Abstract
We describe a new class of electrocatalysts for the O2 reduction, and H2 and methanol oxidation reactions, consisting of a monolayer of Pt deposited on a metal or alloy carbon-supported nanoparticles. These electrocatalysts show up to a 20-fold increase in Pt mass activity compared with conventional all-Pt electrocatalysts. The origin of their increased activity was identified through a combination of experimental methods, employing electrochemical and surface science techniques, X-ray absorption spectroscopy, and density functional theory calculations. The long-term tests in fuel cells demonstrated excellent stability of the anode and good stability of the cathode electrocatalysts. We also describe the stabilization of Pt electrocatalysts against dissolution under potential cycling regimes effected by a submonolayer of Au clusters deposited on Pt surfaces. These new electrocatalysts promise to alleviate some of the major problems of existing fuel cell technology.
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Cleghorn SJC, Ren X, Springer TE. Wilson MS, Zawodzinski C, Zawodzinski TA, Gottesfeld S (1997) Int J Hydrogen Energy 22:1137–1144
Inoue H, Wang JX, Sasaki K, Adzic RR (2003) J Electroanal Chem 554:77–85
Tarasevich MR, Sadkowski A, Eager E (1983) In: Conway BE (ed) Comprehensive treatise of electrochemistry. Plenum, New York, pp 301–398
Adzic RR (1998) In: Jacek Lipkowski PNR (ed) Electrocatalysis. Wiley–VCH, Inc., p 197
Markovic NM, Ross PN (1999) In: Wieckowski A (ed) Interfacial electrochemistry. Marcel Dekker, New York, pp 821
Brankovic SR, Wang JX, Adzic RR (2001) Electrochem Solid-State Lett 4:A217–A220
Zhang J, Lima FHB, Shao MH, Sasaki K, Wang JX, Hanson J, Adzic RR (2005) J Phys Chem B 109:22701–22704
Zhang J, Vukmirovic MB, Sasaki K, Uribe F, Adzic RR, Serb J (2005) Chem Soc 70:513–525
Hammer B, Norskov JK (2000) Advance catalysis. Academic Press Inc., San Diego, pp 71–129
Sasaki K, Wang JX, Balasubramanian M, McBreen J, Uribe F, Adzic RR (2004) Electrochim Acta 49:3873–3877
Zhang J, Mo Y, Vukmirovic MB, Klie R, Sasaki K, Adzic RR (2004) J Phys Chem B 108:10955–10964
Brankovic SR, Wang JX, Adzic RR (2001) Surf Sci 474:L173–L179
Brankovic SR, Wang JX, Adzic RR (2001) J Serb Chem Soc 66:887–898
Vanderbilt D (1990) Phys Rev B 41:7892–7895
Greeley J, Norskov JK, Mavrikakis M (2002) Annu Rev Phys Chem 53:319–348
Hammer M, Hansen LB, Norskov JK (1999) Phys Rev B 59:7413–7421
Greeley J, Mavrikakis M (2004) Nature Mater 3:810–815
Xu Y, Ruban AV, Mavrikakis M (2004) J Am Chem Soc 126:4717–4725
Ashcroft NW, Mermin ND (1976) Solid state physics. Saunders College, Orlando FL
Wang JX, Springer TE, Adzic RR (2006) J Electrochem Soc 153:A1732–A1740
Brankovic SR, Marinkovic NS, Wang JX, Adzic RR (2002) J Electroanal Chem 532:57–66
Koper MTM, Shubina TE, van Santen RA (2002) J Phys Chem B 106:686
de Mongeot FB, Scherer M, Gleich B, Kopatzki E, Behm RJ (1998) Surf Sci 411:249–62
Chen SL, Kucernak A (2004) J Phys Chem B 108:13984–13994
Zhang JL, Vukmirovic MB, Xu Y, Mavrikakis M, Adzic RR (2005) Angew Chem Int Ed 44:2132–2135
Zhang JL, Vukmirovic MB, Sasaki K, Nilekar AU, Mavrikakis M, Adzic RR (2005) J Am Chem Soc 127:12480–12481
Rodriguez JA (1996) Surf Sci Rep 24:225–287
Kitchin JR, Norskov JK, Barteau MA, Chen JG (2004) J Chem Phys 120:10240–10246
Mukerjee S, Srinivasan S, Soriaga MP, McBreen J (1995) J Phys Chem 99:4577–4589
Ruckman MW, Strongin M (1994) Acc Chem Res 27:250–256
Markovic NM, Schmidt TJ, Stamenkovic V, Ross PN (2001) Fuel Cells 1:105
Murthi VS, Urian RC, Mukerjee S (2004) J Phys Chem B 108:11011–11023
Shao M, Liu P, Zhang J, Adzic RR (2007) J Phys Chem 111:6772–6775
Zhang J, Sutter SKE. Adzic RR (2007) Science 315:220
Woods R (1976) In: Bard AJ (ed) Electroanalytical chemistry. Marcel Dekker, New York, pp 1–162
Roudgar A, Groβ A (2004) Surf Sci 559:L180–L186
Del Popolo MG, Leiva EPM, Mariscal M, Schmickler W (2005) Surf Sci 597:133–155
Acknowledgments
This work is supported by U.S. Department of Energy, Divisions of Chemical and Material Sciences, under the Contract No. DE-AC02-98CH10886. Work at UW-Madison was supported by DOE-BES, Chemical Sciences Office, and by S. C. Johnson through a fellowship to AUN. Supercomputing time at NERSC, PNNL, and ORNL resources is gratefully acknowledged.
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Adzic, R.R., Zhang, J., Sasaki, K. et al. Platinum Monolayer Fuel Cell Electrocatalysts. Top Catal 46, 249–262 (2007). https://doi.org/10.1007/s11244-007-9003-x
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DOI: https://doi.org/10.1007/s11244-007-9003-x