Center for Radioisotope and Radiopharmaceutical Technology

National Nuclear Energy Agency (BATAN)

Puspiptek Area, Serpong, South Tangerang, INDONESIA - 15314

Email: imamkey@batan.go.id

ICTP, Trieste, Italy

Trieste, 2-13 October 2017

Assessment of Residual Radioisotopes Following F-18 Radionuclide Production

Imam Kambali

www.batan.go.id

1. Introduction

06/03/2017 2

Fluorine-18 (F-18) is used in nuclear medicine for cancer diagnosis

At Dharmais Cancer Hospital in Jakarta, F-18 is produced using an 11-MeV proton accelerating cyclotron

F-18 production generates a vast number of secondary neutrons which are scattered off and/or transmitted into surrounding materials

It could potentially generate residual radioisotopes in the cyclotron vicinity which eventually become major safety concerns over radiation exposure to the workers

Radiation measurement and radioisotope identification are required

Proton beam H2

18O target neutrons

18O(p,n)18F

Surrounding materials

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2. Experiments

06/03/2017 3

F-18 production was done using an 11-MeV cyclotron at Dharmais Cancer Hospital in Jakarta, Indonesia

Residual radionuclides in post-irradiated H218O were detected

Radiation in the cyclotron vicinity were detected, including the cyclotron’s shielding, cyclotron tank/chamber, cave wall as well as target system

Target

system

Inner surface of

cyclotron shielding

Outer surface of

cyclotron shielding

Outer surface of

cyclotron chamber

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2. Experiments

06/03/2017 4

Eclipse 11 MeV

Cyclotron

Concrete wall

Control room

Cyclotron shielding

UPS

Power supply

11-MeV cyclotron cave in Dharmais Cancer Hospital, Jakarta

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2. Experiments

06/03/2017 5

Target system for F-18 production at Dharmais Cancer Hospital, Jakarta

Enriched water target

Proton beam

Havar window Silver body / tube

Rear screws

Collimator

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2. Experiments

06/03/2017 6

Radiation detection and measurement was performed using HPGe based gamma ray spectrometer and NaI based portable gamma ray spectrometer

TALYS Evaluated Nuclear Data (TENDL 2015) were employed to study the origin of residual radioisotopes

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3. Results and Discussion

06/03/2017 7

3.1 Gamma spectrum of residual radioisotopes detected in Irradiated H2

18O

0 500 1000 1500 20000

100

200

300

400

500

600

700

800

energy (keV)

inte

nsity (

co

unts

)

1000 1500 2000 2500 30000

20

40

60

Sample was measured 2 days following F-18 production Measurement was done using HpGe based gamma spectroscopy system

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3. Results and Discussion

06/03/2017 8

3.1 Residual Radioisotopes Detected in Irradiated H218O, 2

Days Following F-18 Production

Radio-

nuclide

T1/2

(days)

Eγ (keV) Nuclear Reaction Source

57Co 271.8 122 60Ni(p,α)57Co; 58Ni(p,2p)57Co;

58Ni(n,2n)57Co

Havar

57Ni 1.496 511, 1378 58Ni(p,pn)57Ni; 58Ni(p,d)57Ni; 59Co(p,X)57Ni Havar

58Co 70.83 811 58Fe(p,n)58Co; 58Ni(n,p) 58Co; 59Co(n,2n)

58Co

Havar

54Mn 312.1 835 58Fe(n,p)54Mn; 55Mn(n,2n) 54Mn Havar

56Co 77.24 847 56Fe(p,n)57Co; 56Fe(p,2n)57Co Havar

55Co 0.730 931, 2557 58Ni(p,α)55Co Havar

52Mn 5.591 936, 1434 52Cr(p,n)52Mn Havar

48V 15.974 983, 1312 49Ti(p,2n)48V Havar

110Ag 250 657, 885, 937 109Ag(n,γ)110Ag Silver body

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3. Results and Discussion

06/03/2017 9

3.1 Radiation Detected in the Outer Surface of the Cyclotron Chamber

0.4 0.5 0.6 0.7 0.8 0.9 1 1.1 1.2 1.3 1.4 1.50

1000

2000

3000

4000

5000

6000

7000

inte

nsity (

co

un

t)

Energy (MeV)

Mn-54

Annihilation peak

(a)

0 5 10 15 20 25 300

100

200

300

400

500

600

700

800

900

Nucle

ar

Cro

ss-s

ection (

mbarn

)

Proton or Neutron Energy (MeV)

54Fe(n,p)54Mn

55Mn(n,2n)54Mn(b)54Cr(p,n)54Mn

(a) Gamma ray emissions detected in the outer surface of the cyclotron chamber (at 90o with respect

to the incoming proton beam), and (b) TALYS-calculated nuclear cross-sections of 54Cr(p,n)54Mn, 54Fe(n,p)54Mn, and 55Mn(n,2n)54Mn reactions.

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3. Results and Discussion

06/03/2017 10

3.2 Radiation Detected in the Inner Surface of the Shielding

(a) Gamma ray emissions detected in the inner surface of the Eclipse 11 cyclotron’s shielding

(b) TALYS-calculated nuclear cross-sections of several trace elements present in the shielding and

wall of the cyclotron cave in Dharmais Cancer Hospital, Jakarta

0.4 0.5 0.6 0.7 0.8 0.9 1 1.1 1.2 1.3 1.4 1.50

2000

4000

6000

8000

10000

12000

14000

16000

inte

nsity (

count)

Energy (MeV)

0.7 0.8 0.9 1 1.1 1.2 1.30

500

1000

1500 Mn-54

Zn-65

Zn-65

Mn-54

Annihilation peak

0.002 0.004 0.006 0.008 0.01 0.012 0.014 0.016 0.018 0.020

1

2

3

4

5x 10

5

Cro

ss-s

ectio

n (

mb

arn

)

Energy (MeV)

0.005 0.01 0.015 0.020

1000

2000

5 10 15 20 25 300

2000

4000

6000

8000

10000

Cro

ss-s

ectio

n (

mb

arn

)

Energy (MeV)

(2)

(1)

(1)

(2)

(5)(6)(7)

(3)

(4)

(5)

(6) 54

Fe(n,p)54

Mn

(7) 55

Mn(n,2n)54

Mn

(1) 151

Eu(n,)152

Eu

(2) 133

Cs(n,)134

Cs

(3) 45

Sc(n,)46

Sc

(4) 59

Co(n,)60

Co

(5) 64

Zn(n,)65

Zn

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3. Results and Discussion

06/03/2017 11

3.2 Radiation Detected in the Outer Surface of the Shielding

(a) Gamma ray emissions detected in the outer surface

of the Eclipse 11 cyclotron’s shielding

(b) Angular distribution of the Eu-152 gamma ray

intensities

(c) TALYS-calculated nuclear cross-sections of several

trace elements present in the shielding and wall of

the cyclotron cave in Dharmais Cancer Hospital,

Jakarta

0.002 0.004 0.006 0.008 0.01 0.012 0.014 0.016 0.018 0.020

1

2

3

4

5x 10

5

Cro

ss-s

ectio

n (

mb

arn

)

Energy (MeV)

0.005 0.01 0.015 0.020

1000

2000

5 10 15 20 25 300

2000

4000

6000

8000

10000C

ross-s

ectio

n (

mb

arn

)

Energy (MeV)

(2)

(1)

(1)

(2)

(5)(6)(7)

(3)

(4)

(5)

(6) 54

Fe(n,p)54

Mn

(7) 55

Mn(n,2n)54

Mn

(1) 151

Eu(n,)152

Eu

(2) 133

Cs(n,)134

Cs

(3) 45

Sc(n,)46

Sc

(4) 59

Co(n,)60

Co

(5) 64

Zn(n,)65

Zn

0.4 0.5 0.6 0.7 0.8 0.9 1 1.1 1.2 1.3 1.4 1.50

100

200

300

400

500

inte

nsity (

count)

Energy (MeV)

Annihilationpeak

Eu-152

(a)

-10 0 10 20 30 40 50 60 70 80 90 1001

2

3

4

count ra

te (

count/s)

Angle (o)

(b)

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3. Results and Discussion

06/03/2017 12

3.3 Radiation Detected in the Target System

3.3.1 Havar window

(a) Gamma ray emissions detected in the Havar window, and

(b) (b) TALYS-calculated nuclear cross-sections of possible proton-induced radionuclides

0.2 0.4 0.6 0.8 1 1.2 1.40

1

2

3

4

5x 10

4

inte

nsity (

co

un

t)

Energy (MeV)

Co-56

Annihilation

peak

Pb

X-rays

Co-56

(a)

0 2 4 6 8 10 12 14 16 18 200

200

400

600

800

1000

nu

cle

ar

cro

ss-s

ectio

n (

mb

arn

)

proton ennergy (MeV)

(b)96Mo(p,n)96Tc

55Mn(p,n)55Fe

(7)

(6)

(5)(3)(2)

(4)

(1)

(1)

(2)

(5)

(4)

(3)(6)

(7)

59Co(p,n)59Ni

56Fe(p,n)56Co

52Cr(p,n)52Mn

184W(p,n)184Re

58Ni(p,n)58Cu

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3. Results and Discussion

06/03/2017 13

3.3 Radiation Detected in the Target System

3.3.2 Collimator

Gamma ray emissions captured by the portable gamma ray spectrometry system from the collimator

in the target system

0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.50

0.5

1

1.5

2

2.5x 10

4

inte

nsity (

count)

Energy (MeV)

Co-56Pb X-rays

Annihilationpeak

Co-56

0 2 4 6 8 10 12 14 16 18 200

200

400

600

800

1000

nu

cle

ar

cro

ss-s

ectio

n (

mb

arn

)

proton ennergy (MeV)

(b)96Mo(p,n)96Tc

55Mn(p,n)55Fe

(7)

(6)

(5)(3)(2)

(4)

(1)

(1)

(2)

(5)

(4)

(3)(6)

(7)

59Co(p,n)59Ni

56Fe(p,n)56Co

52Cr(p,n)52Mn

184W(p,n)184Re

58Ni(p,n)58Cu

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3. Results and Discussion

06/03/2017 14

3.3 Radiation Detected in the Target System

3.3.3 Target Body

(a) Gamma ray emissions detected in the silver body, and

(b) TALYS-calculated nuclear cross-sections of 109Ag(n,γ)110mAg, 109Ag(p,n)109Cd and 109Ag(p,2n)108Pd nuclear reactions

0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.550

0.5

1

1.5

2x 10

5

inte

nsity (

count)

Energy (MeV)

1.15 1.3 1.451

1.5

2

2.5x 10

4

Ag-110mAg-110m

Pb X-ray

Ag-110m(a)

0 0.2 0.4 0.6 0.8 1

x 10-7

0

0.5

1

1.5

2

2.5

3

3.5

4

4.5x 10

6

nucle

ar

cro

ss-s

ection (

mbarn

)

proton or neutron energy (MeV)

0 5 10 15 20 25 300

600

1200

1800

0 5 10 15 20 25 300

10

2025

(b)

109Ag(p,2n)108Pd

109Ag(p,n)109Cd109Ag(n,)110mAg

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3. Results and Discussion

06/03/2017 15

3.3 Radiation Detected in the Target System

3.3.4 The Rear Screw

(a) Gamma ray emissions detected in the rear screw of the target system, and

(b) TALYS-calculated nuclear cross-sections of 51Mn(n,γ)52Mn and 59Co(p,n)60Co

0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.550

500

1000

1500

2000

2500

3000

3500

inte

nsity (

count)

Energy (MeV)

0.95 1.15 1.35 1.550

50

100

150

200

Annihilationpeak Mn-54

Pb X-rays

(a)Mn-52

Co-60

Co-60

0 1 2 3 4

x 10-8

0

0.5

1

1.5

2x 10

6

nucl

ear

cross

-sect

ion (

mbarn

)

proton ennergy (MeV)

0 5 10 15 200

5

1051Mn(n,)52Mn

59Co(n,)60Co

(b)

51Mn(n,)52Mn

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4. Conclusion

06/03/2017 16

Proton and neutron induced by-products identified in the Dharmais Cancer Hospital, Jakarta

No Investigated Component/Point Observed

Radionuclide

Nuclear Reaction

1. Outer surface of the cyclotron chamber Mn-54 54Fe(n,p)54Mn

2. Inner and outer surface of the cyclotron

shielding

Zn-65

Mn-54

Eu-152

64Zn(n,γ)65Zn

54Fe(n,p)54Mn and/or 55Mn(n, 2n)54Mn

151Eu(n,γ)152Eu

3. Havar windows and collimator Co-56 56Fe(p,n)56Co

4. Silver body Ag-110m 109Ag(n,γ)110mAg

5. Rear screws Mn-52,

Co-60,

Mn-54

51Mn(n,γ)52Mn

59Co(n,γ)60Co

54Fe(n,p)54Mn and/or 55Mn(n, 2n)54Mn

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Thank You Grazie

Terima kasih