Ionic valence change of metal ions by ns and fs lasers applicable for nuclear waste treatment
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1 Ionic valence change of metal ions by ns and fs lasers applicable for nuclear waste treatment Nobuaki Nakashima Toyota Physical and Chemical Research Institute, Nagakute, Japan Toyota Central R&D Labs., Inc., Fundamental Physics to Societal Applications Conference, Tokyo Japan, Nov.18-19(2013) Outline -1. What is an ionic-valence-change? Examples by UV & fs laser excitation -2. Useful for a decrease in nuclear waste -3. Two-color, two-photon Yb 3+ Applicable to Np, Am ions -4. Induced by femtosecond filamentation: Me n+ +e - Me (n-1)+, Me=Eu, Sm, Yb, Fe, Ag -5. Thorium atomic energy 1
2 -1. Ionic valence change by UV laser excitation Eu 3+ Eu 2+ by XeCl (308 nm) laser irradiation Lumi. Fluo. Precip. 40 mj/pulse, 15 Hz, 1) 1s, 2) 30 s, 3) 30 min Ionic valence changes by UV laser / ns two-photon / fs filamentation 248 nm Sm 3+ Sm 2+ Eu 3+ Eu nm, UV, ns, fs 3000 shots, 50mJ/pulse UV, fs Yb shots 0.8 m, fs UV, ns, fs 1) 10 shots 2) 40 shots 3) 6000 shots 308 nm (37 mjcm -2 ) 1.2 m fs 0.8 m, fs shots 10 J/pulse shots 5 J/pulse Ce 3+ UV Fe 3+ Fe 2+ UV, fs Ag + Ag + n UV, fs 2
3 -2. Useful for a decrease in nuclear waste Metal ions are separable after ionic valence change by precipitation & extraction -ray & neutron, in Fusion & Th reactors Separation is first. Using laser A small increase in waste Samples can be remotely irradiated. Waste solution is not transparent for deep UV. NUV, Vis and/or NIR lasers should be. xx M : Elements seen in U-type nuclear waste xx M :Photo-reactive elements among them H He Li Be B C N O F Ne Na Mg Al Si P Se Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe Cs Ba La Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn Fr Ra Ac Du Jo Rf Bh Ha Mt Lanthanide Actinide La Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Ac Th Pa U Np Pu Am Cm Bk Cf Es Fm Md No Lr 3
4 Yb 3+ :Simple electronic structure The mechanism will be clarified. Reactive levels: CT, Non-Reactive levels:f electronic excited states Two-photon reaction & Yield Sm: Nishida, et al., J. Phys. Chem. A 2010, 114, Eu:Nakashima, et al.,. J. Phys. Chem. 1999, 103, Two photon reaction: IR pulse first, later UV pulse resettability 14 ns IR UV t
5 [ ] I UV, I IR Abs./ 0.4 cm I UV 0.17, I IR 4 mj/pulse, 10Hz Wavelength/nm [ ] I UV I IR 12 min 6 3 Weak I UV 3 min, High I UV 0.5 min. 6 Abs. [Yb 2+ ]/0.4 cm Abs.[Yb 2+ ]/0.4 cm Yb 2+ Formation vs. I UV ( I IR IR I 44 mj) I (355 nm) / mj/pulse Yb 2+ Formation vs. I IR I UV 0.12mJ I IR ( 976 nm)/ mj Two photon Yb 3+ has been obsd. CT 4f* absorption, reaction yield, (Yb 3+ )* lifetimes CT (Yb 3+ )* Yb nm 355 nm nm nm 0.2 s 367nm 450 nm N. Nakashima, K. Yamanaka, T. Yatsuhashi, J. Phys. Chem. A, 117 (2013)
6 Shifts of energy sources to renewable ones, but nuclear waste remains. Atomic energy bases : until 2030? How and what we can do for the waste? Introduce Th, TWR? One Through Started in Olkiluoto, Finland Onkalo waste repository Geological Disposal is Japan s choice and the reprocessing may start in 2014? If separate Np, Am, the amount of waste will be reduced to 1/2 and watching time will be reduced to 1/ year 1950 W t Used nuclear fuel 90 Sr(29 y) 137 Cs(30 y) 247 Np( y) 241 Am(470 y) 243 Am(7600 y) Np,Am,Cm: 27 kg/year/1 atomic plant ~ Photons 1W laser/year The curve of Th reactor is close to the blue line. 6
7 If separate Np, Am, the amount of waste will be reduced to 1/2 and watching time will be reduced to 1/ year 1950 W t Used nuclear fuel 90 Sr(29 y) 137 Cs(30 y) 247 Np( y) 241 Am(470 y) 243 Am(7600 y) Np,Am,Cm: 27 kg/year/1 atomic plant ~ Photons 1W laser/year The curve of Th reactor is close to the blue line. Two photon chemistry of Eu 3+ Eu 2+ may be applicable. Am 3+ Am 2+,4+ Two/three photon reaction of Eu 3+ Eu 2+ Nakashima, et al.,. J. Phys. Chem. 1999, 103, Reaction yield has to be re-examined, Can be extended to Am systems. Eu 3+ and Am 3+ have the same f electronic levels. LLevels, Lifetime in MeOH Ln Ac 57 La 89 Ac 58 Ce 90 Th 59 Pr 91 Pa 60 Nd 92 U 61 Pm 93 Np 62 Sm 94 Pu 63 Eu 95 Am 64 Gd 96 Cm 65 Tb 97 Bk 66 Dy 98 Cf 67 Ho 99 Es 68 Er 100 Fm 69 Tm 101 Md 70 Yb 102 No 71 Lu 103 Lr 7
8 Ready to discuss applying the laser chemistry of Eu and Yb ions to Np and Am ions If separate Np, Am, the amount of waste 1/2 and watching time 1/ t Used nuclear fuel 90 Sr(29 y) 137 Cs(30 y) 5 year 1950 W Eu 3+ Eu 2+ Yb 3+ ns two photon, femtosecond filamentation Np 5+ Np 4+ Am 3+ Am 2+,4+ Ready to discuss applying the laser chemistry of Eu and Yb ions to Np and Am ions If separate Np, Am, the amount of waste 1/2 and watching time 1/ t Used nuclear fuel 90 Sr(29 y) 137 Cs(30 y) 5 year 1950 W Eu 3+ Eu 2+ Yb 3+ ns two photon, femtosecond filamentation Np 5+ Np 4+ Am 3+ Am 2+,4+ 8
9 -4. Another method of Ionic valence change of metal ions in solution: femtoseond filametation Laser White Laser Eu 3+ Eu 2+ Sm 3+ Sm 2+ Yb 3+ Fe 3+ Fe 2+ (1.2 m) Ag + Ag n + Many Me n+ systems are worth a try for an ionic valence change by fs laser excitation. Femtosecond Laser Filamentation and related Chemistry On the same line with those Radiation Chemistry Eu 3+ + e sol- Eu 2+ Nishida, D.; Kusaba, M.; Yatsuhashi, T.; Nakashima, N. Chem. Phys. Lett. 2008, 465, 238. Ionic valence change (Me n+ ), Nano-particle (Ag n, C) Many other applications of filamentation: Rain making, Lidar, THz generation, Cancer Therapy 9
10 Eu 3+ Eu 2+ Accompanied by Generation of White-Light Laser Eu 3+ +e - Eu 2+ Ti:Sapphire Laser 0.8, 1.2 m fs The focal point was 20 mm behind the cell J/pulse LED380 ND filter f = 200 mm Spectrophotometer Off-resonant WL (800 nm irradiation Eu m - EuCl 3 in MeOH +15-crown-5 Eu 2+ detected by its fluorescence shots Chem. Phys. Lett. 465 (2008)
11 21/34 White-light laser e - formation, Eu 3+ + e - Eu 2+ Chem. Phys. Lett. 465 (2008)238. Eu 2+ Luminescence Intensity / arb. units Laser Energy / J The slope 2.9, indicating three photon reaction. Two mechanisms would be included. 5hν CH 3 OH CH 3 OH + + e - * 2hν Eu 2+ Eu 3+ 2 photon reverse shots * Liu, et al., Opt. Comm. 255 (2002)193. Solvent is ionized and the solvated electron is trapped. Eu 3+ +e - Eu 2+ Intensity dependent index self-focusing, filament, ionization, and white-light laser 0.8 m fs pulse self-focusing Eu 3+ Eu 2+ white-light laser 0.8 Small m fs refractive pulse sample index due filament to ionization defocusing /cm 3 in a filament of 5, W/cm 2 * 100 filaments/shot shots Total concentration of e M, Trap efficiency ~ 0.2 * Based on Chin et al., Can. J. Phys. 83 (2005)
12 Ionic Valence Change of Me n+ +e - Me (n-1)+ by Femtoseond Filametation 1. Me=Eu, Sm, Yb white-light laser 2. Threshold 3 J by a focused beam 3. How about transition metals? Me=Fe, Ag Chem. Phys. Lett. 465 (2008)238; J. Phys. Chem. A, 114(2010)5648; Chin. J. Phys.(Taipei) Ultrafast Intense Laser Science, submitted. (2013?) Me=Fe Fe 3+ Fe 2+ non-resonant wavelength ex. IR fs pulse 10 J 10 6 shots [Fe 3+ (C 2 O 4 ) 3 ] 3 [Fe 2+ (o-phen) 3 ] 2+ White Laser 800 nm fs pulse 12 J shots 12
13 Color change by Fe 3+ Fe [Fe 3+ (C 2 O 4 ) 3 ] 3 [Fe 2+ (o-phen) 3 ] 2+ / 10 3 M -1 cm IR fs pulse Wavelength/nm 0.8 m Two-photon, 1.2 m Femtosecond filamentation 600 Fe 3+ Fe 2+ Two photon at 0.8 m (the slope of 2.0 with no thres.) Fe 3+ + e sol- Fe 2+ at 1.2 m ( with a threshold) [Fe(II)](Abs. at 520 nm) Fe 3+ Fe m BD WL m Laser energy/ J Guiding line with a slope of Fe 3+ Fe m WL BD : Break down obsd. WL : White laser obsd Obsd. Abs. =0.00, Abs max/min. = 0.005/751= m Laser energy/ J 13
14 Color change by Ag + Ag Ag n + There was a threshold. Ag + + e sol- = Ag Ag +Ag +Ag +.. Ag + = Ag + n Ag cluster Before During After Absorbance/cm After (800 nm pulses) Before Wavelength/nm 800 nm, 100 fs, 5 J/pulse 1kHz 10min. AgClO M in H 2 O With stabilizers:2-proh, PANa Ag n + (Abs.at 1 Ag + n 0.1 WL Laser energy/ J Ionic valence changes have been realized by laser irradiation. M n+ to M m+ by ns laser two photon chemistry. At least Me=Eu, Sm, Yb, fs laser filamentation. At least Me=Eu, Sm, Yb, Fe, Ag Applied to Np and Am ions, leading to separation. Can be treated in a Th reactor. 14
15 Th atomic power: 232 Th atomic power can be compared with U-Pu type No relation to atomic bomb, Small nuclear waste, and simple treatment No severe accident like hydrogen explosion Th: enough resources U several tens years, Th>1000 years Pu can be extinct. HL waste can be burned. In USA, Oak Ridge operated , a molten salt type, 233 U changeable to 232 Th. 15
16 Conclusions Eu 3+ Eu 2+ Yb 3+ ns two photon, femtosecond filamentation Np 5+ Np 4+ Am 3+ Am 2+,4+ Collaborators: T. Yatsuhashi and K. Yamanaka Thank you for your attention! 16
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