# Novel production method for traceable surface sources by aluminium functionalisation

Dilan Tuzun, V. Lourenço, Lucille Chambon, Yann Kergadallan

► To cite this version:

Dilan Tuzun, V. Lourenço, Lucille Chambon, Yann Kergadallan. Novel production method for traceable surface sources by aluminium functionalisation. ICRM 2023 - 23rd International Conference on Radionuclide Metrology and its Applications, Mar 2023, Bucarest, Romania. cea-04272758

HAL Id: cea-04272758

https://cea.hal.science/cea-04272758

Submitted on 6 Nov 2023

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Distributed under a Creative Commons Attribution 4.0 International License
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Novel production method for traceable surface sources
by aluminium functionalisation

Dilan Tüzün, V. Lourenço, L. Chambon, Y. Kergadallan

Université Paris-Saclay, CEA, List, LNE-LNHB, Palaiseau, France
# Aim: Measuring radioactivity on complex surfaces

Planning

Physical and radiological
characterisation

Decontamination

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[IAEA, 2016]

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## Challenges:

* Discrimination of non-contaminated surface from low-level contaminated surface

* Very large areas

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* Non-flat surfaces

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# Aim: Measuring radioactivity on complex surfaces

<figure><img src="image_10.png" /><figcaption>## Complex shapes</figcaption></figure>

### Needs:

* Reliable contamination measurements

* Calibration of measurement systems

### Aim:

* Traceable activity and emitted flux

* Large surface areas

* Non-contaminating surface (use on-site)

* Complex shapes

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<figure><img src="image_12.png" /><figcaption>## Commercial source</figcaption></figure>

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Provide metrologically traceable standard surface sources of various shapes
# Our approach: chemical attachment

<figure><img src="image_14.png" /></figure>

## Commercial source

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## Commercial sources :
Radionuclide dried + protected

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Al thickness:
3 mm

Adsorption / Physisorption E_bonding ~ kJ/mol

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## Chemical bonds radionuclide-surface

<figure><img src="image_19.png" /></figure>

Al thickness: 0.3 mm

Chemisorption E_bonding > 100 kJ/mol

## Use of functionalisation

* Strong chemical bonds (non-contaminating sources, to check)
  → **No cover layer**

* Thin sources → **Minimise self-absorption** of low penetration radiation (α, β)

<figure><img src="image_20.png" /></figure>

Radionuclide

Surface functionalisation

Substrate

## Chosen substrates:

* **Aluminium foil**

* Polymeric surfaces

<figure><img src="image_21.png" /></figure>

Emitted particles

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### 1) Functionalisation

- Attach functions to the surface

- 3 main methods

### 3) Radionuclide Binding

- Attach the radionuclide $^{152}$Eu and $^{241}$Am

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Uniform, traceable, large area surface sources ?

### 4) Radiological Characterization

- Uniformity

- Traceability

- Non-contamination

### 2) Chemical characterization

- SEM analyses (topology of the surface)

- Infrared Spectroscopy (Chemical bonds)

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# Functions on the surface

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<figure><img src="image_32.png" /><figcaption>Manganese oxide/hydroxide</figcaption></figure>

## Manganese oxide layer

$Ra^{2+}$, $UO_2^{2+}$

* Reduction of Mn(VII)

* Precipitate as an oxide layer

* Not polymeric

* Brownish colored layer

(Ren et al, 2020)

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<figure><img src="image_35.png" /><figcaption>Chromium oxide/hydroxide</figcaption></figure>

## Chromium oxide layer

$Ra^{2+}$, $UO_2^{2+}$

* Reduction of Cr(VI)

* Inorganic polymer

* Soft-gel like mixture formed

* Yellow to dark brown color

(Pommiers et. al. 2014)

<figure><img src="image_36.png" /></figure>

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## Sulfonation Treatment

$Eu^{3+}$, $Am^{3+}$

* Greyish color

(Gao et.al. 2017, Oudah et.a., 2018)

Act as cation exchangers to bind radioactive element
<figure><img src="image_38.png" /></figure>

1) Functionalisation

* Attach functions to the surface

* 3 main methods

3) Radionuclide Binding

* Attach the radionuclide
  ¹⁵²Eu and ²⁴¹Am

<figure><img src="image_39.png" /></figure>

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Uniform,
traceable, large
area surface
sources ?

<figure><img src="image_42.png" /></figure>

4) Radiological
Characterization

* Uniformity

* Traceability

* Non-contamination

2) Chemical characterization

* SEM analyses (topology of the surface)

* Infrared Spectroscopy
  (Chemical bonds)

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<figure><img src="image_44.png" /></figure>
# How effective is functionalisation?

3D animation of vibrations
in infrared spectroscopy

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SYMMETRIC
STRECHING

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ANTISYMMETRIC
STRECHING

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ROCKING

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WAGGING

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TWISTING

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SCISSORING

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Infrared spectra

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Magnification: x800 x35000

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Al-OH bonds

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1) Functionalisation

* Attach functions to the surface

* 3 main methods

3) Radionuclide Binding

* Attach the radionuclide
  ¹⁵²Eu and ²⁴¹Am

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Uniform,
traceable, large
area surface
sources ?

4) Radiological
Characterization

* Uniformity

* Traceability

* Non-contamination

2) Chemical characterization

* SEM analyses (topology of the surface)

* Infrared Spectroscopy
  (Chemical bonds)

<figure><img src="image_67.png" /></figure>

<figure><img src="image_68.png" /></figure>
# Radionuclide binding experiment

<figure><img src="image_69.png" /></figure>

Functionalised
aluminium

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Radionuclide
($^{152}$Eu or $^{241}$Am) medium
Condition: pH 2

<figure><img src="image_71.png" /></figure>

<figure><img src="image_72.png" /></figure>

Under agitation 4 hours

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1 mL from the
radionuclide
solution

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Sampling from the
radionuclide medium

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Weighing the radioactive
source

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Liquid scintillation counter

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Rinsed with water

Radioactive sample

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Digital autoradiography with imaging plate
# Experimental conditions

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Activity (Bq = s⁻¹)

$$n = \frac{A \cdot T_{1/2}}{N_A \cdot \ln 2}$$

Amount of substance (mol)

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$^{241}$Am

$^{152}$Eu

Half-life ($t_{1/2}$)

432.2 y

13.54 y

Emitter type

α, γ

β, γ

<table><thead><tr><td>Samples</td><td>Radionuclide</td><td>Stable/Active element ratio</td><td>Total amount of element in solution (picomol)</td></tr></thead><tbody><tr><td>Sulfonation</td><td><sup>152</sup>Eu</td><td>~ 57</td><td>~ 0.4</td></tr><tr><td>Chromium oxide layer</td><td><sup>152</sup>Eu</td><td>~ 57</td><td>~ 0.4</td></tr><tr><td>Manganese oxide layer</td><td><sup>152</sup>Eu</td><td>~ 57</td><td>~ 0.4</td></tr><tr><td>Manganese oxide layer</td><td><sup>241</sup>Am</td><td>No carrier</td><td>~ 0.5</td></tr></tbody></table>
3rd step

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1) Functionalisation

* Attach functions to the surface

* 3 main methods

3) Radionuclide Binding

* Attach the radionuclide
  ¹⁵²Eu and ²⁴¹Am

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<figure><img src="image_86.png" /></figure>

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Uniform,
traceable, large
area surface
sources ?

4) Radiological
Characterization

* Uniformity

* Traceability

* Non-contamination

2) Chemical characterization

* SEM analyses (topology of the surface)

* Infrared Spectroscopy
  (Chemical bonds)

<figure><img src="image_94.png" /></figure>
# Activity of the sources

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<table><thead><tr><td>Samples</td><td>RN</td><td>% LSC activity decrease</td><td>Max nber of moles on the surface (picomol)</td><td>Max activity bound (Bq.cm<sup>-2</sup>)</td></tr></thead><tbody><tr><td>Sulfonation</td><td><sup>152</sup>Eu</td><td>(15 ± 1)%</td><td>~ 0.07</td><td>3.5 ± 0.3</td></tr><tr><td>Cr oxide</td><td><sup>152</sup>Eu</td><td>(19 ± 1)%</td><td>~ 0.07</td><td>5.0 ± 0.5</td></tr><tr><td>Mn oxide</td><td><sup>152</sup>Eu</td><td>(8.0 ± 0.5)%</td><td>~ 0.03</td><td>2.0 ± 0.2</td></tr><tr><td>Mn oxide</td><td><sup>241</sup>Am</td><td>(70 ± 5)%</td><td>~ 0.4</td><td>18.5 ± 2</td></tr></tbody></table>

<figure><img src="image_97.png" /></figure>
# Autoradiography imaging

<figure><img src="image_98.png" /><figcaption>Digital autoradiography
(Amersham™ Typhoon™)</figcaption></figure>

<figure><img src="image_99.png" /><figcaption>Sources on the screen</figcaption></figure>

* Close contact with screen for exposure

<figure><img src="image_100.png" /><figcaption>Autoradiography images</figcaption></figure>

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# Autoradiography imaging

<figure><img src="image_102.png" /></figure>

Manganese oxide layer
Uniformity (standard dev.): 95%

Chromium oxide layer
Uniformity: ~50%

Sulfonation
Uniformity: ~80%

<figure><img src="image_103.png" /></figure>
<figure><img src="image_104.png" /></figure>

<figure><img src="image_105.png" /></figure>

- Uniformity

- Traceability

- Non-contamination

## 2) Chemical characterization

- SEM analyses (topology of the surface)

- Infrared Spectroscopy (Chemical bonds)

<figure><img src="image_106.png" /></figure>
# Conclusions & future work

<figure><img src="image_107.png" /></figure>

## ACHIEVEMENTS

* 3 different source production methods

* Surface activities from 2-20 Bq/cm²: **tunable**

* <sup>241</sup>Am and <sup>152</sup>Eu sources

* Some uniform sources (>90%)

<figure><img src="image_108.png" /></figure>

<figure><img src="image_109.png" /></figure>

## IMPROVEMENTS

* Uniformity: by using 0.5 mm Al foils

* <sup>244</sup>Cm binding (α)

* Non-contamination tests to be performed

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