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Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts
Open accessAbstract
Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H 2 O 2). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M–O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M–O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm−2 H 2 O 2 current in alkaline and neutral media, respectively) and high H 2 O 2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H 2 O 2 production.
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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
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction
Shao, M., Chang, Q., Dodelet, J.-P., & Chenitz, R. (2016) · Chemical Reviews · doi:10.1021/acs.chemrev.5b00462 · Cited by 3,903
Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton’s Reaction Chemistry
Brillas, E., Sirés, I., & Oturan, M. A. (2009) · Chemical Reviews · doi:10.1021/cr900136g · Cited by 3,437
Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
Choi, C. H., Kim, M., Kwon, H. C., Cho, S. J., Yun, S., Kim, H.-T., Mayrhofer, K. J. J., Kim, H., & Choi, M. (2016) · Nature Communications · doi:10.1038/ncomms10922 · Cited by 849
Cited by
Chen, S., Luo, T., Li, X., Chen, K., Fu, J., Liu, K., Cai, C., Wang, Q., Li, H., Chen, Y., et al. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.2c01194 · Cited by 560
Shi, Z., Wang, Y., Li, J., Wang, X., Wang, Y., Li, Y., Xu, W., Jiang, Z., Liu, C., Xing, W., et al. (2021) · Joule · doi:10.1016/j.joule.2021.05.018 · Cited by 554
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Metadata
- Authors
- Yang, Q., Xu, W., Gong, S., Zheng, G., Tian, Z., Wen, Y., Peng, L., Zhang, L., Lu, Z., & Chen, L.
- Venue
- Nature Communications
- Published
- 2020-10-30
- Volume
- 11
- Issue
- 1
- Pages
- 5478-5478
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W3097391371
- Cited by
- 241
- References
- 5
- FWCI
- 5.01
- Type
- journal article
- Language
- en
- Open access
- gold
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