Journal of Nuclear and Radiochemical Sciences, Vol. 16, pp. 5-10, 2016

ArticlesThe 3rd Japan-China Academic Symposium on Nuclear Fuel Cycle, ASNFC 2015

Actinides Separation from Lanthanides Using a Liquid Ga Electrode in LiCl-KCl Melts
T. Murakamia,*, S. Kitawakib, Y. Sakamuraa, M. Iizukaa, T. Nohirac and H. KofujibaCentral Research Institute of Electric Power Industry, Tokyo, 201-8511, Japan
Japan Atomic Energy Agency, Ibaraki 319-1195, Japanc
Kyoto University, Kyoto 611-0011, Japanb

Received February 7, 2016; Accepted October 11, 2016
A novel pyroprocess is proposed to recover actinides from spent nuclear fuels, in which a liquid Ga is used as the
key electrode material to achieve a high actinide/lanthanide separation efficiency. To evaluate the proposed pyroprocess, it is necessary to clarify the separation performance in the system of LiCl-KCl/liquid Ga electrode. In
this study, an electrochemical actinides recovery was conducted by galvanostatic electrolysis of the liquid Ga
electrode in LiCl-KCl melts containing both actinides (U, Pu and Am) and lanthanides (Ce, Nd, La and Gd) chlorides at 773 K. The obtained Ga alloy after the electrolysis was analyzed quantitatively to calculate the separation
factors of Pu and Am based on Ce. The calculated separation factors in LiCl-KCl/liquid Ga electrode systemwere more than 10 times higher than those in LiCl-KCl/liquid Cd system.

tation concept, where a liquid Ga metal was used as the key
electrode material in molten chlorides. As shown in Figure 1,
the proposed pyroprocess consists of two steps; actinide/lanthanide separation step and actinide recovery step. At
actinide/lanthanide separation step, a metallic basket loading
spent nuclear fuels is immersed in LiCl-KCl melts and is usedas the anode. Then, the dissolution of actinides (An) containedin the fuels proceeds at the anode,

1. Introduction
Pyroprocess which utilizes molten salts and liquid metals as
the reaction media has been developed as one of the promisingprocesses for reprocessing various kinds of spent nuclear
fuels, such as metal alloys, oxides, nitrides and so on [1, 2].
Furthermore, the pyroprocess is expected to be applied in theconcept of partitioning and transmutation [3]. In this concept,
long half life nuclides such as TRUs (Pu, Np, Am and Cm) arerecovered from spent nuclear fuels and high level liquid waste(HLLW) to be transmuted to stable or short half life nuclides.
Thus, the reduction of an environmental burden of spent
nuclear fuels is expected to be accomplished, which is a crucial challenge in the world. Since spent nuclear fuels and
HLLW contain fission products as well, such as lanthanides,
alkali metals, alkaline earth metals and noble metals, a recovery of TRUs and a separation from the fission products mustbe achieved at the same time in this concept. It is especially
important to separate TRUs from lanthanides because chemical proper ties of lanthanides are similar with those ofactinides.
In the previous study [4], the authors proposed a novel pyroprocess which can be applied in the partitioning and transmu-

An → An3+ + 3e-

The fission products of lanthanides, alkalis and alkaline earths
dissolve at the same time to form their cations and accumulate
in the melts, while noble metal fission products remain in theanode basket to be separated from actinides. At the cathode,actinides are selectively deposited into a liquid Ga to form
An-Ga alloy,
An3+ + 3e- → An in Ga

Actinide recovery step

An-Ga
An-Ga

Spent nuclear fuel(An, RE, AL, ALE)

(2)

Then, actinides are recovered from An-Ga alloy at the actinide
recovery step. Here, the recovery of actinides from An-Ga
alloy by the distillation of the Ga is not reasonable as an indus-

Actinide/Lanthanide separation step

An3+

(1)

An-Ga

An3+

An-Cd

Cd distillationGa
An recovery
LiCl-KCl

REn+, AL+, ALE2+

LiCl-KCl

Figure 1. The concept of the proposed pyroprocess to recover actinides separating from fission products in LiCl-KCl melts 4. An: actinides, RE:
rare earths, AL: alkali metals, ALE: alkaline earth metals.
*1Corresponding author. E-mail: m-tsuyo@criepi.denken.or.jp,
fax; +81334807956© 2016 The Japan Society of Nuclear and Radiochemical Sciences
Published on Web 10/31/2016

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J. Nucl. Radiochem. Sci., Vol. 16, 2015

Murakami

trial process because of the very high boiling point of Ga (2673
K). Thus, electrochemical de-alloying reaction is applied at
the actinide recovery step. When the formed An-Ga alloy
electrode is used as the anode, actinides in An-Ga alloy are
anodically dissolved,
An in Ga → An3+ + 3e-(3)A liquid Cd cathode is used to deposit actinides as An-Cd
alloys,An3+ + 3e- → An in Cd(4)

The liquid Cd cathode has been conventionally used for agroup recovery of actinides at the pyroprocess [1, 2]. By distilling Cd of the An-Cd alloy, the actinides are finally recovered [5]. The liquid Ga after the actinides recovery step isused again as the cathode material at the actinide/lanthanide
separation step. As repeating the two steps, the concentrationsof the fission products, such as lanthanides, alkalis and alkaline earths, increase in the melts at the actinide/lanthanide
separation step. Thus, a part of the melts is periodicallytreated by zeolite to remove the fission products [6]: The fission products are adsorbed and/or occluded in the structure ofzeolite.
In order to evaluate the actinide/lanthanide separation efficiency of the proposed pyroprocess, it is necessary to investigate the elect rochemical deposition of actinides andlanthanides at a liquid Ga electrode. However, the studies on
the electrochemical behavior of a liquid Ga electrode in LiClKCl melts were limited. Thus, in the previous study, theauthors first measured the following basic properties of a liquid Ga electrode in LiCl-KCl melts [4];(1) the electrochemical window of the liquid Ga electrode,(2) the potentials for binary alloy formation at 773 K; U-Ga
(U3+ + 3e - → U in Ga , 1.55 V(vs. Li+/Li)), Pu-Ga (Pu 3+ +3e - → Pu in Ga, 1.4 V), Ce-Ga (Ce3+ + 3e - → Ce in Ga, 1.3
V), Nd-Ga (Nd3+ + 3e- → Nd in Ga, 1.3 V) and Li-Ga (Li++ e- → Li in Ga, 1.1 V),(3) the current efficiency (~100 %) for the binary alloys formation and their de-alloying and(4) the activity coefficient of U, Pu, Ce and Li in liquid Ga.
In the present study, based on the above basic properties,
two runs of the electrochemical actinides recovery were conducted using the liquid Ga electrode in the LiCl-KCl melts
containing both actinides and lanthanides chlorides at 773 K.
Then, the separation factors, which are inevitable to evaluate
the proposed pyroprocess quantitatively, were calculated.
Here, the distribution factor of element M (DFM) is defined by
the following equation,
DFM = (XM in Ga)/(XM in melts)

is defined by the ratio of DFM to DFCe,SFM = (XCe in melts)/(XM in melts)/(XCe in Ga)×(XM in Ga)(6)

The experiments of the equilibrium distribution of actinides
and lanthanides between the LiCl-KCl melts and liquid Ga
were also performed to calculate the separation factors at theequilibrium state which were compared with those obtained
from the electrochemical actinides recovery experiments.
2. Experimental
All experiments were carried out in an Ar glove box with apurification system. Concentrations of impurities were kept tobe low in the glove box (oxygen < 20 ppm, water < 10 ppm). A
eutectic mixture of LiCl-KCl (58.8:41.2 mol%, 99.9 % purity,m.p. 625 K) containing lanthanide chlorides and/or actinidechlorides were loaded in an alumina crucible (SSA-S, Nikkato
corp.) and melted at 773 K. Ga metal (99.9999 % purity) was
also loaded at the bottom of the crucible in the case of theequilibrium distribution experiments. The weights of the
LiCl-KCl melts and Ga metal used at the equilibrium distribution experiments (RUN1 and 2) and the electrochemical
actinides recovery (RUN3 and 4) are summarized in Table 1.
Table 2 lists the initial concentration of actinides and lanthanides in the LiCl-KCl melts. As seen in Figure 2, for theelectrochemical measurements, the working electrodes were a
Ta wire (1 mm diameter, 99.95 % purity) electrode and a liquid
Ga electrode. The liquid Ga electrode consisted of Ga metal(99.9999 % purity) loaded in an alumina crucible (SSA-S,
inner diameter 13 mm, Nikkato corp.) with the lead of a Ta
wire which was covered by an alumina insulator not to contact
with the LiCl-KCl melts. The reference electrode was Ag+/Ag
reference electrode: LiCl-KCl-1wt%AgCl and a Ag wire (1mm diameter, 99.99% purity) as the lead were loaded in a
Pyrex tube with a thin bottom wall. All potentials presented
were calibrated to the potential of Li metal deposited electrochemically on a Ta wire in the LiCl-KCl melts, which was-2.405 V vs. Ag+/Ag. A liquid Cd-0.1wt%Li alloy was used as
the counter electrode material where a following reaction was
expected to occur,
Li in Cd = Li+ + e-

(7)

TABLE 1: Weights of the LiCl-KCl melts and Ga metal
used at each RUN(5)

where XM in melts and XM in Ga represent the concentration of element M in the LiCl-KCl melts and in the liquid Ga, respectively. The separation factor of element M based on Ce (SFM)

LiCl-KCl melts /g

Ga metal /g

RUN1

65.01

198.99RUN2

20.56925.072RUN3202.7612.004RUN4202.7612.243

TABLE 2: The initial concentrations of actinides (U, Pu and Am) and lanthanides (Ce, Nd, Gd, La, Pr and Eu) in the LiClKCl melts in mol% at each RUN
U
RUN1

6.21×10Pu-1

7.24×10Am-1

2.54×10

Ce
-2

RUN2

Nd

3.69×10
9.78×10

-1

-2

Gd

Pr

Eu

1.02×10 -1

1.09×10 -1

8.44×10 -2

8.22×10 -2

3.61×10-2

3.67×10
9.61×10

La

-1

-1

RUN3

4.32×10 -3

2.25×10 -1

9.22×10 -3

7.34×10 -2

6.77×10 -2

6.82×10 -2

7.28×10 -2

RUN4

3.82×10 -3

2.23×10 -1

8.25×10 -3

7.58×10 -2

6.97×10 -2

7.01×10 -2

7.57×10 -2

J. Nucl. Radiochem. Sci., Vol. 16, 2015

Actinides Separation from Lanthanides Using a Liquid Ga ElectrodeHNO3 before the quantitative analysis.

Ar glove box

3. Results and discussion

(c)
(b)

(d)

3.1. Equilibrium distribution of actinides and lanthanides in LiCl-KCl/liquid Ga system. Two runs of equilibrium distribution experiments were carried out at 773 K.
Initially, the LiCl-KCl melts contained lanthanides and/or
actinides (see Table 2), while no actinides and lanthanides
were contained in the liquid Ga phase at the bottom of the crucible. Ga-3.8wt%Li alloy was then added to the LiCl-KCl
melts as the reductant to proceed the following reaction,(a)M3+ + 3Li in Ga = M in Ga + 3Li+

(f)

(h)

(e)

(M: An or Ln)(8)

The added amounts of Ga-3.8wt%Li alloy at RUN1 and RUN2
corresponded to approximately 77 % of the initial amounts ofactinides in the LiCl-KCl melts and to approximately 75 % of
the initial amounts of lanthanides in the LiCl-KCl melts,
respectively, to be extracted into the liquid Ga phase. The distribution between the LiCl-KCl melts and liquid Ga phase wasconsidered to reach the equilibrium within 6 hours after the
addition of the reductant. According to the quantitative analysis results of the LiCl-KCl melts and Ga, the distribution factors and the separation factors were calculated. The calculated
values are listed in Table 3 and 4 together with the reported
values [7, 8]. The distribution factor and the separation factorof U at RUN1 and those of Eu at RUN2 could not be obtained
because the concentrations XU in melts and XEu in Ga were below thedetection limit of ICP-AES. The obtained separation factorsof Pu and Am in LiCl-KCl/liquid Ga system agreed with thosereported by Toda et al. and were confirmed to be around
10~30 times higher than those of the LiCl-KCl/liquid Cd system [7, 8]. It was also found that lanthanides distributed withthe comparable separation factors between LiCl-KCl/liquid Ga
and LiCl-KCl/liquid Cd systems [8].

(i)

(g)

Figure 2. Schematic drawing of experimental setup for electrochemical measurements. (a) Ag+/Ag reference electrode, (b) liquid
Ga electrode, (c) Ta wire electrode, (d) Cd-Li counter electrode, (e)alumina crucible, (f) LiCl-KCl melts, (g) small alumina crucible, (h)liquid Ga and (i) liquid Cd-Li.

The structure of the counter electrode was the same as theliquid Ga electrode. The electrochemical measurements were
perfor med using a potentiostat /galvanostat (H Z5000,
HOKUTO Denko Corp.). Parts of the LiCl-KCl melts and theliquid Ga alloys were sampled and analyzed by Induction coupled plasma–atomic emission spectroscopy (ICP–AES). A
gamma analysis was conducted to measure Am quantitatively.
All samples were dissolved in 1N HNO3 and/or concentrated

3.2. Electrochemical separation of actinides from lanthanides using a liquid Ga electrode. Cyclic voltammetry
was perfor med in the LiCl-KCl melts containing bothactinides (U, Pu, Am) and lanthanides (Ce, Nd, La, Gd) chlorides at 773 K to determine the electrochemical conditions for

TABLE 3: Distribution factors of actinides and lanthanides obtained at equilibrium distribution
experiments at 773 K. DFM = (XM in Ga)/(XM in melts)

RUN1

DFPu

DFAm

DFCe

DFNd

DFGd

7.3×101

2.3×101

1.9×10 -1

2.6×10 -1

7.0×10 -2

3.9

4.9

1.2

RUN2

DFLa

DFPr

9.0×10 -1

5.2

TABLE 4: Equilibrium separation factors of actinides and lanthanides based on Ce at 773 K
SFM = (XCe in melts)/(XM in melts)/(XCe in Ga)×(XM in Ga)
systemSFU
RUN1

LiCl-KCl /liquid Ga

LiCl-KCl /liquid Cd

-

SFPu

SFAm
2

3.8×10SFCe
2

1.2×10

RUN2
Reportedvalue73.0×104

2.60×102

Reportedvalue8

5.56×101

2.50×101

Reportedvalue77

1.3×101

1.12×102

7

SFNd

SFGd

SFLa

SFPr

-1

1.4

3.7×101.2

3.2×10 -1

2.3×10 -1

1.3

1.04

2.70×10 -1

3.70×10 -1

1.14

1(base)

J. Nucl. Radiochem. Sci., Vol. 16, 2015
0.1

0.005

(a1)
(a2) (a3)0.05

Current /A

Murakami

0

(a4)

0
(c2)

(c3)

Current /A

8

(c4)

-0.05
-0.1
-0.15
-0.5

-0.005-0.01-0.015

(c1)

-0.02

0

0.5

1

1.5

2

1.2

1.3

1.4

1.5

1.6

1.7

1.8

+

Potential /V vs. Li /Li+

Potential /V vs. Li /Li
Figure 3. Cyclic voltammogram of a Ta wire electrode in LiCl-KCl
melts containing actinides (U, Pu and Am) and lanthanides (Ce, Nd,
La and Gd) chlorides at 773 K. Concentrations of U, Pu, Am, Ce,
Nd, La and Gd in the melts were 5.99×10 -3, 2.32×10 -1, 9.64×10 -3,
7.42×10 -2, 7.02×10 -2, 7.24×10 -2 and 6.83×10 -2, respectively, in mol%.
Scan rate was 100 mV s-1.

Figure 4. Cyclic voltammogram of a liquid Ga electrode in LiClKCl melts containing actinides (U, Pu and Am) and lanthanides (Ce,Nd, La and Gd) chlorides at 773 K. Concentrations of U, Pu, Am,
Ce, Nd, La and Gd in the melts were 3.82×10 -3, 2.23×10 -1, 8.25×10 -3,
7.58×10 -2, 6.97×10 -2, 7.57×10 -2 and 7.01×10 -2, respectively, in mol%.
Scan rate was 10 mV s-1.

actinides/lanthanides separation using a liquid Ga electrode.
Figure 3 shows a cyclic voltammogram of a Ta wire electrodein the melts. Several cathodic current rises and their corresponding anodic peaks are observed in the cyclic voltammogram. The cathodic current rise, c1, and the anodic current
peak, a1, observed at around 0 V (vs. Li+/Li) were ascribed to
Li metal deposition (reaction 9) and its dissolution (reaction10), respectively,

metals deposition seemed to overlap the cathodic current
increases of c3 and c2, respectively,

Li+ + e- → Li

(9)

Li → Li+ + e-

(10)

The cathodic current increases from approximately 0.45 V (c2)and the corresponding anodic current peak is observed ataround 0.6 V (a2). The former current increase corresponded
to the lanthanide metal deposition (reaction 11) and the lattercurrent peak to the reverse reaction (reaction 12), respectively[9, 10].
Ln3+ + 3e- → Ln
Ln → Ln3+ + 3e-(Ln: La, Ce, Gd)

(11)
(12)

The small cathodic current increases from approximately 0.74
V (c3) and 0.90 V (c4) were considered to be due to the deposition of Pu (reaction 13) and U (reaction 14) metals, respectively[11, 12].
Pu3+ + 3e- → Pu

(13)

U3+ + 3e- → U(14)

The anodic current peak (a3) and current shoulder (a4) wereconsidered to be ascribed to the dissolutions of Pu (reaction15) and U (reaction 16) metals, respectively [11, 12].
Pu → Pu3+ + 3e-(15)

U → U3+ + 3e-(16)

Concerning Am and Nd, of which divalent cations are stable in
the LiCl-KCl melts, complicated electrochemical behaviors
have been proposed. According to the reports [13, 14], thecathodic current for Am (reaction 17) and Nd (reaction 18)

Am2+ + 2e- → Am

(17)

Nd3+ + 3e- → Nd

(18)

The anodic current for the dissolution of Am, the reverse reaction of reaction 17, could be considered to overlap peak a3 [13].
The formations of their divalent cations were considered toproceed from the potential approximately 0.2 V more positive
than their metal deposition potentials [13, 14].
Am3+ + e- → Am2+

(19)

Nd3+ + e- → Nd2+

(20)

Cyclic voltammetry was also carried out using a liquid Ga
electrode in the melts. As shown in Figure 4, a cathodic current starts to increase from around 1.5 V. As mentioned above,in our previous study [4], the potentials of binary Ga alloy formation for U-Ga, Pu-Ga, Ce-Ga, Nd-Ga and Li-Ga were foundto proceed at lower potential than 1.55 V, 1.4 V, 1.3 V, 1.3 V
and 1.1 V, respectively. Therefore, the cathodic current
observed in Figure 4 corresponded to actinides-Ga alloy formation (reaction 2). Furthermore, the corresponding anodic
peak at 1.43 V in Figure 4 was due to the de-alloying reaction(actinides dissolution from the alloy (reaction 3)). Our previous study also showed that the liquid Ga dissolution (reaction21) proceeded at more positive potential than 1.85 V [4],Ga → Ga3+ + 3e-(21)

The large potential difference between the actinide dissolution
and the Ga dissolution suggested that de-alloying at the second
step of the proposed process (Figure 1) would proceed without
any Ga loss by controlling the anodic potential below 1.85 V.
Two runs of actinides recovery were conducted using a liquid Ga electrode in the LiCl-KCl melts containing bothactinides and lanthanides chlorides. The electrolysis condition
was determined based on the results of cyclic voltammetry(Figure 4); galvanostatic electrolysis at -6 mA at RUN3 and-20 mA at RUN4 for group recovery of actinides with a limited lanthanides deposition. The electrolysis was stopped
before the concentration of actinides in the liquid Ga reachedJ. Nucl. Radiochem. Sci., Vol. 16, 2015

Actinides Separation from Lanthanides Using a Liquid Ga Electrode
1.48

TABLE 5: Distribution factors of actinides and lanthanides obtained at electrochemical recovery of actinides
at 773 K. DFM = (XM in Ga)/(XM in melts)

1.44

Potential /V vs. Li+/Li

9

DFU
1.4

1.36

DFPu
-1

RUN3

1.7×10

RUN4

2.2×10 -1

DFAm-2

2.6×10 -2

1.1×10 -1

6.9×10 -2

6.3×10(a)

1.32

TABLE 6: Non-equilibrium separation factors of actinides
based on Ce
SFM = (XCe in melts)/(XM in melts)/(XCe in Ga)×(XM in Ga)

(b)

SFU

SFPu

SFAm

RUN3

>1.2×103>4.2×102>1.8×102

RUN4

2

2

2

1.28
0

500

1000

1500

2000

2500

Time /s
Figure 5. The liquid Ga electrode potential developments during
electrochemical actinides recovery experiments. (a): galvanostatic
electrolysis using the liquid Ga electrode at -6 mA in LiCl-KCl melts
at 773 K at RUN3. Concentrations of U, Pu, Am, Ce, Nd, La and Gd
in the melts were 4.32×10 -3, 2.25×10 -1, 9.22×10 -3, 7.34×10 -2, 6.77×10 -2,
7.28×10 -2 and 6.82×10 -2 , respectively, in mol%. (b): galvanostatic
electrolysis using the liquid Ga electrode at -20 mA in LiCl-KCl
melts at 773 K at RUN4. Concentrations of U, Pu, Am, Ce, Nd, La
and Gd in the melts were 3.82×10 -3, 2.23×10 -1, 8.25×10 -3, 7.58×10 -2,
6.97×10 -2, 7.57×10 -2 and 7.01×10 -2, respectively, in mol%.

their solubility (0.034 mol%-U at 772 K [15], 0.17 mol%-Pu at
773 K [16]). The passed electrical charges at RUN3 and RUN4
were 12.1 C and 14.1 C, respectively. These values corresponded to 0.024 mol%-actinides and 0.028 mol%-actinides
recovered in the liquid Ga at RUN3 and RUN4, respectively,
under the assumption of 100 % current efficiency. As shownin Figure 5, the potential shifts gradually to the negative direction along with the electrolysis time indicating the concentration increase of actinides in the liquid Ga. It was noticed thatduring the electrolysis the potential of liquid Ga electrode was
kept at higher than the lanthanide-Ga alloy formation potential; 1.3 V for Ce-Ga and Nd-Ga alloys as shown in our previous study [4]. Thus, actinides were expected to be recoveredas actinides-Ga alloy more preferentially than the lanthanidesGa alloy. The liquid Ga electrode was removed from the melts
just after ending the electrolysis. Then, parts of Ga alloys
were sampled and analyzed quantitatively to calculate the distribution factors and the separation factors. Table 5 and 6 list
the calculated values. The separation factor of U was higher
than that of Pu and Am, indicating the preferential recovery of
U in liquid Ga among actinides. High separation factors of Pu
and Am were achieved by using the liquid Ga electrode.
These values were more than 10 times higher than the separation factors of the LiCl-KCl/liquid Cd system (see Table 4). It
seemed that the separation factors of Pu and Am were close to
those obtained from the equilibrium distribution experimentsin the LiCl-KCl/liquid Ga system, while the separation factorsof U were considered to be different between the electrochemical actinides recovery and equilibrium distribution; lower at
non-equilibrium state (electrochemical actinides recovery
experiment in this study) than at equilibrium state (equilibrium distribution experiment reported by Toda et al. [7]). The
lower value at non-equilibrium state could be explained by thesmaller amount of U in the liquid Ga electrode due to the limitation of diffusion of U in the LiCl-KCl melts or in the liquid
Ga phase during the electrolysis. Further investigation isrequired to clarify the effect of the electrolysis conditions on
the non-equilibrium separation factors.

>4.5×10>2.2×10SFCe>1.4×101(base)

Since XCe in Ga was below detection limit of ICP-AES, SF M
was evaluated using the lower detection limit of Ce.

4. Conclusion
Galvanostatic electrolyses were performed using a liquid Ga
electrode in the LiCl-KCl metls containing both actinides andlanthanides chlorides at 773 K to recover actinides in the liquid Ga with limited amounts of lanthanides codeposition. The
obtained results confirmed that the separation factors of Pu
and Am based on Ce at non-equilibrium state were more than
10 times higher than those of the LiCl-KCl/liquid Cd system.
Thus, liquid Ga was confirmed to be a promising electrodematerial to recover actinides. The proposed pyroprocess using
a liquid Ga electrode was likely to have a higher TRUs (Pu andminor actinides)/lanthanides separation efficiency comparedto the conventional pyroprocess where a liquid Cd electrode isused for the group recovery of actinides. As the future study,
the separation factors of other minor actinides, Np and Cm,should be measured.
Acknowledgement
This paper is the results of “Novel pyroprocess with a highseparation efficiency of actinides from lanthanides” entrusted
to Central Research Institute of Electric Power Industry(CRIEPI) by the Ministry of Education, Culture, Sports,
Science and Technology (MEXT). The authors would like toexpress their appreciation to Mr. H. Tanaka for his great
efforts on the presented works.
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