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Discharge Plasmas of Molecular Gases / J ¥4~r~~~: 'o j~ ~7 ~,~U;~I u t= ~]f~LL*~ ~~~~~~; 4. Isotope Separation in Discharge Plasmas of Molecular Gases EZOUBTCHENKO, Alexandre N.t, AKATSUKA Hiroshi and SUZUKI Masaaki Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, Tokyo 152-8550, Japan (Received 25 December 1997) Abstract We review the theoretical principles and the experimental methods of isotope separation achieved through the use of discharge plasmas of molecular gases. Isotope separation has been accomplished in various plasma chemical reactions. It is experimentally and theoretically shown that a state of non- equilibrium in the plasmas, especially in the vibrational distribution functions, is essential for the isotope redistribution in the reagents and products. Examples of the reactions, together with the isotope separ- ation factors known up to the present time, are shown to separate isotopic species of carbon, nitrogen and oxygen molecules in the plasma phase, generated by glow discharge and microwave discharge. Keywords: isotope separation, vibrational nonequilibrium, glow discharge, microwave discharge, plasma chemistry 4.1 Introduction isotopic species will be redistributed between the rea- Plasmas generated by electric discharge of molecu- gents and the products. We can elaborate a new lar gases under moderate pressures (10 Torr < p < method of the plasma isotope separation for light ele- 200 Torr) are usually in a state of nonequilibrium. We ments . can define various temperatures according to the kine- There were a few experimental studies of isotope tics of various particles in such plasmas, for example, separation phenomena in the nonequilibrium electric electron temperature ( T*), gas translational temperature discharge. Semiokhin et al. measured C02 enrichment ( To), gas rotational temperature ( TR) and vibrational in i3C02 and 12C160180 with a separation factor a ~ temperature ( Tv), where the relationships T* > Tv ;~ 1.01 in the C02 Silent (barrier) discharge in the pres- TR- To usually hold. Especially pronounced non- sure range of 100 - 760 Torr [2]. They measured 02 equilibrium in found in the plasmas of N2, C02 and CO enrichment in 180 with a = 1.09 through dissociation discharges. The high vibrational temperature. can acti- of C02, and nondissociated C02 enrichment in 13C vate some endothermic reactions of the molecules listed with (x = 1.024 in the glow discharge plasma of pure above, and at the same time, Iower To Prevents reversal C02 (30 - 100 Torr). They also observed relatively high exothermic reactions, which can not be activated by (oe - 1.10) ozone enrichment in 180 during ozone syn- vibrations. Since isotopic species of these gases have thesis in the 02 Silent discharge under 760 Torr [3]- different vibrational quanta, they can have different The latter seems to be profitable for oxygen isotope en- vibrational distribution functions (VDF). This phe- richment because of relatively small energy cost of nomenon is similar to the Treanor effect in the VDF of ozone molecule ( - 15 - 20 eV) in the industrial anharmonic oscillators [ I J . It can result in the different ozonizers. There were, however, no further investiga- rate constants of endothermic reactions, therefore the tions in this field. The silent discharge in the molecular tPresent Address: Laboratory of New Methods of Isotope Separation, Molecular Physics Institute. Russian Research Center Kurchatov Institute, Kurchatov Sq. 1, 123182, Moscow, Russia corresponding authorb e-mail: hakatsuk@ nr. titech. ac.jp 233 ~~ ;~7 ･ ~~~~~~A~i'~~~~~-~"~* 1998~~ 3 ~ gases provides a nonequilibrium condition ( T. >> To), but the role of vibrations was not elucidated. 1 .O The important role of vibrations in the gas dis- 0.9 charge became clear when the CO and C02 plasmas were discovered to be active media for infrared lasers. 0.8 :~ It was established both theoretically and experimentally O, (DL 0.7 :: that CO, C02 and N2 can be easily vibrationally excited O = 0.6 by an electron impact in the glow discharge with a high O 1'L rate constant k*v * 10-8 cm3/s at T* -- I - 2 eV. A G,O 0.5 a, resonance exchange of vibrational quanta between the ~- O 0.4 same molecular species usually has the rate constant E ~:O kvv * 10-11 _ 10-9 cm3/s, which is much larger than C:IO 0.3 L that of vibration-to-translation energy transfer kvT * LL 0.2 10-19 _ 10-14 cm3/s. It is the fundamentals for the vi- brationally nonequilibrium state in the gas discharge 0.1 with an appropriate pressure and an ionization degree. 0.0 0.1 4.2 Basic qualitative concepts of possible sep- Reduced electric1 .O field I E/N0.0 [ 10-16 v cm2] aration phenomena in the vibrationally 0.35 1.0 1.5 2.5 3.5 nonequilibrium gas discharge plasmas Average electron energy T* [ eV J In discharging plasmas of diatomic or triatomic ga- Fig. I Channels of electron energy loss in C02 electric dis- seous molecules, it is well-known that it is possible to charge: I - C02 rotations, 2 - C02 vibrations, 3 - ex- direct most of the electron energy into the molecular vi- citation of electron levels and ionization. brational energy, by adjusting the reduced electric field E/N into the range of (2 - 6) X 10-16 V ･ cm2 [4]･ For example, the energy balance of the electrons in the C02 plasma is shown in Fig. I as a function of E/N, which 10+16 controls T*. A rate constant of the excitation of the co -'~ lower lying vibrational levels of C02 by an electron im- ~o I0+15 pact is estimated to be k*v = 10-8 cm3/s at T* = I eV. ~~, We can estimate kvv to be 10-9 cm3/s at To = 300 K F~ OH I0+14 12C160 for lower lying vibrational levels of C02 and kvT ~ 11:; c~ 10-14 cm3/s for the fastest process of C02 v2 bending ,~Ff P~o l0+13 mode. Therefore some kinds of a vibrational population p~ 13C160 distribution will be formed with Tlo = (hv)/(kln(No/ F: L~3Ho I n+'^2 N1)) >> To, where h is the Planck constant, k is the c~; Iv :H Boltzmann constant, N1 and No are the number den- 12C180 ~*H> sities of the population of the first excited vibrational l0+11 level and of the ground state, respectively. For a dia- o 5 Io 15 20 25 30 35 V tomic gas CO, such a VDF was experimentally vibration level measured up to the 40th vibrationally excited level. As Fig. 2 The CO vibrational distribution function (VDF) in the an example, the VDF's for the components of 12C160, CO - N2 - He giow discharge. E/N * 10-16 V･cm2, To 13C160 and 12C180 are shown in Fig. 2 [5]. We can see * 100 K, T~o = 2,000 - 3,000 K. that they are not Boltzmann distributions, but that each of them has a plateau for (5 - 7) < v < (30 - 40), We have to consider more complicated systems of where v is the vibrational quantum number. Such char- the vibrational excitations in triatomic gaseous mole- acteristics of the VDF are determined by the anhar- cules, since they have plural vibrational modes. Bailly et monicity of molecular vibrations. The drop with the al. measured a VDF for the C02 v3 asymmetric mode angle - 1/To in the populations of the highly excited in the glow discharge of the mixture of C02 - N2 - He levels appears when kvT' which is proportional to v, for a C02 Iaser up to v3 ~ 10 [6]. They showed that an becomes larger than kvv' observed VDF slightly deviated from the Boltzmann 234 /i'4~~i~ 4. Isotope Separation in Discharge Plasmas of Molecular Gases Ezoubtchenko, ~i~~~~ ~^.~~ N 13 16 Nv mA > mB 1 E-1 V( C O) NVIll2r L 16nvl l No NOA << N.^_~ KB << KVT ,: Ea E'a :SO '~' A :, l S ,l ll2Cl60 I11) t ~'10 O Cl SO a [ nat'Jrat= C: :~!O 1 E-2 af B ,:L N 12 18 > V( C O) :-O ~5 N 12 16 ,S V( C O) 15 O: nClsO 2 1 10 '2CldO) -3 [ '1'~ral= vibratiOn level V 1 E-3 10 Fig.4 Vibrational distribution functions in the isotopic vibration level mixture of diatomic molecules for a not rapid O 20 30 40 chemica] reaction. E~ denotes the activation energy. Fig. 3 Relative vibrational populations of heavier isotopic components in a glow discharge in the mixture CO - N2 - He. transferred through a quasiresonance energy exchange, which is called a V - V' quasiresonance exchange, simi- distribution in the region of v3 * 7 - 8. lar to the exchange among anharmonic oscillators, but Belenov et al. first suggested the possibility of ap- with a larger resonance defect. A qualitative diagram of plication of the vibrational nonequilibrium for isotope a possible VDF for the not rapid chemical reaction is separation [7]. Subsequently, the difference in a VDF shown in Fig. 4, where Ea and Ea' are the possible acti- for isotopic species of diatomic gaseous molecules, such vation energy of the reaction. The activation energy Ea as 12C160 - 13C160 or 14Nl4N - 15Nl4N, was calculated in Fig. 4 makes the reaction products enriched in the A [8, 9]. It is shown that there will be a strong difference component. Meanwhile, the activation energy Ea' re- in the population of highly excited vibrational levels for sults in the opposite sign. isotopic components when we keep Tro >> To' Figure Concerning a rapid chemical reaction with the 3 shows the strong excess of the populations of the vi- rate constant kR, that is, when the drop of the VDF is brationally excited states for 13C160 and 12C180 in the CO - N2 - He glow discharge.
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