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Binding energy shifts for nitrogen‐containing graphene‐based electrocatalysts – experiments and DFT calculations
Abstract
A detailed analysis of the physiochemical nature, thermodynamic properties, and electrochemical characterization of N motifs present in self‐assembled nitrogen functionalized transition metal and nitrogen doped graphene pyrolyzed materials has been conducted in this study. First principle density‐functional‐theory calculations were performed to assess the thermochemistry of Fe–N x and graphitic‐N defects and to predict N1s core‐level‐shifts. Combining this prediction with our X‐ray photoelectron spectroscopy and rotating ring disk electrode experiments, we find that graphitic‐N contributes significantly to hydrogen peroxide formation in oxygen reduction reactions, while materials containing nitrogen coordinated transition metal result in the complete reduction of oxygen to water. Lastly, we show how the synergy of experimental, electrochemical, and computational approaches can accelerate the accurate identification and characterization of nitrogen functionalized graphene moieties present in pyrolyzed electrocatalysts for fuel cells. Copyright © 2016 John Wiley & Sons, Ltd.
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Cites
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
Greeley, J., Stephens, I. E. L., Bondarenko, A. S., Johansson, T. P., Hansen, H. A., Jaramillo, T. F., Rossmeisl, J., Chorkendorff, I., & Nørskov, J. K. (2009) · Nature Chemistry · doi:10.1038/nchem.367 · Cited by 3,203
Evolution of nitrogen functionalities in carbonaceous materials during pyrolysis
Pels, J. R., Kapteijn, F., Moulijn, J. A., Zhu, Q., & Thomas, K. M. (1995) · Carbon · doi:10.1016/0008-6223(95)00154-6 · Cited by 2,041
Cited by
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
Yang, H. B., Hung, S.-F., Liu, S., Yuan, K., Miao, S., Zhang, L., Huang, X., Wang, H.-Y., Cai, W., Chen, R., et al. (2018) · Nature Energy · doi:10.1038/s41560-017-0078-8 · Cited by 2,239
Large-Scale and Highly Selective CO2 Electrocatalytic Reduction on Nickel Single-Atom Catalyst
Zheng, T., Jiang, K., Ta, N., Hu, Y., Zeng, J., Liu, J., & Wang, H. (2019) · Joule · doi:10.1016/j.joule.2018.10.015 · Cited by 887
Ebner, K., Clark, A. H., Saveleva, V. A., Smolentsev, G., Chen, J., Ni, L., Li, J., Zitolo, A., Jaouen, F., Kramm, U. I., et al. (2022) · Advanced Energy Materials · doi:10.1002/aenm.202103699 · Cited by 61
Metadata
- Authors
- Kabir, S., Artyushkova, K., Serov, A., Kiefer, B., & Atanassov, P.
- Venue
- Surface and Interface Analysis
- Publisher
- Wiley
- Published
- 2016-01-22
- Volume
- 48
- Issue
- 5
- Pages
- 293-300
- ISSN
- 0142-2421 (ISSN-L)
- 1096-9918
- OpenAlex
- W2312071824
- Cited by
- 204
- References
- 2
- FWCI
- 5.63
- Type
- journal article
- Language
- en
- Open access
- closed
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- Kabir, S., Artyushkova, K., Serov, A., Kiefer, B., & Atanassov, P. (2016). Binding energy shifts for nitrogen‐containing graphene‐based electrocatalysts – experiments and DFT calculations. Surface and Interface Analysis. https://doi.org/10.1002/sia.5935
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