The DOI matches its Crossref record; 4 of the 4 references it cites were found in a registry or an index.
Double-Trap Kinetic Equation for the Oxygen Reduction Reaction on Pt(111) in Acidic Media
Abstract
We derived an intrinsic kinetic equation for the four-electron oxygen reduction reaction (ORR) in acidic media using free energies of activation and adsorption as the kinetic parameters. Our kinetic model consists of four essential elementary reactions: a dissociative adsorption (DA) and a reductive adsorption (RA), which yield two reaction intermediates, O and OH; a reductive transition (RT) from O to OH; and a reductive desorption (RD) of OH. Analytic expressions were found for the O and OH adsorption isotherms by solving the steady-state rate equations. For the ORR on Pt(111) in 0.1 M HClO4 solution, we analyzed the measured polarization curves, thereby deducing activation free energies that are consistent with the values from theoretical calculations. The reductive adsorption (DeltaG*0RA=0.46 eV) is not the rate-determining step (RDS) for the ORR on Pt because dissociative adsorption (DeltaG*0DA=0.26 eV) offers a more favorable pathway at high potentials. It, however, generates strongly adsorbed O. The high activation barriers for the O to OH transition (DeltaG*0RT=0.50 eV) and OH desorption (DeltaG*0RD=0.45 eV) cause a large potential loss for the desorption-limited ORR. As the OH coverage increases to a constant value with decreasing potential, the Tafel slope increases to the value determined by a symmetric electron-transfer coefficient. We discuss the role of adsorption isotherm in kinetic analysis and, via activity-and-barrier plots, illustrate why the RDS may vary with reaction conditions or may not exist. Recognizing such features of electrocatalytic reactions can facilitate reaching the long-standing goal of quantitative descriptions and predictions of electrocatalysts' activities.
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Citations
Cites
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
Nørskov, J. K., Rossmeisl, J., Logadottir, A., Lindqvist, L., Kitchin, J. R., Bligaard, T., & Jónsson, H. (2004) · The Journal of Physical Chemistry B · doi:10.1021/jp047349j · Cited by 13,153
Improved Oxygen Reduction Activity on Pt 3 Ni(111) via Increased Surface Site Availability
Stamenkovic, V. R., Fowler, B., Mun, B. S., Wang, G., Ross, P. N., Lucas, C. A., & Marković, N. M. (2007) · Science · doi:10.1126/science.1135941 · Cited by 4,421
Tian, N., Zhou, Z.-Y., Sun, S.-G., Ding, Y., & Wang, Z. L. (2007) · Science · doi:10.1126/science.1140484 · Cited by 3,073
Adsorption and Dissociation of O 2 on Pt−Co and Pt−Fe Alloys
Xu, Y., Ruban, A. V., & Mavrikakis, M. (2004) · Journal of the American Chemical Society · doi:10.1021/ja031701+ · Cited by 636
Cited by
Shinagawa, T., Garcia-Esparza, A. T., & Takanabe, K. (2015) · Scientific Reports · doi:10.1038/srep13801 · Cited by 3,287
Metal-Free Catalysts for Oxygen Reduction Reaction
Dai, L., Xue, Y., Qu, L., Choi, H.-J., & Baek, J.-B. (2015) · Chemical Reviews · doi:10.1021/cr5003563 · Cited by 2,380
Wang, J. X., Inada, H., Wu, L., Zhu, Y., Choi, Y., Liu, P., Zhou, W.-P., & Adzic, R. R. (2009) · Journal of the American Chemical Society · doi:10.1021/ja9067645 · Cited by 719
Self-citationCore‐Protected Platinum Monolayer Shell High‐Stability Electrocatalysts for Fuel‐Cell Cathodes
Sasaki, K., Naohara, H., Cai, Y., Choi, Y. M., Liu, P., Vukmirovic, M. B., Wang, J. X., & Adzic, R. R. (2010) · Angewandte Chemie International Edition · doi:10.1002/anie.201004287 · Cited by 596
Self-citationKoenigsmann, C., & Wong, S. S. (2011) · Energy Environ. Sci. · doi:10.1039/c0ee00197j · Cited by 392
Improved oxygen reduction reactivity of platinum monolayers on transition metal surfaces
Nilekar, A. U., & Mavrikakis, M. (2008) · Surface Science · doi:10.1016/j.susc.2008.05.036 · Cited by 226
Setzler, B. P., & Fuller, T. F. (2015) · Journal of The Electrochemical Society · doi:10.1149/2.0361506jes · Cited by 117
Futter, G. A., Gazdzicki, P., Friedrich, K. A., Latz, A., & Jahnke, T. (2018) · Journal of Power Sources · doi:10.1016/j.jpowsour.2018.04.070 · Cited by 94
Hu, J., Wu, L., Kuttiyiel, K. A., Goodman, K. R., Zhang, C., Zhu, Y., Vukmirovic, M. B., White, M. G., Sasaki, K., & Adzic, R. R. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b04999 · Cited by 94
Self-citationHow theory and simulation can drive fuel cell electrocatalysis
Eslamibidgoli, M. J., Huang, J., Kadyk, T., Malek, A., & Eikerling, M. (2016) · Nano Energy · doi:10.1016/j.nanoen.2016.06.004 · Cited by 83
Low-Coordination Sites in Oxygen-Reduction Electrocatalysis: Their Roles and Methods for Removal
Cai, Y., Ma, C., Zhu, Y., Wang, J. X., & Adzic, R. R. (2011) · Langmuir · doi:10.1021/la200753z · Cited by 80
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Metadata
- Authors
- Wang, J. X., Zhang, J., & Adzic, R. R.
- Venue
- The Journal of Physical Chemistry A
- Publisher
- American Chemical Society (ACS)
- Published
- 2007-12-01
- Volume
- 111
- Issue
- 49
- Pages
- 12702-12710
- ISSN
- 1089-5639 (ISSN-L)
- 1520-5215
- OpenAlex
- W2074646172
- Cited by
- 203
- References
- 4
- FWCI
- 5.18
- Type
- journal article
- Language
- en
- Open access
- closed
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