Materials Science

SOFC, PEFC

2.indd 1

2010/06/17 13:33:19

1 2 3

PEFC

amezawa@ee.mech.tohoku.ac.jp
2

unemoto@tagen.tohoku.ac.jp
3

kawada@ee.mech.tohoku.ac.jp

1SOFC........................................ 2
1-1 ..................................................................... 2
1-2SOFC ........................................................ 2
1-2-1 .................................................................. 3
1-2-2.............................................. 3
1-2-3.............................................. 3
1-2-4 ................................................ 3
2SOFC ........................................................... 4
2-1................................................ 4
2-2 .............................................................. 4
2-2-1.................................................... 4
2-2-2................ 5
2-2-3 ....................................................... 5
3 .................................... 6
3-1 ................................................... 6
3-2 .......................................................... 6
3-3 .............................................................. 6
3-4 ..... 7
4 ................................................................................... 7
5 ............................................................................ 7

1SOFC
1-1

Polymer Electrolyte Fuel Cell, PEFC

PEFC

2009 1kW
1PEFC

Solid Oxide Fuel Cell, SOFC 2-7

2.indd 2

Materials Science

PAFC

MCFC
SOFC

Li/K, Li/Na

H+

H+

80

200

LPG

LPG

LPG

30 40

35 45

40 65

40 65

CO3-

O2-

600 700 700 1000

SOFC
12

4
5

NEF2007 1kW

2009 67 8
PEFC 42-48 LHV
SOFC
SOFC

SOFC
SOFC

1-2SOFC
1 SOFC SOFC

SOFC

1V

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:34

(a)

(b)

e-

H2O

;O

;A

O2-

;M

;B

;O

2a MO2 b ABO3

O2

H2

1 SOFC

SOFC
1kW SOFC
750 800
100kW
SOFC 1000
SOFC

SOFC
9-15

1-2-1
SOFC
ZrO2 ZrO2 1150
2370
2Zr 4
3 Y

SOFC

SOFC

CeO2 2
LaGaO3
Ce
4 Gd Sm
3

n
SOFC

La
3 Sr
2 Ga3 Mg2

Ga Co

SOFC

1-2-2
SOFC 3d
LnMO3Ln = La, Pr, Sm M = Mn,
Fe, Co

3 Sr Ca
2
SOFC
MnO3
La,SrMnO3La,Ca

SOFC
La,Sr
Co,Fe
O3

La,Sr
Co,FeO3

1-2-3
SOFC Ni
Ni

Ni Ni

1-2-4
SOFC

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 3

Materials Science

2010/06/17 13:33:34

LaCrO3
SrTiO3
SOFC

Fe-Cr Cr Ni

Cr

2SOFC
SOFC

SOFC
SOFC

16-27

2-1

954
2
3

#1000

(a)

(b)

3
4 3a

2 3b

4 2

2-2
2-2-1
2-1

l I
S V

l S
I V

SOFC

10Hz 1MHz

mV

3a4 b2

SOFC

2.indd 4

Materials Science

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:35

2-2-2

/ 5a
RC

Zi

1
1
j Ci
R
i

Ri

2 2
1 2 Ri Ci

R 2Ci
2 2
1 2 Ri Ci

i = ggbif
Ri Ci
=1/2 ff 5b 5a

5a

5b

2
Ri /2
Rb Rgb Rif

Rb
(a)

(b)

5
a
b

5b

Rb Rgb

2-2-3

SOFC

SOFC

O2
H2

Ar N2
SOFC

H2
H2 H2
H2O

H2O

H2 H2O

SOFC

SOFC

SOFC

16-23, 24-26

3-1 28-30

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 5

Materials Science

2010/06/17 13:33:35

J
C / x

t=0
Cx,y,tt=0
C0

3
D
m2 s-13

t x x x
J t x
J
x
t x
J x
C
4
34

10

C0

5
11
35
6
7

911
8
29
12

SOFC

D Dchem

3-2

8
2-1 4
2a 2b 2c

a, b << c

2.indd 6

Materials Science

Mt t
L1L2
13
14

3-3

A
M MO
A+ M2+

Krger-Vink

15

16

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:36

3.0x10

-3

17

/ Scm

1516

-1

2.5

2.0

18

V O
17

18K

>>
A'M
h

2
V O

1.5

1.0
0

500

1000

1500

2000

2500

3000

Time / sec

19

6Al:SrTiO3, 1123K, p
O2=
0.01 1bar20

h 1/4

16

3-4

3-3

16

12
30, 31

20

t t

20

D kL1,
L2, ,
Al SrTiO3
6 Al
Ti
19
3-3 AxM1-xO1-

t=0

D k 20

28-30

4
SOFC

SOFC

SOFC

5
1 http://www.
fca-enefarm.org/ 2010-4-27
2 1998
3 SOFC 2005
4 D. J. L. Brett; A. Atkinson; N. P. Brandon; S.J. Skinner, Chem. Soc. Rev., 2008, 37, 1568.
5 A. Weber; E. Ivers-Tiffee; J. Power Sources, 2004, 127, 273.
6 R. M. Ormerod, Chem. Soc. Rev., 2003, 32, 17.
7 N. Q. Minh, J. Am. Ceram. Soc., 1993, 76, 563.
8 http://
sofc.nef.or.jp/ 2010-4-27
9 K. Huang; J. Wan; J.B. Goodenough, J. Mat. Sci., 2001, 36, 1093.
10 T. Ishihara, Bull. Chem. Soc. Jpn., 2006, 79, 1155.
11 E. V. Tsipis; V. V. Kharton, J. Solid State Chem., 2008, 12, 1039.
12 E. V. Tsipis; V. V. Kharton, J. Solid State Chem., 2008, 12, 1367.
13 S. B. Adler, Chem. Rev., 2004, 104, 4791.
14 C. Sun; U. Stimming, J. Power Sources, 2007, 171, 247.
15 Z. Yang, Int. Mat. Rev., 2008, 53, 39.
16 1986
17 1990
18 P. G. Bruce ed., Solid State Electrochemistry, Cambridge University Press, 1995.
19 1995
20 1999
21 - -
2001
22 2001
23 2002
24 JIS 12 28
p. 1662002
25 7 5 2004
26 2005
27 Electrochemistry, 2006, 74, 417
28 P. G. Shewmon, Diffusion in Solids, McGraw-Hill1963.
1976
29 J. Crank, The Mathematics of Diffusion, 2nd ed., Oxford University Press1975
30 1988
31 I. Yasuda, T. HIkita, J. Electrochem. Soc., 1994, 141, 1268
32 I. Yasuda, M. Hishinuma, J. Solid State Chem., 1996, 123, 382

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 7

Materials Science

2010/06/17 13:33:36

www.sigma-aldrich.com/
alternative-jp

Lanthanum strontium cobalt ferrite, LSCF 6428

La0.6Sr0.4Co0.2Fe0.8O3

704288-10G

Lanthanum strontium manganite, LSM-20

(La0.80Sr0.20)MnO3

704296-10G

Lanthanum strontium manganite, LSM-35

(La0.65Sr0.35)MnO3

704261-10G

Lanthanum strontium cobalt ferrite composite cathode powder, LSCF/GDC

(Ce0.9Gd0.1)O1.95 : (La0.60Sr0.40)(Co0.20Fe0.80)O3 = 1 : 1

704253-10G

Lanthanum strontium manganite composite cathode powder, LSM-20/YSZ

(Y2O3)0.08(ZrO2)0.92 : (La0.80Sr0.20)MnO3 = 1 : 1

704245-10G

Lanthanum strontium manganite composite cathode powder, LSM20-GDC10

(Ce0.9Gd0.1)O1.95 : (La0.80Sr0.20)MnO3 = 1 : 1

704237-10G

Nickel oxide - Cerium samarium oxide for coatings, NiO/SDC, 99+ % trace metals basis
NiO : (CeO2 - Sm2O3) = 60 : 40

704210-10G

Nickel oxide - Yttria-stabilized zirconia (YSZ) for general applications, NiO/YSZ, 99+ % trace metals basis
NiO : (Y2O3 ZrO2) = 60 : 40

704229-10G

Nickel oxide - Yttria-stabilized zirconia (YSZ) for coatings, NiO/YSZ, 99+ % trace metals basis
NiO : (Y2O3 - ZrO2) = 66 : 34

704202-10G

Cerium(IV) oxide-gadolinium doped (GDC) nanopowder

Gd 10 mol % as dopant

572330-25G

Cerium(IV) oxide-gadolinium doped (GDC) nanopowder

Gd 20 mol % as dopant

572357-25G

Cerium(IV) oxide-samaria doped nanopowder

SmO2 15 mol % as dopant

572365-25G

Zirconium(IV) oxide-yttria stabilized (YSZ) nanopowder

Y2O3 3 % as stabilizer

572322-25G

Zirconium(IV) oxide-yttria stabilized (YSZ) nanopowder

Y2O3 8 % as stabilizer

572349-25G

Zirconium(IV) oxide-yttria stabilized (YSZ) submicron powder

Y2O3 8 % as stabilizer, 99.9% trace metals basis (purity excludes 2% HfO2)

464228-100G, 500G

Cerium(IV)-zirconium(IV) oxide nanopowder , <50 nm particle size (BET), 99.0% trace metals basis
Ce : Zr = 1: 1 (ZrO2 and CeO2 or an intermediate compound)

634174-25G, 100G

Aldrich

Materials Science

Vol.3, No.4
2Vol.4, No.4

http://www.sigma-aldrich.com/ms-jp

2.indd 8

Materials Science

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:37

1 2

(b)

(a)

tamaki.t.aa@m.titech.ac.jp

yamag@res.titech.ac.jp

1 ............................................................................ 9
2PEFC ............................................................... 9
2-1 .... 9
2-2 ................................................................... 10
3PEFC ............................................................. 10
3-1 ................................................................... 10
3-2 .......................................................................... 11
3-3MEA............................................ 11
4PEFC .......................................................... 12
4-1.............................................. 12
4-2 ............................... 12
4-2-1 ...... 13
4-2-2 ................. 13
5 .......................................................................... 14
6 .......................................................................... 15

CH3OH+H2OCO2+6H++6e-

Anode

H22H++2e-

Anode

Cathode

O2+2H++2e-H2O

Cathode 3/2O2+6H++6e-3H2O

1 PEFCa DMFCb
2

G H 1

PEFC
100

2PEFC

HHV
LHV
251
G -237 kJ/mol H -286 kJ/molHHV
83 LHV
H -242 kJ/mol 98
G -702
kJ/mol H -727 kJ/molHHV 97

G E0 2

2-1

PEFC

DMFC 1
PEFC DMFC
H+

2
n F
E 1.23 V
E 1.21 V
PEFC

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 9

Materials Science

2010/06/17 13:33:38

PEFC 50
PEFC

35 PEFC

80

15
30 40
PEFC

2-2
PEFC 2
2
EV2
A/cm
I
E0

a
IR IR
c

E0

[ V ]

a
IR
c

- MEA

3-1

3
3a 3b

Rmembrane

3c
3c R
C
Rmembrane 3
S/cm
3
cmw
l
cmdcm
l
l Rmembrane

(a)

(b)

Pt

l (cm)

Pt()
Pt
()

w (cm)

(c)
R
Rmembrane
C

l (cm)

3ab
c

[A/cm2 ]
2PEFC E0 a
IR IR c

PEFC Pt

DMFC
IR
RR
I IR I RV

PEFC

PEFC

3PEFC

10

2.indd 10

Materials Science

IECmeq/g

IEC 1 EW
g/eq
DMFC

4a H

kg
J
m-2 s-1
dQ
Am24

dt

4b

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:38

(a)

(b)

H+

e-

O2

4 :ab

4 J d
Methanol permeability
kg m m-2 h-1

Pm2/s
Cmol/m35
5
4b
Dm2/s6
6
PEFC Nafion

IEC

MEA

PEFC

ppm Fe2+

SEMTEM
X XRDX
XPS

1
IRAS XPSX XAS
in-situ
1

MEA
Pt

3-3 MEA
MEA

MEA 2
3-2
PEFC 6

3-2
PEFC Pt Pt
nm

CB
CB
nm
m
CB
5

O2

H2

6 PEFC MEA

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 11

Materials Science

11

2010/06/17 13:33:38

MRI
MEA

4PEFC
PEFC

PEFC

PEFCDMFC
120
3-1

PEFC PEFC

4-1
PEFC Nafion Flemion
-CF2-
2 7
PTFE
Nafion Flemion PTFE

3
CF 2 CF 2

CF 2 CF

O CF 2 CFO

CF 2

SO 3 H

CF3
Nafion: m>2, n=2, x=5 - 13.5, y=1000
Dow : m=0, n=2
Aciplex : m=0, 3, n=2-5, x=1.5 - 14
Flemion: m=0, 1, n=1 - 5

3 6

9, 10

11, 12
DMFC

4-2

nm

1989
13

14

DMFC

-CH2-

4, 5

6, 7

12

2.indd 12

Materials Science

Pore

Porous substrate

Filling electrolyte

Substrate
Pore-filling electrolyte membrane

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:40

4-2-1

CLPE 25 m 100 nm
PI 30 m 300 nm 2

AAVS 2-
-2- ATBS

25
9 15

3-1

AAVS
ATBS

DMFC
Nafion117

Nafion
PTFE-AA
CLPE-AA
PTFE-AAVS
CLPE-AAVS
PI-AAVS
CLPE-ATBS
PI-ATBS

2
Inverse of MeOH permeability [m h/kg m]

0.1

0.01

0.001
0.001

0.01

0.1

10 Nafion117

MEA
6

Nafion117 200 m CLPE-ATBS

25 m MEA
Pt- Ru
2 mg/cm2 Pt 1 mg/cm2
8 wt2.5 M 32 wt
10 M50 DMFC
11 CLPE-ATBS a Nafion117
b MEA DMFC 16DMFC
Nafion117 DMFC
16 wt
32 wt

Nafion117 200 m
CLPE-ATBS 25 m
16 wt 70 mW/cm232 wt 50 mW/
cm2

17

Proton conductivity [S/cm]

Voltage

0.6

60

0.4

40

0.2

20

0.8

80

0.6

60

0.4

40

0.2

20

0
0
200 400 600 800
2
Current density [mA/cm ]

0
0
200 400 600 800
2
Current density [mA/cm ]

100
(b)

Volltage [V]

Voltage [V]

80

100
(a)

Power density [mW/cm ]

DMFC

1
0.8

Power density [mW/cm 2 ]

10
Nafion117

Power density

8 wt%
16 wt%
32 wt%

11a25 m CLPE-ATBS b
Nafion117 DMFC Pt-Ru 2
mg/cm2

4-2-2

Tel:03-5796-7340Fax:03-5796-7345 E-mail:safcjp@sial.com

2.indd 13

Materials Science

13

2010/06/17 13:33:40

SEM
TEM 12

TEM
1 m

Membrane

50 oC

80 oC

Nafion 117

PI-SPES

1200

1000
MeOH permeability [ kg m/m2 h]

SPESSPES

PI
PI 180

800

600

400

200

0
0

10

20

30

40

50

60

MeOH conc. in feed [wt%]

SEM

SEM

Pore-filling

SEM

TEM

1m

12PI PI-SPES SEM

TEM

PI
SPES PI-SPES
503ppm FeSO4 3
H2O2 13 PI-SPES
SPES
SPES 30
PI-SPES 10 10wt

Weight loss [wt%]

-20

-40
SPES cast membrane
SPES filling polymer
PI substrate

-80

-100
2

10

Time [hour]

13SPES PE PI-SPES
PI-SPES

PI-SPES Nafion117 50 80
14
PI-SPES
PI-SPES

14

2.indd 14

Materials Science

50 30 wtPI-SPES
2 kg m/m2h Nafion117 430 kg m/
m2h 1 25
300
80
18
PI-SPES RH100
Nafion117 80 0.05 Scm-1

19

PEFC
1

-60

14Nafion117 PI-SPES

PEFC
PEFC
PEFC
PEFC

- 20-22

23, 24 Pt

Tel:03-5796-7330Fax:03-5796-7335 E-mail:sialjpts@sial.com

2010/06/17 13:33:41

25, 26
Pt
27-29

Nafion is a registered trademark of E.I. DuPont de Nemours & Co. Aciplex is a registered
trademark of Asahi Kasei Chemicals Co. Flemion is a registered trademark of Asahi Glass Co., Ltd.

6
1 , , , , , 2005.
2 T. A. Zawodzinski, T. E. Springer, F. Uribe and S. Gottesfeld, Solid State Ionics, 1993, 60,
199.
3 M. Watanabe, H. Uchida, Y. Seki, M. Emori, P. Stonehart, J. Electrochem. Soc., 1996,
143, 3847.
4 M. Rikukawa and K. Sanui, Prog. Polym. Sci., 2000, 25, 1463.
5 T. Lehtinen, G. Sundholm, S. Holmberg, F. Sundholm, P. Bjornbom and M. Bursell,
Electrochim. Acta, 1998, 43, 1881.
6 K. Miyatake, H. Zhou, H. Uchida, and M. Watanabe, Chem. Commun., 2003, 2003, 368.
7 Y. Yin, J. Fang, H. Kita, K. Okamoto, Chem. Lett., 2003, 32, 328.
8 J.S. Wainright, J.T. Wang, D. Weng, R.F. Savinell, M.H. Litt, J. Electrochem. Soc., 1995,
142, L121.

9 I. Honma, Y. Takeda, J. M. Bae, Solid State Ionics, 1999, 120, 255.

10 L. Depre, M. Ingram, C. Poinsignon, M. Popall, Electrochim. Acta, 2000, 45, 1377.
11 W. Lee, A. Shibasaki, K. Saito, K. Sugita, K. Okuyama, T. Sugo, J. Electrochem. Soc.,
1996, 143, 2795.
12 K. Scott, W. M. Taama and P. Argyropoulos, J. Membrane Sci., 2000, 171, 119.
13 T. Yamaguchi, S. Nakao, S. Kimura, Macromolecules, 1991, 24, 5522.
14 T. Yamaguchi, Y. Miyazaki, T. Tsuru, S. Nakao, S. Kimura, Ind. Eng. Chem. Res., 1998, 37,
177.
15 T. Yamaguchi, F Miyata, S. Nakao, Adv. Mater., 2003, 15, 1198.
16 T. Yamaguchi, H. Kuroki, F. Miyata, Electrochem. Commun., 2005, 7, 730.
17 A. Yamauchi, T. Ito, T. Yamaguchi, J. Power Sources, 2007, 174, 170.
18 T. Yamaguchi, Z. Hua, T. Nakazawa, N. Hara, Adv. Mater., 2007, 19, 592.
19 N. Hara, H. Ohashi, T. Ito, T. Yamaguchi, J. Phys. Chem. B., 2009, 113, 4656.
20 G. M. Anilkumar, S. Nakazawa, T. Okubo, T. Yamaguchi, Electrochem. Commun., 2006, 8,
133.
21 J.-M. Lee, H. Ohashi, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn., 2009, 42, 918.
22 J.-M. Lee, Y. Kikuchi, H. Ohashi, T. Tamaki, T. Yamaguchi, J. Mater. Chem., in press.
23 N. Limjeerajarus, Y. Nishiyama, H. Ohashi, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn., 2009,
42, 616.
24 N. Limjeerajarus, T. Yanagimoto, H. Ohashi, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn.,
2009, 42, 771.
25 H. Mizuhata, S. Nakao, T. Yamaguchi, J. Power Sources, 2004, 138, 25.
26 H. Kuroki, T. Yamagcuhi, J. Electrochem. Soc., 2006, 153, A1417.
27 N. Limjeerajarus, T. Yanagimoto, T. Yamamoto, T. Ito, T. Yamaguchi, J. Power Sources,
2008, 185, 217.
28 N. Limjeerajarus, T. Yanagimoto, T. Yamamoto, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn.,
2009, 42, 39.
29 H. Ishikawa, T. Tamaki, T. Ito, H. Ohashi, T. Yamaguchi, J. Chem. Eng. Jpn., in press.

www.sigma-aldrich.com/alternative-jp
www.sigma-aldrich.com/nano-jp

Nafion 5 wt. % dispersion, H2O15-20 wt. %, propanol (75-80 wt. %)

Available Acid Capacity (meq/g, H+ polymer basis)> 0.9

274704-25ML, 100ML

Nafion 5 wt. % dispersion, H2O45 wt. %, 1-propanol (50 wt. %)

Available Acid Capacity (meq/g, H+ polymer basis)> 1.00

527084-25ML, 100ML

Available Acid Capacity (meq/g, H+ polymer basis)> 0.92

510211-25ML, 100ML

Nafion 10 wt. % dispersion, H2O90 wt. %

Available Acid Capacity (meq/g, H+ polymer basis)> 1.00

527114-25ML

Available Acid Capacity (meq/g, H+ polymer basis)> 0.92

527106-25ML

Nafion 20 wt. % dispersion, H2O34 wt. %, 1-propanol (46 wt. %)

Available Acid Capacity (meq/g, H+ polymer basis)> 1.00

663492-25ML

Available Acid Capacity (meq/g, H+ polymer basis)> 0.92

527122-25ML

1-propanol : 2-propanol = 45 : 45

Nafion 117
8 x 10 x 0.007 inch (20.32 cm x 25.4 cm x 183 m)Available Acid Capacity> 0.9 meq/g

274674-1EA

12 x 12 x 0.007 inch (30.48 cm x 30.48 cm x 183 m)Available Acid Capacity> 0.9 meq/g

292567-1EA

12 x 12 x 0.005 inch (30.48 cm x 30.48 cm x 127 m)Available Acid Capacity> 0.9 meq/g

541346-1EA

12 x 12 x 0.002 inch (30.48 cm x 30.48 cm x 51 m)Available Acid Capacity> 0.92 meq/g

676470-1EA

Nafion 115

Nafion NRE-212

1-3 Material
Matters Vol.4, No.1 www.sigma-aldrich.com/
mscatalog-jp
Platinum black, 99.9+% trace metal basis, fuel cell grade
Surface Area: 25-34 m2/g, Sulfur: 50 ppm, Trace Metal Analysis: 350.0 ppm, Water Soluble Chloride: 220ppm

520780-1G, 5G

Platinum(IV) chloride, 99.99% trace metals basis

379840-250MG, 1G

Chloroplatinic acid hydrate, 99.995% trace metals basis (H2PtCl6xH2O)

254029-250MG, 1G, 5G

1)Size-specific catalytic activity of platinum clusters enhances oxygen reduction reactionsYamamoto K.; Imaoka T.; Chun W.-J.; Enoki O.; Katoh H.; Takenaga M.; Sonoi A. Nature Chemistry, 2009,
1, 397. 2)Homogeneous Deposition of Platinum Nanoparticles on Carbon Black for Proton Exchange Membrane Fuel CellFang, B.; Chaudhari, N. K.; Kim, M.-S.; Kim, J. H.; Yu, J.-S. J. Am. Chem.
Soc., 2009, 131, 15330. 3)A class of non-precious metal composite catalysts for fuel cellsBashyam, R.; Zelenay, P. Nature, 2006, 443, 63.

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24-4
5-1

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