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Acoustic Cavitation near Metal Surfaces Contaminated with Radionuclides

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HAL Id: hal-02338997

https://hal.archives-ouvertes.fr/hal-02338997

Submitted on 13 Dec 2019

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Acoustic Cavitation near Metal Surfaces Contaminated

with Radionuclides

R. Ji, M. Virot, R. Pflieger, Sergey I. Nikitenko

To cite this version:

R. Ji, M. Virot, R. Pflieger, Sergey I. Nikitenko. Acoustic Cavitation near Metal Surfaces Contami-nated with Radionuclides. XVemes Journees Nationales de Radiochimie et de Chimie Nucleaire, Sep 2016, Nice, France. 2018. �hal-02338997�

(2)

Mg surfaces immersed in oxalic acid saturated with argon at 18 ℃, agitation and sonication

• Mass Spectrometer (MS) monitors H

2

production in gas

• Scanning Electron Microscope (SEM) follows surface morphology

• Drop Shape Analyzer (DSA) measures contact angle of surface

Acoustic Cavitation near Metal Surfaces

Contaminated with Radionuclides

Ran Ji, Matthieu Virot, Rachel Pflieger, Sergey I. Nikitenko

Institut de Chimie Séparative de Marcoule (ICSM) – UMR 5257 CNRS/CEA/UM2/ENSCM

Site de Marcoule, BP17171, 30207 Bagnols sur Cèze, France

Ultrasonic cleaning is a widely used

technology in the areas of industry,

scientific

research

and

medical

application. It is able to decontaminate

items with complex surfaces with less

damages and erosion to the material

It is interesting and important to apply

this

method

to

nuclear

waste

decontamination process to remove

radioactive nuclides and finally reduce

the volume of radioactive solid wastes

Ultrasonic cleaning is based on acoustic cavitation, which creates extreme temperature and pressure

(plasma) inside bubbles, forms radicals and excited species, and induces mechanical effects (shock

wave, microjets) in solutions

In the vicinity of extended solid surfaces,

violent shock waves and micro-jets erode

the solid surfaces directly

Nucleation

Growth and

Diffusion

Maximum

Diameter

Implosion and

Shock Waves

Cycle Repeats and New bubbles grow

Gas (inlet)

CCD

Ultrasound

Transducer

Sample

Solution

Observation

Window

Gas (outlet)

Agitation

SL Spectroscopy

Standing Wave under 100 kHz within luminol solution

H

2

O →)))→ H˙ + OH˙

Luminol emits visible blue light

200 300 400 500 600 700 800 0 50 100 150 200 250 300

SL Continuum

Na

S

L in

t, A.U.

, nm

OH

0 2 4 6 8 10 12 14 16 18 4 5 6 7 8 9 10 11 12 13 14 15 16 N a i n te n si ty/ C o n ti n u u m in te n si ty

z (mm)

Relative higher Na intensity

closer to the surface

During asymmetric cavitation (microjets), Na

+

ions

are injected inside the bubble and form Na atoms

H

2

production can be controlled by [H

2

C

2

O

4

]

and start/stop sonication

MS

SEM

500μm 500μm 500μm 500μm

Initial Mg surface with

an oxide layer

1 hour treatment in

0,001M oxalic acid

Pits, whose average size

decreases with the

ultrasound frequency

Sonication results indicate that Mg decontamination is possible by controlled dissolute of surface. Mg surface morphology is transformed from

hydrophobic to hydrophilic, with pits and the appearance of precipitations or secondary phases. By modifying [H

2

C

2

O

4

] or start/stop ultrasound, it

is possible to control the generation of H

2

and the dissolution of Mg

In the presence of a metal surface, sonoluminescence spectra show that Na atom relative intensity increases. It proves the impact of solid surface

to the cavitation bubble deformation in solution, and this impact is only effective close to the surface ( ≈ 3 mm )

Mg Surface Sonication Experiments

Sonoluminescence Experiments

10 µm

Excited radicals and species can be detected by their sonoluminescence (SL) light

• Long exposure gives standing waves distribution

• SL spectroscopy quantify light intensity

204 kHz

50μm

100 kHz

No Sonication

5μm 100μm

Mg Surface

Precipitation or

secondary phases

appear

100μm

Only corrosion by

oxalic acid

Mg + 2 H

2

O → Mg(OH)

2

+ H

2

Mg(OH)

2

+ C

2

O

4

2-

→ MgC

2

O

4 (↓)

+ 2 OH

-

MgC

2

O

4

(↓)

→)))→ MgC

2

O

4

(l)

K

sp

(MgC

2

O

4

) = 8,6e-5

 H

2

generation and formation of a passive Mg(OH)

2

layer

 Nature change in the passive layer

 Sonolysis removes the passive layer and new pure Mg

layer repeat this cycle

DSA

Start 205 kHz

Ultrasound

Stop

Ultrasound

hydrophilic

hydrophobic

Acid makes a strong

erosion already after 10

minutes

Then

sonication

pit

emergence influences Mg

surface contact angle (no

change of the surface

nature)

362 kHz Sonolysis in 1M NaCl solution with argon at 15 ℃

Mapping of sonochemistry

cavitation activity

Higher Na emission closer to the surface

Long Exposure

0

10

20

30

40

50

60

0

20

40

60

80

100

120

140

Co

ntact

Angl

e

)

Time (min)

No Sonication

204 kHz

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