SOFC SOFC
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- たいち りゅうとう
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1 2 SOFC, PEFC
2 amezawa@ee.mech.tohoku.ac.jp 2 unemoto@tagen.tohoku.ac.jp 3 kawada@ee.mech.tohoku.ac.jp 1SOFC SOFC SOFC SOFC Polymer Electrolyte Fuel Cell, PEFC PEFC kW 1 PEFC Solid Oxide Fuel Cell, SOFC PEFC PAFC MCFC SOFC Li/K, Li/Na H + H + - CO 3 O LPG SOFC NEF2007 1kW PEFC LHV SOFC SOFC SOFC SOFC 1-2 SOFC LPG LPG SOFC SOFC SOFC 1V 2 Tel: Fax: sialjpts@sial.com
3 (a) (b) e - H 2 O ; O ; A ; O O 2- ; M ; B 2 a MO 2 b ABO 3 H 2 1 SOFC O 2 La 3 Sr2 Ga3 Mg2 Ga Co SOFC SOFC 1kW SOFC kW SOFC 1000 SOFC SOFC SOFC ZrO 2 ZrO Zr 4 3 Y SOFC SOFC CeO 2 2 LaGaO 3 Ce4 Gd Sm 3 n SOFC SOFC 3d LnMO 3 Ln = La, Pr, Sm M = Mn, Fe, Co 3 Sr Ca 2 SOFC La,Sr MnO 3 La,Ca MnO 3 SOFC La,SrCo,Fe O 3 La,SrCo,Fe O SOFC Ni Ni Ni Ni SOFC Tel: Fax: safcjp@sial.com 3
4 LaCrO 3 SrTiO 3 SOFC Fe-Cr Cr Ni Cr 2 SOFC SOFC SOFC SOFC #1000 (a) (b) 3 4 3a 2 3b l S I V 1 σ l S I V SOFC Hz 1MHz mv 4 2 3a 4 b 2 SOFC 4 4 Tel: Fax: sialjpts@sial.com
5 2-2-2 / 5a RC Z 1 R i ω R 2 C i 2 ω C i R j i 1 ω i C i R 2 2 j 1 2 R ω i i C i i = ggb if R i C i ω =1/2πf f 5b 5a 5a 5b 2 R i /2 R b R gb R if R b (a) (b) 5 a b 5b R b R gb SOFC SOFC O 2 H 2 Ar N 2 SOFC H 2 H 2 H 2 H 2 O H 2 O H 2 H 2 O SOFC 3 SOFC SOFC 16-23, Tel: Fax: safcjp@sial.com 5
6 J C / x 3 D m 2 s -1 3 Δt x x Δx ΔJ J x Δt J x Δx Δt Δx ΔC t=0 C x,y,tt=0 C C 0 C k SOFC D D chem a 2b 2c a, b << c M t t L 1 L 2 α β A M MO A + M 2+ Kröger-Vink Tel: Fax: sialjpts@sial.com
7 K 3.0x σ / S cm V O h 1718 K 2 V O A M >> h h 1/ , σ t t 20 D k L 1, L 2, α, β Al SrTiO 3 6 Al Ti 3-3 A x M 1-x O 1-δ 19 6 t=0 D k Time / sec Al:SrTiO 3, 1123K, p O 2 = bar20 4 SOFC SOFC SOFC fca-enefarm.org/ SOFC D. J. L. Brett; A. Atkinson; N. P. Brandon; S.J. Skinner, Chem. Soc. Rev., 2008, 37, A. Weber; E. Ivers-Tiffee; J. Power Sources, 2004, 127, R. M. Ormerod, Chem. Soc. Rev., 2003, 32, N. Q. Minh, J. Am. Ceram. Soc., 1993, 76, sofc.nef.or.jp/ K. Huang; J. Wan; J.B. Goodenough, J. Mat. Sci., 2001, 36, T. Ishihara, Bull. Chem. Soc. Jpn., 2006, 79, E. V. Tsipis; V. V. Kharton, J. Solid State Chem., 2008, 12, E. V. Tsipis; V. V. Kharton, J. Solid State Chem., 2008, 12, S. B. Adler, Chem. Rev., 2004, 104, C. Sun; U. Stimming, J. Power Sources, 2007, 171, Z. Yang, Int. Mat. Rev., 2008, 53, P. G. Bruce ed., Solid State Electrochemistry, Cambridge University Press, JIS p Electrochemistry, 2006, 74, P. G. Shewmon, Diffusion in Solids, McGraw-Hill J. Crank, The Mathematics of Diffusion, 2nd ed., Oxford University Press I. Yasuda, T. HIkita, J. Electrochem. Soc., 1994, 141, I. Yasuda, M. Hishinuma, J. Solid State Chem., 1996, 123, 382 Tel: Fax: safcjp@sial.com 7
8 alternative-jp Lanthanum strontium cobalt ferrite, LSCF 6428 La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O G Lanthanum strontium manganite, LSM-20 (La 0.80 Sr 0.20 )MnO G Lanthanum strontium manganite, LSM-35 (La 0.65 Sr 0.35 )MnO G Lanthanum strontium cobalt ferrite composite cathode powder, LSCF/GDC (Ce 0.9 Gd 0.1 )O 1.95 : (La 0.60 Sr 0.40 )(Co 0.20 Fe 0.80 )O 3 = 1 : G Lanthanum strontium manganite composite cathode powder, LSM-20/YSZ (Y 2 O 3 ) 0.08 (ZrO 2 ) 0.92 : (La 0.80 Sr 0.20 )MnO 3 = 1 : G Lanthanum strontium manganite composite cathode powder, LSM20-GDC10 (Ce 0.9 Gd 0.1 )O 1.95 : (La 0.80 Sr 0.20 )MnO 3 = 1 : G Nickel oxide - Cerium samarium oxide for coatings, NiO/SDC, 99+ % trace metals basis NiO : (CeO 2 - Sm 2 O 3 ) = 60 : G Nickel oxide - Yttria-stabilized zirconia (YSZ) for general applications, NiO/YSZ, 99+ % trace metals basis NiO : (Y 2 O 3 ZrO 2 ) = 60 : G Nickel oxide - Yttria-stabilized zirconia (YSZ) for coatings, NiO/YSZ, 99+ % trace metals basis NiO : (Y 2 O 3 - ZrO 2 ) = 66 : G Cerium(IV) oxide-gadolinium doped (GDC) nanopowder Gd 10 mol % as dopant G Cerium(IV) oxide-gadolinium doped (GDC) nanopowder Gd 20 mol % as dopant G Cerium(IV) oxide-samaria doped nanopowder SmO 2 15 mol % as dopant G Zirconium(IV) oxide-yttria stabilized (YSZ) nanopowder Y 2 O 3 3 % as stabilizer G Zirconium(IV) oxide-yttria stabilized (YSZ) nanopowder Y 2 O 3 8 % as stabilizer G Zirconium(IV) oxide-yttria stabilized (YSZ) submicron powder Y 2 O 3 8 % as stabilizer, 99.9% trace metals basis (purity excludes 2% HfO 2 ) G, 500G Cerium(IV)-zirconium(IV) oxide nanopowder, <50 nm particle size (BET), 99.0% trace metals basis Ce : Zr = 1: 1 (ZrO 2 and CeO 2 or an intermediate compound) G, 100G Aldrich Vol.3, No.4 2 Vol.4, No Tel: Fax: sialjpts@sial.com
9 1 2 1 tamaki.t.aa@m.titech.ac.jp 2 yamag@res.titech.ac.jp (a) (b) PEFC PEFC MEA PEFC Anode H 2 2H + +2e- Cathode O2 +2H+ +2e - H 2 O Anode CH 3 OH+H 2 O CO 2 +6H + +6e - Cathode 3/2O 2 +6H + +6e - 3H 2 O 1 PEFC a DMFC b 2 ε E ε ΔG ΔH PEFC PEFC 2-1 PEFC DMFC 1 PEFC DMFC H + ΔH HHV LHV 251 ΔG -237 kj/mol ΔH -286 kj/mol HHV ε 83 LHV ΔH -242 kj/mol ε 98 ΔG -702 kj/mol ΔH -727 kj/mol HHV ε 97 ΔG E n F E 1.23 V E 1.21 V PEFC Tel: Fax: safcjp@sial.com 9
10 PEFC 50 PEFC 35 PEFC PEFC 2-2 PEFC 2 I A/cm 2 E V 2 E 0 η a IR η IR η c [ V ] E 0 η a η IR η c - MEA a 3b R membrane Ω 3c 3c R C R membrane 3 σ S/cm 3 l cmw cmd cm l l R membrane (a) Pt l (cm) w (cm) (b) Pt () Pt () l (cm) (c) R membrane R C 3 ab c [A/cm 2 ] 2 PEFC E 0 η a η IR IR η c PEFC Pt DMFC IR R ΩR I IR I R V PEFC PEFC 3 PEFC IEC meq/g IEC 1 EW g/eq DMFC 4a H J kg m -2 s -1 dq dt A m b 10 Tel: Fax: sialjpts@sial.com
![(cm) (c) R membrane R C 3 ab c [A/cm 2 ] 2 PEFC E 0 η a η IR IR η c PEFC Pt DMFC IR R ΩR I IR I R V PEFC PEFC 3 PEFC IEC](/docs-images/42/23076877/images/page_10.jpg "meq/g IEC 1 EW g/eq DMFC 4a H J kg m -2 s -1 dq dt A m2 4 4 4b 10 Tel:03-5796-7330 Fax:03-5796-7335 E-mail :")
11 (a) (b) Q H + e - θ O 2 4 : a b 4 J d Methanol permeabilitykg m m -2 h -1 P m 2 /s ΔC mol/m θ 4b θ D m 2 /s6 6 PEFC Nafion IEC σ σ MEA PEFC ppm Fe PEFC Pt Pt nm CB CB nm μm CB 5 5 SEMTEM X XRDX XPS 1 IRAS XPS X XAS in-situ 1 MEA Pt 3-3 MEA MEA MEA PEFC 6 H 2 O 2 6 PEFC MEA Tel: Fax: safcjp@sial.com 11
12 MRI MEA 4 PEFC PEFC PEFC PEFC DMFC PEFC PEFC 4-1 PEFC Nafion Flemion -CF PTFE Nafion Flemion PTFE 3 CF 2 CF 2 x CF 2CF y O CF2 CFO m CF2 SO 3 H n CF 3 Nafion : m>2, n=2, x=5-13.5, y=1000 Dow : m=0, n=2 Aciplex : m=0, 3, n=2-5, x= Flemion : m=0, 1, n= , 10 γ 11, 12 DMFC 4-2 nm Pore DMFC -CH 2-4, 5 4 6, 7 Porous substrate Filling electrolyte Substrate Pore-filling electrolyte membrane 8 12 Tel: Fax: sialjpts@sial.com
13 CLPE 25 μm 100 nm PI 30 μm 300 nm 2 AAVS ATBS AAVS ATBS DMFC Nafion 117 Nafion PTFE-AA 1 CLPE-AA PTFE-AAVS CLPE-AAVS PI-AAVS CLPE-ATBS 2PI-ATBS 0.1 Inverse of MeOH permeability [m h/kg μ m] Proton conductivity [S/cm] 9 10 Nafion 117 DMFC 10 Nafion 117 MEA 6 Nafion μm CLPE-ATBS 25 μm MEA Pt- Ru 2 mg/cm 2 Pt 1 mg/cm 2 8 wt2.5 M 32 wt 10 M50 DMFC 11 CLPE-ATBS a Nafion 117 b MEA DMFC 16 DMFC Nafion 117 DMFC 16 wt 32 wt Nafion μm CLPE-ATBS 25 μm 16 wt 70 mw/cm 2 32 wt 50 mw/ cm 2 17 Voltage [V] (a) Voltage 8 wt% 16 wt% 32 wt% Power density [mw/cm 2 ] Volltage [V] Power density Current density [ma/cm 2 ] Current density [ma/cm 2 ] 11 a 25 μm CLPE-ATBS b Nafion 117 DMFC Pt-Ru 2 mg/cm (b) Power density [mw/cm 2 ] Tel: Fax: safcjp@sial.com 13
![5 M 32 wt 10 M50 DMFC 11 CLPE-ATBS a Nafion 117 b MEA DMFC 16 DMFC Nafion 117 DMFC 16 wt 32 wt Nafion 117 200 μm CLPE-ATBS 25 μm 16 wt 70 mw/cm 2 32 wt 50 mw/ cm 2 17 Voltage [V] 1 0.8 0.6 0.4 0.](/docs-images/42/23076877/images/page_13.jpg "2 (a) Voltage 8 wt% 16 wt% 32 wt% 100 80 60 40 20 Power density [mw/cm 2 ] Volltage [V] Power density 0 0 0 0 0 200 400 600 800 0 200 400 600 800 Current density [ma/cm 2 ] Current density [ma/cm 2 ]")
14 SPESSPES PI PI 180 SEM TEM 12 TEM 1 μm MeOH permeability [ kg μm/m 2 h] Membrane o 50 C o 80 C Nafion 117 PI-SPES MeOH conc. in feed [wt%] SEM SEM 14 Nafion 117 PI-SPES SEM Pore-filling 1μm TEM 12 PI PI-SPES SEM TEM PI SPES PI-SPES 503ppm FeSO 4 3 H 2 O 2 13 PI-SPES SPES SPES 30 PI-SPES 10 10wt Weight loss [wt%] SPES cast membrane SPES filling polymer PI substrate Time [hour] 13 SPES PE PI-SPES PI-SPES PI-SPES Nafion PI-SPES PI-SPES wtpi-spes 2 kg μm/m 2 h Nafion kg μm/ m 2 h PI-SPES RH100 Nafion Scm PEFC1 PEFC PEFC PEFC PEFC , 24 Pt 14 Tel: Fax: sialjpts@sial.com
![0-20 -40-60 -80 SPES cast membrane SPES filling polymer PI substrate -100 0 2 4 6 8 10 Time [hour] 13 SPES PE PI-SPES PI-SPES PI-SPES Nafion 117 50 80 14 PI-SPES PI-SPES 50 30 wtpi-spes 2](/docs-images/42/23076877/images/page_14.jpg "kg μm/m 2 h Nafion 117 430 kg μm/ m 2 h 1 25 300 80 18 PI-SPES RH100 Nafion 117 80 0.")
15 25, 26 Pt 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,,,,, T. A. Zawodzinski, T. E. Springer, F. Uribe and S. Gottesfeld, Solid State Ionics, 1993, 60, M. Watanabe, H. Uchida, Y. Seki, M. Emori, P. Stonehart, J. Electrochem. Soc., 1996, 143, M. Rikukawa and K. Sanui, Prog. Polym. Sci., 2000, 25, T. Lehtinen, G. Sundholm, S. Holmberg, F. Sundholm, P. Bjornbom and M. Bursell, Electrochim. Acta, 1998, 43, K. Miyatake, H. Zhou, H. Uchida, and M. Watanabe, Chem. Commun., 2003, 2003, Y. Yin, J. Fang, H. Kita, K. Okamoto, Chem. Lett., 2003, 32, J.S. Wainright, J.T. Wang, D. Weng, R.F. Savinell, M.H. Litt, J. Electrochem. Soc., 1995, 142, L I. Honma, Y. Takeda, J. M. Bae, Solid State Ionics, 1999, 120, L. Depre, M. Ingram, C. Poinsignon, M. Popall, Electrochim. Acta, 2000, 45, W. Lee, A. Shibasaki, K. Saito, K. Sugita, K. Okuyama, T. Sugo, J. Electrochem. Soc., 1996, 143, K. Scott, W. M. Taama and P. Argyropoulos, J. Membrane Sci., 2000, 171, T. Yamaguchi, S. Nakao, S. Kimura, Macromolecules, 1991, 24, T. Yamaguchi, Y. Miyazaki, T. Tsuru, S. Nakao, S. Kimura, Ind. Eng. Chem. Res., 1998, 37, T. Yamaguchi, F Miyata, S. Nakao, Adv. Mater., 2003, 15, T. Yamaguchi, H. Kuroki, F. Miyata, Electrochem. Commun., 2005, 7, A. Yamauchi, T. Ito, T. Yamaguchi, J. Power Sources, 2007, 174, T. Yamaguchi, Z. Hua, T. Nakazawa, N. Hara, Adv. Mater., 2007, 19, N. Hara, H. Ohashi, T. Ito, T. Yamaguchi, J. Phys. Chem. B., 2009, 113, G. M. Anilkumar, S. Nakazawa, T. Okubo, T. Yamaguchi, Electrochem. Commun., 2006, 8, J.-M. Lee, H. Ohashi, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn., 2009, 42, 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, N. Limjeerajarus, T. Yanagimoto, H. Ohashi, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn., 2009, 42, H. Mizuhata, S. Nakao, T. Yamaguchi, J. Power Sources, 2004, 138, H. Kuroki, T. Yamagcuhi, J. Electrochem. Soc., 2006, 153, A N. Limjeerajarus, T. Yanagimoto, T. Yamamoto, T. Ito, T. Yamaguchi, J. Power Sources, 2008, 185, N. Limjeerajarus, T. Yanagimoto, T. Yamamoto, T. Ito, T. Yamaguchi, J. Chem. Eng. Jpn., 2009, 42, H. Ishikawa, T. Tamaki, T. Ito, H. Ohashi, T. Yamaguchi, J. Chem. Eng. Jpn., in press. Nafion 5 wt. % dispersion, H 2 O wt. %, propanol (75-80 wt. %) Available Acid Capacity (meq/g, H + polymer basis) > 0.9 Nafion 5 wt. % dispersion, H 2 O 45 wt. %, 1-propanol (50 wt. %) Available Acid Capacity (meq/g, H + polymer basis) > 1.00 Available Acid Capacity (meq/g, H + polymer basis) > 0.92 Nafion 10 wt. % dispersion, H 2 O 90 wt. % Available Acid Capacity (meq/g, H + polymer basis) > 1.00 Available Acid Capacity (meq/g, H + polymer basis) > 0.92 Nafion 20 wt. % dispersion, H 2 O 34 wt. %, 1-propanol (46 wt. %) Available Acid Capacity (meq/g, H + polymer basis) > 1.00 Available Acid Capacity (meq/g, H + polymer basis) > propanol : 2-propanol = 45 : ML, 100ML ML, 100ML ML, 100ML ML ML ML ML Nafion 117 Nafion 115 Nafion NRE x 10 x inch (20.32 cm x 25.4 cm x 183 μm) Available Acid Capacity > 0.9 meq/g 12 x 12 x inch (30.48 cm x cm x 183 μm) Available Acid Capacity > 0.9 meq/g 12 x 12 x inch (30.48 cm x cm x 127μm) Available Acid Capacity > 0.9 meq/g 12 x 12 x inch (30.48 cm x cm x 51μm) Available Acid Capacity > 0.92 meq/g EA EA EA EA 1-3 Material Matters Vol.4, No.1 mscatalog-jp Platinum black, 99.9+% trace metal basis, fuel cell grade Surface Area: m 2 /g, Sulfur: 50 ppm, Trace Metal Analysis: ppm, Water Soluble Chloride: 220ppm G, 5G Platinum(IV) chloride, 99.99% trace metals basis Chloroplatinic acid hydrate, % trace metals basis (H 2 PtCl 6 xh 2 O) MG, 1G MG, 1G, 5G 1) Size-specific catalytic activity of platinum clusters enhances oxygen reduction reactions Yamamoto K.; Imaoka T.; Chun W.-J.; Enoki O.; Katoh H.; Takenaga M.; Sonoi A. Nature Chemistry, 2009, 1, ) Homogeneous Deposition of Platinum Nanoparticles on Carbon Black for Proton Exchange Membrane Fuel Cell Fang, B.; Chaudhari, N. K.; Kim, M.-S.; Kim, J. H.; Yu, J.-S. J. Am. Chem. Soc., 2009, 131, ) A class of non-precious metal composite catalysts for fuel cells Bashyam, R.; Zelenay, P. Nature, 2006, 443, 63. Tel: Fax: safcjp@sial.com 15
16 TM Aldrich URL Material Matters sialjp@sial.com
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