The DOI matches its Crossref record; 28 of the 28 references it cites were found in a registry or an index.
Hydrogen Peroxide Synthesis via Enhanced Two-Electron Oxygen Reduction Pathway on Carbon-Coated Pt Surface
Abstract
Continuous on-site electrochemical production of hydrogen peroxide (H 2 O 2 ) can provide an attractive alternative to the present anthraquinone-based H 2 O 2 production technology. A major challenge in the electrocatalyst design for H 2 O 2 production is that O 2 adsorption on the Pt surface thermodynamically favors “side-on” configuration over “end-on” configuration, which leads to a dissociation of O–O bond via dominant 4-electron pathway. This prefers H 2 O production rather than H 2 O 2 production during the electrochemical oxygen reduction reaction (ORR). In the present work, we demonstrate that controlled coating of Pt catalysts with amorphous carbon layers can induce selective end-on adsorption of O 2 on the Pt surface by eliminating accessible Pt ensemble sites, which allows significantly enhanced H 2 O 2 production selectivity in the ORR. Experimental results and theoretical modeling reveal that 4-electron pathway is strongly suppressed in the course of ORR due to a thermodynamically unfavored end-on adsorption of O 2 (the first electron transfer step) with 0.54 V overpotential. As a result, the carbon-coated Pt catalysts show an onset potential of ∼0.7 V for ORR and remarkably enhanced H 2 O 2 selectivity up to 41%. Notably, the produced H 2 O 2 cannot access the Pt surface due to the steric hindrance of the coated carbon layers, and thus no significant H 2 O 2 decomposition via disproportionation/reduction reactions is observed. Furthermore, the catalyst shows superior stability without considerable performance degradation because the amorphous carbon layers protect Pt catalysts against the leaching and ripening in acidic operating conditions.
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Cited by
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Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
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Self-citationHighly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination
Jiang, K., Back, S., Akey, A. J., Xia, C., Hu, Y., Liang, W., Schaak, D., Stavitski, E., Nørskov, J. K., Siahrostami, S., et al. (2019) · Nature Communications · doi:10.1038/s41467-019-11992-2 · Cited by 820
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One- or Two-Electron Water Oxidation, Hydroxyl Radical, or H2O2 Evolution
Siahrostami, S., Li, G.-L., Viswanathan, V., & Nørskov, J. K. (2017) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.6b02924 · Cited by 384
Metadata
- Authors
- Choi, C. H., Kwon, H. C., Yook, S., Shin, H., Kim, H., & Choi, M.
- Venue
- The Journal of Physical Chemistry C
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-12-15
- Volume
- 118
- Issue
- 51
- Pages
- 30063-30070
- ISSN
- 1932-7447 (ISSN-L)
- 1932-7455
- OpenAlex
- W2320907518
- Cited by
- 339
- References
- 28
- FWCI
- 2.95
- Type
- journal article
- Language
- en
- Open access
- closed
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