5582
V.A. Sethuraman et al. / Electrochimica Acta 54 (2009) 5571–5582
DO∗
oxygen diffusion coefficient in the electrolyte (cm2 s−1
oxygen diffusion coefficient in Nafion® film (cm2 s−1
diffusion coefficient of O2 in Nafion® 112 membrane
)
[5] M. Inaba, H. Yamada, R. Umebayashi, M. Sugishita, A. Tasaka, Electrochemistry
2
75 (2007) 207.
DOf
)
[6] T. Kinumoto, M. Inaba, Y. Nakayama, K. Ogata, R. Umebayashi, A. Tasaka, Y.
Iriyama, T. Abe, Z. Ogumi, J. Power Sources 158 (2006) 1222.
[7] D.A. Schiraldi, J. Macromol. Sci. C: Polymer Rev. 46 (2006) 315.
[8] US Patents 5,013,618 (1991); 4,880,711 (1989); 4,447,506 (1984).
[9] US Patents 5,189,005 (1993); 5,593,934 (1997).
[10] T.J. Schmidt, H.A. Gasteiger, G.D. Stäb, P.M. Urban, D.M. Kolb, R.J. Behm, J. Elec-
trochem. Soc. 145 (1998) 2354.
[11] T.J. Schmidt, U.A. Paulus, H.A. Gasteiger, R.J. Behm, J. Electroanal. Chem. 508
(2002) 41.
[12] N. Markovic, P.N. Ross, J. Electroanal. Chem. 330 (1992) 499.
[13] V. Stamenkovic, N.M. Markovic, P.N. Ross Jr., J. Electroanal. Chem. 500 (2001)
44.
[14] L.H. Gevantman, in: D.R. Lide (Ed.), CRC Handbook of Chemistry and Physics,
79th ed., CRC Press, New York, 1998–1999, p. 8.
[15] W.J. Albery, M.L. Hitchman, Ring-Disc Electrodes, Clarendon Press, Oxford, 1971.
[16] Rotated Ring-Disk Electrodes: DT21 Series, Pine Instrument Company, Raleigh,
NC 27617.
[17] S. Trasatti, O.A. Petrii, Pure Appl. Chem. 63 (1991) 711.
[18] T. Biegler, D.A.J. Rand, R. Woods, J. Electroanal. Chem. 29 (1971) 269.
[19] J. Bett, K. Kinoshita, K. Routsis, P. Stonehart, J. Catal. 29 (1973) 160.
[20] V. Mittal, H.R. Kunz, J.M. Fenton, Abstract #1192, in: 208th Meeting of the
Electrochemical Society, Los Angeles, CA, October 16, 2005.
[21] V.O. Mittal, H.R. Kunz, J.M. Fenton, Electrochem. Solid State Lett. 9 (2006)
A299.
2
DOm
2
(cm2 s−1
)
E◦
equilibrium potential (0.695 V vs. SHE at 25 ◦C and
101 kPa)
Ea∗
Eapp
EW
F
activation energy for H2O2 formation (J mol−1
applied potential (V vs. SHE)
)
equivalent weight of Nafion® polymer (1100 g equiv.−1
)
Faraday constant (96,485 C mol−1
)
I
current density (A cm−2
ring current (mA)
)
Iring
Idisk
j
jdisk
jD
jkin
kb
kf
disk current (mA)
total peroxide current density (mA cm−2
)
disk current density (mA cm−2
diffusion-limited current density (mA cm−2
kinetic current density (mA cm−2
)
)
)
rate constant for H2O2 electro-oxidation (s−1
)
rate constant for H2O2 formation (mol2 cm−5 s−1
collection efficiency
)
N
n
[22] V.O. Mittal, H.R. Kunz, J.M. Fenton, J. Electrochem. Soc. 153 (2006) A1755.
[23] V.O. Mittal, H.R. Kunz, J.M. Fenton, J. Electrochem. Soc. 154 (2007) B652.
[24] M.R. Tarasevich, A. Sadkowski, E. Yeager, in: J.O’.M. Bockris, B.E. Conway, E. Yea-
ger, S.U.M. Khan, R.E. White (Eds.), Comprehensive Treatise in Electrochemistry,
Plenum Press, New York, 1983 (Chapter 6).
number of electrons transferred per O2 molecule in H2O2
formation (2)
POm
permeability of O2 in Nafion® 112 membrane
2
[25] S.K. Zecˇevic´, J.S. Wainright, M.H. Litt, S.Lj. Gojkovic´, R.F. Savinell, J. Electrochem.
(mol cm−1 s−1
)
Soc. 144 (1997) 2973.
Q
Q
R
T
charge density (C cm−2) (geometric area)
[26] A. Damjanovic, G. Hudson, J. Electrochem. Soc. 135 (1988) 2269.
[27] U.A. Paulus, A. Wokaun, G.G. Scherer, T.J. Schmidt, V. Stamenkovic, V. Rad-
milovic, N.M. Markovic, P.N. Ross, J. Phys. Chem. B 106 (2002) 4181.
[28] K.C. Neyerlin, W. Gu, J. Jorne, H.A. Gasteiger, J. Electrochem. Soc. 153 (2006)
A1955.
charge density of Pt (C cm−2) (geometric area)
universal gas constant (8.314 J mol−1 K−1
temperature (K)
)
[29] A.J. Bard, L.R. Faulkner, Electrochemical Methods, Wiley & Sons, Inc., New York,
1980.
t
V
v
time (s)
potential (V vs. SHE)
[30] A.B. Anderson, T.V. Albu, J. Electrochem. Soc. 147 (2000) 4229.
[31] R.A. Sidik, A.B. Anderson, J. Electroanal. Chem. 528 (2002) 69.
[32] Y. Wang, P.B. Balbuena, J. Chem. Theory Comput. 1 (2005) 935.
[33] V. Stamenkovic, B.N. Grgur, P.N. Ross, N.M. Markovic, J. Electrochem. Soc. 152
(2005) A277.
scan rate (V s−1
)
W
catalyst loading (mgPt cm−2) (geometric area)
Greek
˛
ı
[34] N.A. Anastasijevic, Z.M. Dimitrijevic, R.R. Adzic, Electrochim. Acta 31 (1986)
1125.
transfer coefficient
[35] D.R. Morris, X. Sun, J. Appl. Polym. Sci. 50 (1993) 1445.
[36] D. Rivin, C.E. Kendrick, P.W. Gibson, N.S. Schneider, Polymer 42 (2001) 623.
[37] N.H. Jalani, P. Choi, R. Datta, J. Membrane Sci. 254 (2005) 31.
[38] T. Zawodzinski, M. Neeman, L. Sillerud, S. Gottesfeld, J. Phys. Chem. 95 (1991)
6040.
[39] J.T. Hinatsu, M. Mizuhata, H. Takenaka, J. Electrochem. Soc. 141 (1994) 1493.
[40] L.M. Onishi, J.M. Prausnitz, J. Newman, J. Phys. Chem. B 111 (2007) 10166.
[41] S. Motupally, A.J. Becker, J.W. Weidner, J. Electrochem. Soc. 147 (2000) 3171.
[42] T. Fuller, Ph.D. Dissertation, University of California, Berkeley, 1989.
[43] R.C. Reid, J.M. Prausnitz, T.K. Sherwood, The Properties of Gases and Liquids,
McGraw Hill Inc., New York, 1977.
Pt/C electrode thickness (cm)
ıf
Nafion® film thickness (cm)
density of Nafion® (g cm−3
)
ꢃ
Á
ꢄ
ꢂH
ω
kinematic viscosity (cm2 s−1
overpotential (V vs. SHE)
)
moles of water per sulfonic acid group in Nafion®
fraction of O2 reducing to H2O2
O
2
2
electrode rotation rate (s−1
)
[44] T. Sakai, H. Takenaka, E. Torikai, J. Electrochem. Soc. 133 (1986) 88.
[45] K. Broka, P. Ekdunge, J. Appl. Electrochem. 27 (1997) 117.
[46] W. Liu, D. Zukerbrod, J. Electrochem. Soc. 152 (2005) A1165.
[47] S. Burlatsky, T. Jarvi, V. Atrazhev, Abstract # 502, The Electrochemical Society
Meeting Abstracts, Volume 2005-2, Los Angeles, CA, October 16–21, 2005.
[48] A. Panchenko, H. Dilger, J. Kerres, M. Hein, A. Ullrich, T. Kaz, E. Roduner, Phys.
Chem. Chem. Phys. 6 (2004) 2891.
Superscript
0
a
c
standard state or equilibrium
anode
cathode
[49] A. Panchenko, Dipl.-Chem., Institut für Physikalische Chemie der Universität
Stuttgart, October 2004.
[50] P. Yu, M. Pemberton, P. Plasse, J. Power Sources 144 (2005) 11.
[51] L. Protsailo, Development of High Temperature Membranes and Improved
Cathode Catalysts, United States Department of Energy Report, December
2005.
[52] A.T. Haug, L.V. Protsailo, S. Modi, V.A. Sethuraman, S. Motupally, Characteriza-
tion of membranes and catalysts for high temperature PEM fuel cells, United
States Department of Energy—High Temperature Working Group, in: 208th
Meeting of the Electrochemical Society, Los Angeles, CA, October 20, 2005.
[53] V.A. Sethuraman, J.W. Weidner, A.T. Haug, L.V. Protsailo, J. Electrochem. Soc. 155
(2008) B119.
Subscript
ad
b
D
disk
f
adsorbed
backward reaction, bulk
diffusion
Pt/Nafion® coated disc electrode
Nafion® film or forward reaction
kinetic
kin
ring
Pt ring electrode
[54] Z. Jusys, R.J. Behm, J. Phys. Chem. B 108 (2004) 7893.
[55] M. Inaba, M. Sugishita, J. Wada, K. Matsuzawa, H. Yamada, A. Tasaka, J. Power
Sources 178 (2008) 699.
References
[56] Q. Guo, V.A. Sethuraman, R.E. White, J. Electrochem. Soc. 151 (2004) A983.
[57] K.A. Mauritz, R.B. Moore, Chem. Rev. 104 (2004) 4535.
[58] R.H. Perry, D.W. Green, Perry’s Chemical Engineer’s Handbook, 7th ed., McGraw
Hill, 1997.
[59] U.A. Paulus, T.J. Schmidt, H.A. Gasteiger, R.J. Behm, J. Electroanal. Chem. 495
(2001) 134.
[1] E. Yeager, Electrochim. Acta 29 (1984) 1527.
[2] V.A. Sethuraman, J.W. Weidner, A.T. Haug, S. Motupally, L.V. Protsailo, J. Elec-
trochem. Soc. 155 (2008) B50.
[3] A. Bosnjakovic, S. Schlick, J. Phys. Chem. B 108 (2004) 4332.
[4] M. Inaba, T. Kinumoto, M. Kiriake, R. Umebayashi, A. Tasaka, Z. Ogumi, Elec-
trochim. Acta 51 (2006) 5746.