Abstract
Polymer electrolyte fuel cell (PEFC) is considered as one of the most promising power sources for futurist’s hydrogen economy. As shown in Fig. 1, operation of a Nafion-based PEFC is dictated by transport processes and electrochemical reactions at catalyst/polymer electrolyte interfaces and transport processes in the polymer electrolyte membrane (PEM), in the catalyst layers consisting of precious metal (Pt or Ru) catalysts on porous carbon support and polymer electrolyte clusters, in gas diffusion layers (GDLs), and in flow channels. Specifically, oxidants, fuel, and reaction products flow in channels of millimeter scale and diffuse in GDL with a structure of micrometer scale. Nafion, a sulfonic acid tetrafluorethylene copolymer and the most commonly used polymer electrolyte, consists of nanoscale hydrophobic domains and proton conducting hydrophilic domains with a scale of 2–5 nm. The diffusivities of the reactants (O2, H2, and methanol) and reaction products (water and CO2) in Nafion and proton conductivity of Nafion strongly depend on the nanostructures and their responses to the presence of water. Polymer electrolyte clusters in the catalyst layers also play a critical role in the catalysis of the nano-sized Pt catalysts. Electrochemical reactions occur at the interfaces between catalysts (Pt or Pt/Ru) and Nafion. The catalytic activity of the Pt catalysts is believed to be dictated by transport processes, adsorption/desorption, and charge transfer in the interfacial area. While transport processes may occur in an area of a few nanometers, adsorption/desorption and charge transfer occur within a region of a few angstroms from the surface of a nano-particulate catalyst. Thus, modeling or simulation of PEFC is a multiscale problem.
This is a preview of subscription content, log in via an institution.
Buying options
Tax calculation will be finalised at checkout
Purchases are for personal use only
Learn about institutional subscriptionsREFERENCES
K.D. Kreuer, S.J. Paddison, E. Spohr, M. Schuster, Chem. Rev. 104, 4637 (2004)
K.D. Kreuer, Solid State Ionics 94, 5562 (1997)
E. Spohr, P. Commer, A.A. Kornyshev, J. Phys. Chem. B 106, 10560 (2002)
D. Seeliger, C. Hartnig, E. Spohr, Electrochim. Acta 50, 4234 (2005)
S. Walbran, A.A. Kornysheva, J. Chem. Phys. 114, 10039 (2001)
M. Tuckerman, K. Laasonen, M. Sprik, and M. Parrinello, J. Phys. Chem. 99, 5749 (1995)
J.A. Morrone, M.E. Tuckermana, J. Chem. Phys. 117, 4403 (2002)
A. Zunger, A. Franceschetti, G. Bester, W.B. Jones, K. Kim, P.A. Graf, L-W. Wang, A. Canning, O. Marques, C. Voemel, J. Dongarra, J. Langou, S. Tomov, J. Phys. B: Conference Series 46, 292 (2006)
S.E. Thompson and S. Parthasarathy, Materials Today 9, 20 (2006)
W. Goddard III, B. Merinov, A.V. Duin, T. Jacob, M. Blanco, V. Molinero, S.S. Jang, Y.H. Jang, Mol. Simul. 32, 251 (2006)
J. Hafner, Acta Mater. 48, 71 (2000)
P. Hohenberg, W. Kohn, Phys. Rev. B 136, 864 (1964)
W. Kohn, L.J. Sham, Phys. Rev. A 140, 1133 (1965)
U.V. Barth, L. Hedin, J. Phys. C: Solid St. Phys. 5, 1629 (1972)
J.P. Perdew, A. Zunger, Phys. Rev. B 23, 5075 (1981)
J.P. Perdew, Phys. Rev. B 33, 8822 (1986)
J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996)
W.A. Goddard III, T. Cagin, M. Blanco, N. Vaidehi, S. Dasgupta, W. Floriano, M. Belmares, J. Kua, G. Zamanakos, S. Kashihara, M. Iotov, G. Gao, Comput. Theor. Polym. Sci. 11, 329 (2001)
R. Car, M. Parrinello, Phys. Rev. Lett. 55, 2471 (1985)
M.P. Allen, Computational Soft Matter: From Synthetic Polymers to Proteins, 23, 1 (2004)
L. Mayo, B.D. Olafson, W.A. Goddard III, J. Phys. Chem. 94, 8897 (1990)
P. Jannasch, Curr. Opin. Colloid Interface Sci. 8, 96 (2003)
E. Chalkova, X. Zhou, C. Ambler, M.A. Hofmann, J.A. Weston, H.R. Allcock, S.N. Lvov, Electrochem. Solid-State Lett. 10, 221 (2002)
P. Spinelli, C. Francia, E.P. Ambrosio, M. Lucariello, J. Power Sources 178, 517 (2008)
M.D. Macia, J.M. Campina, E. Herrero, J.M. Feliu, J. Electroanal. Chem 564, 141 (2004)
M. Watanabe, S. Motto, J. Electroanal. Chem. 60, 275 (1975)
J. Kua, W.A. Goddard III, J. Am. Chem. Soc. 121, 10928 (1999)
A.B. Anderson, E. Grantscharova, S. Seong, J. Electrochem. Soc. 148, 2075 (1996)
A.B. Anderson, Int. J. Quantum Chem., 49, 581 (1994)
T. Jacob, B.V. Merinov, W.A. Goodard III, Chem. Phys. Lett. 385, 374 (2004)
G. Barabino, C. Gavotti, M. Marchesi, Chem. Phys. Lett. 104, 478 (1984)
C.Y. Lee, J.A. McCammon, P.J. Rossky, J. Chem. Phys. 80, 4448 (1984)
E. Spohr, K. Heinzinger, Electrochim. Acta 33, 1211 (1988)
P.S. Crozier, R.L. Rowley, D. Henderson, J. Chem. Phys. 113, 9202 (2000)
C. Hartnig, M.T.M. Koper, J. Phys. Chem. B 108, 3824 (2004)
E. Spohr, J. Phys. Chem. 93, 6171 (1989)
J.I. Siepmann, M. Sprik, J. Chem. Phys. 102, 511 (1995)
I.-C. Yeh, M.L. Berkowitz, Chem. Phys. Lett. 301, 81 (1999)
E. Spohr, J. Chem. Phys. 107, 6342 (1997)
E. Spohr, Electrochim. Acta 49, 23 (2003)
J.P. Badiali, M.L. Rosinberg, J. Goodisman, J. Electroanal. Chem. Interfacial Electrochem. 130, 31 (1981)
W. Schmickler, J. Electroanal. Chem. Interfacial Electrochem. 150, 19 (1983)
J.W. Halley, D. Price, Phys. Rev. B 35, 9095 (1987); K. Rice, Phys. Rev. 31, 1051 (1928)
D.L. Price, J.W. Halley, Phys. Rev. B 38, 9357 (1988)
J. Goodisman, J. Chem. Phys. 90, 5756 (1989)
D.L. Price, J.W. Halley, J. Chem. Phys. 102, 6603 (1995)
J.W. Halley, A. Mazzolo, Y. Zhou, and D. Price, J. Electroanal. Chem. 450, 273 (1998)
S. Izvekov, A. Mazzolo, K. VanOpdorp, G.A. Voth, J. Chem. Phys. 114, 3248 (2001)
P. Vassilev, R.A. van Santen, M.T.M. Koper, J. Chem. Phys. 122, 54701 (2005)
A.B. Anderson and N.C. Debnath, J. Am. Chem. Soc. 105, 18 (1983)
S. Seong, A.B. Anderson, J. Phys. Chem. 100, 11744 (1996)
A.B. Anderson, T.V. Albu, J. Am. Chem. Soc. 121, 11855 (1999)
T.V. Albu, A.B. Anderson, Electrochim. Acta 46, 3001 (2001)
R.A. Sidik, A.B. Anderson, J. Electroanal. Chem. 528, 69 (2002)
A.B. Anderson, N.M. Neshev, R.A. Sidik, P. Shiller, Electrochim. Acta 47, 2999 (2002)
A.B. Anderson, Electrochim. Acta 48, 3743 (2003)
J. Narayanasamy, A.B. Anderson, J. Phys. Chem. B 107, 6898 (2003)
M.F. Toney, J.N. Howard, J. Richer, G.L. Borges, J.G. Gordon, O.R. Melroy, D.G. Wiesler, D. Yee, and L.B. Sorensen, Nature 368, 444 (1994)
Y. Lozovoi, A. Alavi, J. Kohanoff, R.M. Lynden-Bell, J. Chem. Phys. 115, 1661 (2001)
J.-S. Filhol, M. Neurock, Angew. Chem., Int. Ed. 45, 402 (2006)
C.D. Taylor, S.A. Wasileski, J.-S. Filhol, M. Neurock, Phys. Rev. B 73, 165402 (2006)
M.J. Janik, C.D. Taylor, M Neurock, J. Electrochem. Soc. 156, B126 (2009)
K. Raghavan, K. Foster, K. Motakabbir, M. Berkowitz, J. Chem. Phys. 94, 2110 (1991)
E. Spohr, J. Chem. Phys. 93, 6171 (1989)
S. Senapati, A. Chandra, J. Chem. Phys. 113, 8817 (2000)
X. Xia, M.L. Berkowitz, Phys. Rev. Lett. 74, 3193 (1995)
I.-C. Yeh, M.L. Berkowitz, J. Chem. Phys. 112, 10491 (2000)
P.G. Kusalik, I.M. Svishchev, Science 265, 1219 (1994)
I.M. Svishchev, P.G. Kusalik, J. Wang, R.J. Boyd, J. Chem. Phys. 105, 4742 (1996)
M.F. Toney, J.N. Howard, J. Richer, G.L. Borges, J.G. Gordon, O.R. Melroy, D.G. Wiesler, D. Yee, L.D. Sorensen, Surf. Sci. 335, 326 (1995)
J.I. Siepmann, M. Sprik, J. Chem. Phys. 102, 511 (1995)
J.W. Halley, A. Mazzolo, Y. Zhou, D. Proce, J. Electroanal. Soc. 450, 273 (1998)
P.B. Balbuena, E.J. Lamas, Y. Wang, Electrochim. Acta 50, 3788 (2005)
E.J. Lamas, P.B. Balbuena, Electrochim. Acta 51, 5904 (2006)
A.P. Sutton, J. Chen, Philos. Mag. Lett. 61, 139 (1990)
H.J.C. Berendsen, J.R. Grigera, T.P. Straatsma, J. Phys. Chem. 91, 6269 (1987)
I. Kusaka, Z.G. Wang, J.H. Seinfeld, J. Phys. Chem. 108, 6829 (1998)
A.K. Rappe, W.A. Goddard, J. Phys. Chem. 95, 3358 (1991)
MSI, Force-field based simulations, San Diego, 1997
S.J. Paddison, T.A. Zawodzinski, Solid State Ionics 115, 333 (1998)
A.C.T. van Duin, S. Dasgupta, F. Lorant, and W.A. Goddard, J. Phys. Chem. A, 105(41), 9396 (2001)
H. Steininger, S. Lehwald, H. Ibach, Surf. Sci. 123, 1 (1982)
C. Puglia, A. Nilsson, B. Hernnaes, O. Karis, P. Bennich, N. Martensson, Surf. Sci. 342, 119 (1995)
J.L. Gland, B.A. Sexton, G.B. Fisher, Surf. Sci. 95, 587 (1980)
D.A. Outka, J. Stoehr, W. Jark, P. Stevens, J. Solomon, R.J. Madix, Phys. Rev. B 35, 4119 (1987)
W. Wurth, J. Stoehr, P. Feulner, X. Pan, K.R. Bauchspiess, Y. Baba, E. Hudel, G. Rocker, D. Menzel, Phys. Rev. Lett. 65, 2426 (1990)
B.C. Stipe, M.A. Rezaei, W. Ho, Science 279, 1907 (1998)
B. Hammer, J.K. Nørskov, Adv. Catal. 45, 71 (2000)
B. Hammer, L.B. Hansen, J.K. Nørskov, Phys. Rev. B 59, 7413 (1999)
J. Greeley, J.K. Nørskov, M. Mavrikakis, Annu. Rev. Phys. Chem. 53, 319 (2002)
A. Ruban, B. Hammer, P. Stoltze, H.L. Skriver, J.K. Nørskov, J. Mol. Catal. A 115, 421 (1997)
A. Eichler, J. Hafner. Phys. Rev. Lett. 79, 4481 (1997)
T. Toda, H. Igarashi, H. Uchida, M. Watanabe, J. Electroanal. Chem. 146, 3750 (1999)
A. Ruban, H.L. Skriver, J.K. Nørskov, Phys. Rev. B 59, 15990 (1999)
Y. Xu, A.V. Ruban, M. Mavrikakis, J. Am. Chem. Soc. 126, 4717 (2004)
P.B. Balbuena, D. Altomare, L. Agapito, J.M. Seminario, J. Phys. Chem. B 107, 13671 (2003)
Z.D. Wei, F. Yin, L.L. Li, X.W. Wei, X.A. Liu, J. Electroanal. Chem. 541, 185 (2003)
R.R. Nazmutdinov, G.A. Tsirlina, O.A. Petrii, Y.I. Kharkats, A.M. Kuznetsov, Electrochim. Acta 45, 3521 (2000)
O.A. Petrii, R.R. Nazmutdinov, M.D. Bronshtein, G.A. Tsirlina, Electrochim. Acta 52, 3493 (2007)
A. Damjanovic, V. Brusic, Electrochim. Acta 12, 615 (1967)
E. Yeager, M. Razaq, D. Gervasio, A. Razaq, Electrocatalysis and Oxygen Electrochemistry Proc. 92, 440 (1992)
C.D. Taylor, M.J. Janik, M. Neurock, R.G. Kelly, Mol. Simul. 33, 429 (2007)
M.J. Janik, M. Neurock, Electrochim. Acta 52, 5517 (2007)
A.B. Anderson, T.V. Albu, J. Electrochem. Soc. 147, 4229 (2000)
T. Li, P.B. Balbuena, Chem. Phys. Lett. 367, 439 (2003)
J.K. Nørskov, J. Rossmeisl, A. Logadottir, L. Lindqvist, J.R. Kitchin, T. Bligaard, H. Jónsson, J. Phys. Chem. B 108, 17886 (2004)
J. Zhang, M.B. Vukmirovic, Y. Xu, M. Mavrikakis, R.R. Adzic, Ang. Chem. Int. Ed. 44, 2132 (2005)
R. Jinnouchi, K. Okazaki, Microscale Thermophys. Eng. 7, 15 (2003)
Y. Wang, P.B. Balbuena J. Phys. Chem. B 109, 14896 (2005)
J.-S. Filhol, M. Neurock, Angew. Chem. Int. Ed. 45, 402 (2006)
M.J. Buehler, A.C.T. van Duin, T. Jacob, Y. Jang, B. Merinov, W.A. Goddard III, MRS Proceedings Fall 2005
M.T.M. Koper, Surf. Sci. 548, 1 (2004)
A.B. Anderson, E. Grantscharova, J. Phys. Chem. 99, 9143 (1995)
T.E. Shubina, C. Hartnigw, M.T.M. Koper, Phys. Chem. Chem. Phys. 6, 4215 (2004)
T.E. Shubina, M.T.M. Koper, Electrochim. Acta 47, 3621 (2002)
P. Liu, A. Logadottir, J.K. Nørskov, Electrochim. Acta 48, 3731 (2003)
D. Cao, G.-Q. Lu, A. Wieckowski, S.A. Wasileski, M. Neurock, J. Phys. Chem. B 109, 11622 (2005)
X. Gong, Z. Liu, R. Raval, P. Hu, J. Am. Chem. Soc. 126, 8 (2004)
X. Gong, P. Hu, R. Raval, J. Chem. Phys. 119, 6324 (2003)
C.J. Zhang, P. Hu, J. Am. Chem. Soc. 122, 2134 (2000)
S. Desai, M. Neurock, Electrochim. Acta 48, 3759 (2003)
C. Hartnig, J. Grimminger, E. Spohr, Electrochim. Acta 52, 2236 (2007)
C. Hartnig, E. Spohr, Chem. Phys. 319, 185 (2005)
J. Ludwig, D.G. Vlachos, A.C.T. van Duin W.A. Goddard, J. Phys. Chem. B 110, 4274 (2006)
A.A. Kulikovsky, E. Spohr, NIC Symposium 32, 269 (2006)
J. Choi, H. Lee, S. Moon, J. Colloid Interface Sci. 238, 188 (2001)
R. Pomes, B. Roux, Biophys. J. 71, 19 (1996)
Y.S. Park, T. Hatae, H. Itoh, M.Y. Jang, Y. Yamazaki, Electrochim. Acta 50, 592 (2004)
S. Banerjee, D.E. Curtin, J. Fluorine Chem. 125, 1211 (2004)
C.J.D. von Grotthuss. Ann. Chim. 8, 54 (1806)
S. Urata, J. Irisawa, A. Takada, S. Tsuzuki, W. Shinodab, M. Mikami, Phys. Chem. Chem. Phys. 6, 3325 (2004)
S.J. Paddison, J.A. Elliottb, Phys. Chem. Chem. Phys. 8, 2193 (2006)
S.J. Paddison, J.A. Elliottb, J. Phys. Chem. A 109, 7583 (2005)
M. Eikerling, S.J. Paddison, L.R. Pratt, T.A. Zawodzinski Jr, Chem. Phys. Lett. 368, 108 (2003)
S.J. Paddison, T.A. Zawodzinski Jr, Solid State Ionics 113–115, 333 (1998)
J. Ennari, M. Elomaa, F. Sundholm, Polymer 40, 5035 (1999)
J. Ennari, I. Neelov, F. Sundholm, Polymer 41, 2149 (2000)
X. Zhou, Z. Chen, F. Delgado, D. Brenner, R. Srivastava, J. Electrochem. Soc. 154, B82 (2007)
S.S. Jang, V. Molinero, T. Cüagın, W.A. Goddard III, J. Phys. Chem. B 108, 3149 (2004)
S. Dokmaisrijan, E. Spohr, Journal of Molecular Liquids 129, 92 (2006)
D. Seeliger, C. Hartnig, E. Spohr, Electrochim. Acta 50, 4234 (2005)
M.K. Petersen, F. Wang, N.P. Blake, H. Metiu, G.A. Voth, J. Phys. Chem. B 109, 3727 (2005)
M.K. Petersen, G.A. Voth, J. Phys. Chem. B 110, 18594 (2006)
Acknowledgment
The authors would like to thank the National Science Foundation for financial support for this work via Grant # CBET-0933393.
Author information
Authors and Affiliations
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2009 Springer Science+Business Media, LLC
About this chapter
Cite this chapter
Zhou, X., Zhou, J., Yin, Y. (2009). Atomistic Modeling in Study of Polymer Electrolyte Fuel Cells – A Review. In: Wang, CY., Pasaogullari, U. (eds) Modeling and Diagnostics of Polymer Electrolyte Fuel Cells. Modern Aspects of Electrochemistry. Springer, New York, NY. https://doi.org/10.1007/978-0-387-98068-3_9
Download citation
DOI: https://doi.org/10.1007/978-0-387-98068-3_9
Published:
Publisher Name: Springer, New York, NY
Print ISBN: 978-0-387-98067-6
Online ISBN: 978-0-387-98068-3
eBook Packages: Chemistry and Materials ScienceChemistry and Material Science (R0)