change upon binding. Overall, this study shows that EF‐hand loop peptides are capable of binding cerium (III) ions in solution and when attached to a solid substrate.

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Section: Methodsmentioning

confidence: 99%

Characterization of cerium (III) ion binding to surface‐immobilized EF‐hand loop I of calmodulin

Renner

2019

Peptide Science

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“…In agreement with [28][29][30], we point to the possibility of (metastable) hydroxide complexes forming possibly still in dispersion. There are two ways out of the metastable region (bottom left of Pourbaix diagram), either by upwardshift through oxidative precipitation [26,27] leading to quaternary hydroxides, or through pH-reversal [48], leading to ternary hydroxides. Growth of solid or gel-type precipitates of Ce(OH) 4 = CeO 2 .…”

Section: S 72 S 0 S (A) (B) (C)mentioning

confidence: 99%

“…Irradiation induced enhancement of the fraction of Ce 3+ species in our CeO 2 particles is another mechanism, complementary to and distinct from standard reductive dissolution, where the Ce-reduction originates by water. Other most recent work have proposed alternatively either solid Ce(OH) 3 [48] species as end product or solid Ce 2 O 3 species [53] as temporary intermediate. Our reported high dissolution rates [31] are however compatible with early stage persistance of CeO 2 , and reproduced in [53].…”

Section: S 72 S 0 S (A) (B) (C)mentioning

confidence: 99%

In-situ observation of radiation physics and chemistry of nanostructured cerium oxide in water

Asghar¹,

Inkson²,

Seal³

et al. 2018

Mater. Res. Express

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Room temperature electron irradiation in aqueous environment is applied to CeO 2 nanoparticles using a transmission electron microscope equipped with liquid environmental cell. Oxide dissolution kinetics become accessible at unprecedented scale of spatial and time resolution through irradiation activation of water within a sub-µm size volume, allowing direct measurements of transformation rate and morphologies. Successful liveobservation of the formation of nano-needles provides essential inside in how 1D-nanostructures can form. Furthermore, formation of hydrogen bubbles is found and interpreted in relation to the dose needed for ceria dissolution. The results are of importance for many research applications of ceria in water, e.g. for catalysis, environmental remediation, biomedical radiation protection, anti-corrosion coatings, and ultimately via analogy to UO 2 also for fission-power fuel engineering and waste disposal.

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“…[11,12] In such ad evice, as ub-micron-thick water layer is insulated from the TEM vacuum by being enclosed between two thin amorphous Si-nitride membranes. [19] Our work aims at introducing liquid-cell TEM as am ajor tool for mainstream dissolution studies, anda lso providing quantified measurement leading to dissolution rates suitable for comparison. [13][14][15] There are many liquid-cell TEM research efforts dealing with growth of nanoparticles, but only af ew of them also mention some observation of dissolution as as econdary effect, including for Au [13,16] andC a-carbonate.…”

mentioning

confidence: 99%

“…[17] AB romine etching study on Pd nanoparticles is presented in, [18] whileaparticlegrowth study from Ce-nitrate solution is now also available. [19] Our work aims at introducing liquid-cell TEM as am ajor tool for mainstream dissolution studies, anda lso providing quantified measurement leading to dissolution rates suitable for comparison. Further,weaim to link the topic through to industrially relevant applications, where knowledge of thesed issolution rates is crucial, particularly for cerium oxides.…”

mentioning

confidence: 99%

Giant Radiolytic Dissolution Rates of Aqueous Ceria Observed in Situ by Liquid‐Cell TEM

2017

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The dynamics of cerium oxide nanoparticle aqueous corrosion are revealed in situ. We use innovative liquid-cell transmission electron microscopy (TEM) combined with deliberate high-intensity electron-beam irradiation of nanoparticle suspensions. This enables life video-recording of materials reactions in liquid, with nm resolution. We introduce image quantification to measure detailed rates of dissolution as a function of time and particle size to be compared with literature data. Giant dissolution rates, exceeding any previous reports for chemical dissolution rates at room temperature by many orders of magnitude, are discovered. The reasons for this accelerated dissolution are outlined, including the importance of the radiolysis of water preceding the ceria attack. Electron-water interaction generates radicals, ions, and hydrated electrons, which assist in hydration and reductive dissolution of oxide minerals. The presented methodology has the potential to become a novel accelerated testing procedure to compare multiple nanoscale materials for relative aqueous durability. The ceria-water system is of crucial importance for the fields of catalysis, abrasive polishing, environmental remediation, and as simulant for actinide oxide behaviour in contact with liquid for nuclear engineering.

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The formation of cerium(iii) hydroxide nanoparticles by a radiation mediated increase in local pH

Abstract: High energy electrons are used to generate homogeneously distributed nanometric Ce(iii) particles in situ avoiding large excesses of chemical reagents.

Cited by 67 publications

References 54 publications

Characterization of cerium (III) ion binding to surface‐immobilized EF‐hand loop I of calmodulin

Characterization of cerium (III) ion binding to surface‐immobilized EF‐hand loop I of calmodulin

In-situ observation of radiation physics and chemistry of nanostructured cerium oxide in water

Giant Radiolytic Dissolution Rates of Aqueous Ceria Observed in Situ by Liquid‐Cell TEM

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