L.Zavorka+, J.Adam, A.Baldin, W.Furman, J.Khushvaktov, Yu.Kish, V.Pronskikh, A.Solnyshkin, V.Stegailov,

V.Tsoupko - Sitnikov, J.Vrzalova+, S.Tyutyunnikov, M.Zeman Joint Institute for Nuclear Research, Dubna, Russia +Czech Technical University, Prague, Czech Republic

V. Chilap CPTP «Atomenergomash», Moscow, Russia

& colleagues of the “E&T-RAW” collaboration

«Energy and Transmutation - RAW»

J.Adam, A.Baldin, A.Berlev, W.Furman, N.Gundorin, B.Gus’kov, M.Kadykov, J.Khushvaktov, Yu.Kish, Yu.Kopatch, E.Kostyuhov, I.Kudashkin, A.Makan’kin, I.Mar’in, A.Polansky,

V.Pronskikh, A.Rogov, V.Schegolev, A.Solnyshkin, V.Tsupko-Sitnikov, S.Tyutyunnikov, A.Vishnevsky, N.Vladimirova, A.Wojciechowski, J.Vrzalova, L.Zavorka, M.Zeman

Joint Institute for Nuclear Research, Dubna, Russia V.Chilap, A.Chinenov, B.Dubinkin, B.Fonarev, M.Galanin, V.Kolesnikov, S.Solodchenkova

CPTP «Atomenergomash», Moscow, Russia M.Artyushenko, V.Sotnikov, V.Voronko

KIPT, Kharkov, Ukraine A.Khilmanovich, B.Marcynkevich

Stepanov IP, Minsk, Belarus K. Husak, S.Korneev, A.Potapenko, A.Safronova, I.Zhuk

JIENR Sosny near Minsk, Belarus M.Suchopar, O.Svoboda, V.Wagner

INP, Rez near Praha, Czech Republic Ch. Stoyanov, O.Yordanov, P.Zhivkov

Institute of Nuclear Research and Nuclear Energy, Sofia, Bulgaria M.Shuta, E.Strugalska-Gola, S.Kilim, M.Bielevicz

National Centre for Nuclear Research, Otwock-Swerk, Poland S.Kislitsin, T.Kvochkina, S. Zhdanov

Institute of Nuclear Physics NNC RK, Almaty, Kazakhstan M. Manolopoulou

Aristotle Uni-Thessaloniki, Thessaloniki, Greece W.Westmeier

Gesellschaft for Kernspektrometrie, Germany R.S.Hashemi-Nezhad

School of Physics, University of Sydney, Australia

Focus

1990s

1978

2011-2013

2015 ?

Introduction

• The key problems of the nuclear energy to be solved:

• nuclear safety

• spent nuclear fuel treatment

• effective utilization of natural uranium and thorium reserves

• Subcritical Accelerator Driven Systems (ADS) represent one of possible solutions

4

Introduction

• Different concepts and schemes in ADS research worldwide

• MYRRHA project Belgium • 𝑬𝒑 = 600 MeV

• Relativistic Nuclear Technology (RNT) based on energy production and spent nuclear fuel transmutation in

a hard neutron spectrum

Energy of incident particles Ep,d ~ 10 GeV

5

Fast neutron spectrum

• Transmutation of long-lived fission products (FP) and actinides into short-lived or stable isotopes

• (n,g)

• (n,f)

• (n,xn)

6 10-13 10-11 10-9 10-7 10-5 10-3 10-1 101

10-4

10-3

10-2

10-1

100

101

102

103

104

237Np Cross Sections

Cro

ss s

ectio

n (b

)

Neutron energy (GeV)

(n,f) (n,g) (n,2n)

Experimental background: Beam energy

A. Krása, et al. NIM A (2010)

• ø 10 x 100 cm lead target

• compilation of experimental data + new measurement

• maximum neutron production around the beam energy 1 GeV

V.Yurevich, et al. PPN (2006)

• ø 20 x 60 cm lead target

•Kinetic energy of neutron radiation Ekin and mean neutron energy < En > grow

•Energy W spent on neutron production increases as well

Ed

(GeV) < En > (MeV)

W/Ed (%)

1.03 6.5 32.6

1.98 7.9 43.9

3.76 10.4 45.7

STILL Optimal beam energy for ADS: OPEN

7

Neutrons at higher energies

• Considerable increase in average multiplicity of prompt-fission neutrons up to En = 200 MeV

0 20 40 60 80 100 120 140 160 180 200

2

4

6

8

10

12

14

16

J.Taieb,+ 14215001 J.Frehaut,+ 20490001 J.Frehaut,+ 21685001 T.Ethvignot,+ 13964001 I.Asplund-Nilsson,+ 20075001

Prom

pt n

eutr

on y

ield

(pp

f)

Neutron energy (MeV)

238U

EXFOR:

8

• Prompt-fission neutron average kinetic energy (Watt spectrum) increases as well

(20% higher at En = 200 MeV)

Fundamental requirement:

• Monte Carlo simulation tools:

9

10-11 10-9 10-7 10-5 10-3 10-1 10110-6

10-5

10-4

10-3

10-2

10-1

100

101

102

103

104

R = 30 mm

2 AGeV R30

4 AGeV R30

2 AGeV R120

4 AGeV R120

Neu

tron

flu

x (c

m-2G

eV-1∙d

eute

ron-1

AG

eV-1)

Neutron energy (GeV)

R = 120 mm

MARS15 • Increase in:

• Neutron multiplicity due to (n,xn)

• Mean neutron energy f(Ebeam)

• Average kinetic energy f(En)

• Neutron yield f(En)

• Decrease in: • Neutron production per

one proton above 1 GeV

Maximum hard neutron spectrum

Experimental investigation

at the quasi-infinite target

QUINTA target

500 kg natU December 2013

30 cm

10

Deuteron beam: (Al, Cu monitors)

Ed = 2 AGeV 2.12(3)1013 particles Ed = 4 AGeV 6.08(6)1012 particles

Experimental samples

• 209Bi • Natural uranium • Enriched uranium

• 235U and 238U

10-11 10-9 10-7 10-5 10-3 10-1 101

10-6

10-5

10-4

10-3

10-2

10-1

100

101

102

103

104

R = 30 mm

2 AGeV R30

4 AGeV R30

2 AGeV R120

4 AGeV R120

Neu

tron

flu

x (c

m-2G

eV-1∙d

eute

ron-1

AG

eV-1)

Neutron energy (GeV)

R = 120 mm

10-11 10-9 10-7 10-5 10-3 10-1 101101

102

103

104

105

106

238U(n,2n)

209Bi(n,f)

209Bi(n,xn)

238U(n,f)

238U(n,g)Cro

ss s

ectio

n (m

b)

Neutron energy (GeV)

235U(n,f)

Fundamental cross sections

JENDL-HE/2007TALYS 1.6

11

0.72%

99.28%

Natural uranium95.17%

4.83%

238U 235U

Enriched uranium

Experimental methods

• Activation measurement technique

• Gamma spectroscopy with the use of

HPGe detectors Canberra and ORTEC

(20%, resp. 30% relative efficiency)

Calibrated with standards made in 2013;

FEP eff. Compared with MCNP simulation

12

Isotope identification

• Half-life (≥ 6 measurements)

• Energy and intensity of gamma line

• Reaction rates calculated

from measured activity

• Included corrections: decay during irradiation, cooling and measurement, dead time,

detector efficiency, nonlinearity, beam instability, gamma line intensity, self-absorption, gamma coincidence summing, nonpoint-like source

13

Experimental results on 235U 91Sr, 97Zr, 131I, 133I, 135I, 143Ce, 112Ag, 115Cd

radial production after section № 2

14

0

10

20

30

40

50

natU(n,f)91Sr z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

10

20

30

40

50

238U(n,f)91Sr z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

50

100

150

200

250

300

235U(n,f)91Sr z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

Experimental results on 235U 91Sr, 97Zr, 131I, 133I, 135I, 143Ce, 112Ag, 115Cd

radial production after section № 2

15

0

10

20

30

40

50

238U(n,f)131I z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

10

20

30

40

50

natU(n,f)131I z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

50

100

150

200

250

300

235U(n,f)131I z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

Experimental results on 235U 91Sr, 97Zr, 131I, 133I, 135I, 143Ce, 112Ag, 115Cd

radial production after section № 4

16

0

2

4

6

8

10

12

14

238U(n,f)91Sr z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

2

4

6

8

10

12

14

natU(n,f)91Sr z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

25

50

75

100

125

150

235U(n,f)91Sr z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

Experimental results on 235U 91Sr, 97Zr, 131I, 133I, 135I, 143Ce, 112Ag, 115Cd

radial production after section № 4

17

0

2

4

6

8

10

12

14

238U(n,f)131I z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

2

4

6

8

10

12

14

natU(n,f)131I z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

25

50

75

100

125

150

235U(n,f)131I z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

Experimental results on 235U Comparison between 91Sr and 239Pu

radial production after section № 2 and 4

18

0

100

200

300

400

500

238U(n,g)239Pu (2x-) z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

10-11 10-9 10-7 10-5 10-3 10-1 101101

102

103

104

105

106

238U(n,2n)

209Bi(n,f)

209Bi(n,xn)

238U(n,f)

238U(n,g)Cro

ss s

ectio

n (m

b)

Neutron energy (GeV)

235U(n,f)

Fundamental cross sections

JENDL-HE/2007TALYS 1.6

0

100

200

300

400

500

238U(n,g)239Pu (2x-) z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

25

50

75

100

125

150

235U(n,f)91Sr z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

50

100

150

200

250

300

235U(n,f)91Sr z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

Experimental results on 235U

19

0 20 40 60 80 100 1200

2

4

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 2 AGeV

z = 254 mm

0 20 40 60 80 100 1200

2

4

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 4 AGeV

z = 254 mm

0 20 40 60 80 100 1200

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 2 AGeV

z = 516 mm

0 20 40 60 80 100 1200

2

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 4 AGeV

z = 516 mm

Experimental results on p-t-v

• Inverse peak-to-valley (p-t-v) ratio for 238U using 112Ag, 115Cd isotopes in valley 0 2 4 6 8 10

100

101

102

103

104

112Pd 112Ag

Act

ivity

(s-1)

Time (days)

20

70 80 90 100 110 120 130 140 150 160

0

1

2

3

4

5

6

7143Ce

135I133I

131I

115Cd

112Ag

97Zr

Yie

ld (

%)

Mass number

150 MeV 100 MeV 50 MeV 1 MeV

91Sr

TALYS 1.4

238U • Mean neutron energy in dependence on mass distribution of fission products

Experimental results on p-t-v

21 0 20 40 60 80 100 120

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

112 A

g in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce

112Ag inverse peak-to-valley ratio

Ed = 2 AGeV

z = 516 mm

0 20 40 60 80 100 1200.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

112 A

g in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce

112Ag inverse peak-to-valley ratio

Ed = 4 AGeV

z = 516 mm

0 20 40 60 80 100 1200.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

112 A

g in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce

112Ag inverse peak-to-valley ratio

Ed = 2 AGeV

z = 254 mm

0 20 40 60 80 100 1200.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

112 A

g in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Radius (mm)

91Sr 97Zr 131I 133I 135I 143Ce

112Ag inverse peak-to-valley ratio

Ed = 4 AGeV

z = 254 mm

Experimental results on axial production at R ≈ 20 mm

22 200 300 400 500 600 700

0

2

4

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Longitudinal distance (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 2 AGeV

r ~ 20 mm

200 300 400 500 600 7000

2

4

6

8

10

12

14

235 U

fis

sion

in na

t U (

%)

Longitudinal distance (mm)

91Sr 97Zr 131I 133I 135I 143Ce 112Ag 115Cd

Relative fission contribution of 235U in natU

Ed = 4 AGeV

z ~ 20 mm

200 300 400 500 600 700

0.2

0.3

0.4

0.5

115 C

d in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Longitudinal distance (mm)

91Sr 133I 97Zr 135I 131I 143Ce

115Cd inverse peak-to-valley ratio

Ed = 2 AGeV

r ~ 20 mm

200 300 400 500 600 7000.2

0.3

0.4

0.5

0.6

115 C

d in

vers

e pe

ak-t

o-va

lley

ratio

(-)

Longitudinal distance (mm)

91Sr 133I 97Zr 135I 131I 143Ce

115Cd inverse peak-to-valley ratio

Ed = 4 AGeV

r ~ 20 mm

Experimental results on 209Bi

23

0.0

0.5

1.0

1.5

2.0

209Bi(n,4n)206Bi z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.8

1.2

1.6

2.0

2.4

Rat

io R

E2/R

E1

(-)

Radius (mm)

0.00

0.05

0.10

0.15

0.20

0.25

0.30

0.35

0.40

209Bi(n,4n)206Bi z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.8

1.2

1.6

2.0

2.4

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

2

4

6

8

10

12

14

209Bi(n,x)200Pb z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

1

2

3

4

209Bi(n,x)200Pb z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

2

4

6

8

10

12

14

16

18

20

209Bi(n,x)199Tl z = 254 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.81.01.21.41.61.82.0

Rat

io R

E2/R

E1

(-)

Radius (mm)

0

1

2

3

4

5

209Bi(n,x)199Tl z = 516 mm

2 AGeV 4 AGeV Exp fit Exp fit

Rea

ctio

n R

ate

(1E-2

8∙A

GeV

-1)

0 20 40 60 80 100 1200.8

1.2

1.6

2.0

2.4

Rat

io R

E2/R

E1

(-)

Radius (mm)

No fission registered

Conclusion • Contribution of 235U(n,f) up to approx. 15%

• Constant dependence on Ebeam / slight increase in 238U fission, decrease in 239Pu production and fission of 235U

• Peak-to-valley ratio corresponds to results on spatial distribution of 235U(n,f) fission

• Increase in 209Bi(n,xn) reaction rate f (Ebeam)

Information about the behavior of neutron spectrum inside the target

Future plans • Experiments at BURAN (20t natU)

need to be realized in future (2015)

• QUINTA @ Phasotron Ep = 660 MeV:

• Neutron spectrum measurements with a set of 235,238U, Bi, Au, Y, Co, Al mono-isotope activation detectors

(improvement of measurement methods)

• TIMEPIX Si pixelated detectors

500 kg

20 tons