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Intrinsic Relationship between Enhanced Oxygen Reduction Reaction Activity and Nanoscale Work Function of Doped Carbons
Abstract
Nanostructured carbon materials doped with a variety of heteroatoms have shown promising electrocatalytic activity in the oxygen reduction reaction (ORR). However, understanding of the working principles that underpin the superior ORR activity observed with doped nanocarbons is still limited to predictions based on theoretical calculations. Herein, we demonstrate, for the first time, that the enhanced ORR activity in doped nanocarbons can be correlated with the variation in their nanoscale work function. A series of doped ordered mesoporous carbons (OMCs) were prepared using N, S, and O as dopants; the triple-doped, N,S,O-OMC displayed superior ORR activity and four-electron selectivity compared to the dual-doped (N,O-OMC and S,O-OMC) and the monodoped (O-OMC) OMCs. Significantly, the work functions of these heteroatom-doped OMCs, measured by Kelvin probe force microscopy, display a strong correlation with the activity and reaction kinetics for the ORR. This unprecedented experimental insight can be used to provide an explanation for the enhanced ORR activity of heteroatom-doped carbon materials.
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Cites
Li-O2 and Li-S batteries with high energy storage
Bruce, P. G., Freunberger, S. A., Hardwick, L. J., & Tarascon, J.-M. (2012) · Nature Materials · doi:10.1038/nmat3191 · Cited by 9,479
Electrocatalyst approaches and challenges for automotive fuel cells
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High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
Wu, G., More, K. L., Johnston, C. M., & Zelenay, P. (2011) · Science · doi:10.1126/science.1200832 · Cited by 3,984
Yang, S., Feng, X., Wang, X., & Müllen, K. (2011) · Angewandte Chemie International Edition · doi:10.1002/anie.201100170 · Cited by 1,109
Cited by
Design of electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions
Jiao, Y., Zheng, Y., Jaroniec, M., & Qiao, S. Z. (2015) · Chemical Society Reviews · doi:10.1039/c4cs00470a · Cited by 5,388
Jiao, Y., Zheng, Y., Davey, K., & Qiao, S.-Z. (2016) · Nature Energy · doi:10.1038/nenergy.2016.130 · Cited by 1,196
A defect-driven metal-free electrocatalyst for oxygen reduction in acidic electrolyte
Li, D., Jia, Y., Chang, G., Chen, J., Liu, H., Wang, J., Hu, Y., Xia, Y., Yang, D., & Yao, X. (2018) · Chem · doi:10.1016/j.chempr.2018.07.005 · Cited by 375
Patel, M. A., Luo, F., Khoshi, M. R., Rabie, E., Zhang, Q., Flach, C. R., Mendelsohn, R., Garfunkel, E., Szostak, M., & He, H. (2016) · ACS Nano · doi:10.1021/acsnano.5b07054 · Cited by 359
Jackson, C., Smith, G. T., Inwood, D. W., Leach, A. S., Whalley, P. S., Callisti, M., Polcar, T., Russell, A. E., Levecque, P., & Kramer, D. (2017) · Nature Communications · doi:10.1038/ncomms15802 · Cited by 231
Metadata
- Authors
- Cheon, J. Y., Kim, J. H., Kim, J. H., Goddeti, K. C., Park, J. Y., & Joo, S. H.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-06-13
- Volume
- 136
- Issue
- 25
- Pages
- 8875-8878
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2319861996
- Cited by
- 414
- References
- 5
- FWCI
- 10.59
- Type
- journal article
- Language
- en
- Open access
- closed
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- Cheon, J. Y., Kim, J. H., Kim, J. H., Goddeti, K. C., Park, J. Y., & Joo, S. H. (2014). Intrinsic Relationship between Enhanced Oxygen Reduction Reaction Activity and Nanoscale Work Function of Doped Carbons. Journal of the American Chemical Society. https://doi.org/10.1021/ja503557x
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