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Theory of multiple proton–electron transfer reactions and its implications for electrocatalysis
Open accessAbstract
This perspective article outlines a simple but general theoretical analysis for multiple proton–electron transfer reactions, based on the microscopic theory of proton-coupled electron transfer reactions, recent developments in the thermodynamic theory of multi-step electron transfer reactions, and the experimental realization that many multiple proton-coupled electron transfer reactions feature decoupled proton–electron steps in their mechanism. It is shown that decoupling of proton and electron transfer leads to a strong pH dependence of the overall catalytic reaction, implying an optimal pH for high catalytic turnover, and an associated optimal catalyst at the optimal pH. When more than one catalytic intermediate is involved, scaling relationships between intermediates may dictate the optimal catalyst and limit the extent of reversibility that may be achievable for a multiple proton–electron transfer reaction. The theory is discussed in relation to the experimental results for a number of redox reactions that are of importance for sustainable energy conversion, primarily focusing on their pH dependence.
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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
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
Man, I. C., Su, H., Calle‐Vallejo, F., Hansen, H. A., Martínez, J. I., Inoglu, N. G., Kitchin, J., Jaramillo, T. F., Nørskov, J. K., & Rossmeisl, J. (2011) · ChemCatChem · doi:10.1002/cctc.201000397 · Cited by 4,769
Biomimetic Hydrogen Evolution: MoS 2 Nanoparticles as Catalyst for Hydrogen Evolution
Hinnemann, B., Moses, P. G., Bonde, J., Jørgensen, K. P., Nielsen, J. H., Horch, S., Chorkendorff, I., & Nørskov, J. K. (2005) · Journal of the American Chemical Society · doi:10.1021/ja0504690 · Cited by 4,065
Abild-Pedersen, F., Greeley, J., Studt, F., Rossmeisl, J., Munter, T. R., Moses, P. G., Skúlason, E., Bligaard, T., & Nørskov, J. K. (2007) · Physical Review Letters · doi:10.1103/physrevlett.99.016105 · Cited by 1,678
Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts
Peterson, A. A., & Nørskov, J. K. (2012) · The Journal of Physical Chemistry Letters · doi:10.1021/jz201461p · Cited by 1,667
Cited by
Shinagawa, T., Garcia-Esparza, A. T., & Takanabe, K. (2015) · Scientific Reports · doi:10.1038/srep13801 · Cited by 3,287
A review on fundamentals for designing oxygen evolution electrocatalysts
Song, J., Wei, C., Huang, Z.-F., Liu, C., Zeng, L., Wang, X., & Xu, Z. J. (2020) · Chemical Society Reviews · doi:10.1039/c9cs00607a · Cited by 2,936
Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction
Kulkarni, A., Siahrostami, S., Patel, A., & Nørskov, J. K. (2018) · Chemical Reviews · doi:10.1021/acs.chemrev.7b00488 · Cited by 2,742
A Review of Electrocatalytic Reduction of Dinitrogen to Ammonia under Ambient Conditions
Cui, X., Tang, C., & Zhang, Q. (2018) · Advanced Energy Materials · doi:10.1002/aenm.201800369 · Cited by 1,314
Reier, T., Nong, H. N., Teschner, D., Schlögl, R., & Strasser, P. (2017) · Advanced Energy Materials · doi:10.1002/aenm.201601275 · Cited by 1,253
Metadata
- Authors
- Koper, M. T. M.
- Venue
- Chemical Science
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2013
- Volume
- 4
- Issue
- 7
- Pages
- 2710
- ISSN
- 2041-6520 (ISSN-L)
- 2041-6539
- OpenAlex
- W2135572322
- Cited by
- 898
- References
- 5
- FWCI
- 10.34
- Type
- journal article
- Language
- en
- Open access
- green
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Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
